Bio


Dr. Abild-Pedersen is the acting co-director of SUNCAT Center for Interface Science and Catalysis. He is leading a research team that focuses on developing an understanding of the factors determining the catalytic properties at the interface between gas/solvent and solid surfaces and to apply these insights to processes and catalysts of importance for energy transformations and for sustainable chemical production. His research takes advantage of computer facilities at SLAC and Stanford to gain the necessary understanding and to link these simulations to experiments where new catalyst synthesis methods are developed, and the catalyst materials are characterized both in terms of performance (activity, selectivity, durability, etc.) and in terms of geometrical and electronic structure. The underlying philosophy of his research is that by having a fundamental understanding of the way surfaces catalyze a chemical reaction we can make a quantum leap in our ability to make predictions for new catalysts and processes. This requires the development of a theory of heterogeneous catalysis, including electrocatalysis, based on computational and experimental results.

Dr Abild-Pedersen has extensive experience with simulations and modeling of chemical reactions. His work began with the derivation of energy correlations in catalysis that have helped speed up screening for active, selective and stable catalysts for energy conversion as a graduate student working with Professor Jens K. Nørskov at the Technical University of Denmark. He moved to SLAC in 2010 as a staff scientist and helped build up SUNCAT and define research directions in the field of heterogeneous catalysis.

Education & Certifications


  • PhD, Technical University of Denmark, Physics (2005)

All Publications


  • Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies PHYSICAL REVIEW B Hamamoto, Y., Wella, S., Inagaki, K., Abild-Pedersen, F., Bligaard, T., Hamada, I., Morikawa, Y. 2020; 102 (7)
  • Predicting metal-metal interactions. II. Accelerating generalized schemes through physical insights JOURNAL OF CHEMICAL PHYSICS Choksi, T. S., Streibel, V., Abild-Pedersen, F. 2020; 152 (9)

    View details for DOI 10.1063/1.5141378

    View details for Web of Science ID 000519108300002

  • Predicting metal-metal interactions. I. The influence of strain on nanoparticle and metal adlayer stabilities JOURNAL OF CHEMICAL PHYSICS Streibel, V., Choksi, T. S., Abild-Pedersen, F. 2020; 152 (9)

    View details for DOI 10.1063/1.5130566

    View details for Web of Science ID 000519108300001

  • Revealing the structure of a catalytic combustion active-site ensemble combining uniform nanocrystal catalysts and theory insights. Proceedings of the National Academy of Sciences of the United States of America Yang, A. C., Choksi, T., Streibel, V., Aljama, H., Wrasman, C. J., Roling, L. T., Goodman, E. D., Thomas, D., Bare, S. R., Sánchez-Carrera, R. S., Schäfer, A., Li, Y., Abild-Pedersen, F., Cargnello, M. 2020

    Abstract

    Supported metal catalysts are extensively used in industrial and environmental applications. To improve their performance, it is crucial to identify the most active sites. This identification is, however, made challenging by the presence of a large number of potential surface structures that complicate such an assignment. Often, the active site is formed by an ensemble of atoms, thus introducing further complications in its identification. Being able to produce uniform structures and identify the ones that are responsible for the catalyst performance is a crucial goal. In this work, we utilize a combination of uniform Pd/Pt nanocrystal catalysts and theory to reveal the catalytic active-site ensemble in highly active propene combustion materials. Using colloidal chemistry to exquisitely control nanoparticle size, we find that intrinsic rates for propene combustion in the presence of water increase monotonically with particle size on Pt-rich catalysts, suggesting that the reaction is structure dependent. We also reveal that water has a near-zero or mildly positive reaction rate order over Pd/Pt catalysts. Theory insights allow us to determine that the interaction of water with extended terraces present in large particles leads to the formation of step sites on metallic surfaces. These specific step-edge sites are responsible for the efficient combustion of propene at low temperature. This work reveals an elusive geometric ensemble, thus clearly identifying the active site in alkene combustion catalysts. These insights demonstrate how the combination of uniform catalysts and theory can provide a much deeper understanding of active-site geometry for many applications.

    View details for DOI 10.1073/pnas.2002342117

    View details for PubMedID 32554500

  • Catalyst deactivation via decomposition into single atoms and the role of metal loading NATURE CATALYSIS Goodman, E. D., Johnston-Peck, A. C., Dietze, E. M., Wrasman, C. J., Hoffman, A. S., Abild-Pedersen, F., Bare, S. R., Plessow, P. N., Cargnello, M. 2019; 2 (9): 748–55
  • Single-atom species determine the deactivation of supported catalysts Cargnello, M., Goodman, E., Abild-Pedersen, F., Bare, S. AMER CHEMICAL SOC. 2019
  • Machine Learning for Computational Heterogeneous Catalysis CHEMCATCHEM Lamoureux, P., Winther, K. T., Torres, J., Streibel, V., Zhao, M., Bajdich, M., Abild-Pedersen, F., Bligaard, T. 2019; 11 (16): 3579–99
  • Enhancing Electrocatalytic Water Splitting by Strain Engineering ADVANCED MATERIALS You, B., Tang, M. T., Tsai, C., Abild-Pedersen, F., Zheng, X., Li, H. 2019; 31 (17)
  • Predicting Adsorption Properties of Catalytic Descriptors on Bimetallic Nanoalloys with Site-Specific Precision JOURNAL OF PHYSICAL CHEMISTRY LETTERS Choksi, T. S., Roling, L. T., Streibel, V., Abild-Pedersen, F. 2019; 10 (8): 1852–59
  • Revealing the Synergy between Oxide and Alloy Phases on the Performance of Bimetallic In-Pd Catalysts for CO2 Hydrogenation to Methanol ACS CATALYSIS Snider, J. L., Streibel, V., Hubert, M. A., Choksi, T. S., Valle, E., Upham, D., Schumann, J., Duyar, M. S., Gallo, A., Abild-Pedersen, F., Jaramillo, T. F. 2019; 9 (4): 3399–3412
  • Density-dependent deactivation mechanism in supported catalysts by high-temperature decomposition of particles into single atoms Goodman, E., Johnston-Peck, A., Dietze, E., Wrasman, C., Hoffman, A., Abild-Pedersen, F., Bare, S., Plessow, P., Cargnello, M. AMER CHEMICAL SOC. 2019
  • Uncovering the details of methane combustion on palladium catalysts using well-defined nanocrystal precursors Cargnello, M., Huang, W., Goodman, E., Willis, J., Yang, A., Abild-Pedersen, F., Johnston-Peck, A., Bare, S. AMER CHEMICAL SOC. 2019
  • A coordination-based model for transition metal alloy nanoparticles NANOSCALE Roling, L. T., Choksi, T. S., Abild-Pedersen, F. 2019; 11 (10): 4438–52

    View details for DOI 10.1039/c9nr00959k

    View details for Web of Science ID 000465410200028

  • Enhancing Electrocatalytic Water Splitting by Strain Engineering. Advanced materials (Deerfield Beach, Fla.) You, B., Tang, M. T., Tsai, C., Abild-Pedersen, F., Zheng, X., Li, H. 2019: e1807001

    Abstract

    Electrochemical water splitting driven by sustainable energy such as solar, wind, and tide is attracting ever-increasing attention for sustainable production of clean hydrogen fuel from water. Leveraging these advances requires efficient and earth-abundant electrocatalysts to accelerate the kinetically sluggish hydrogen and oxygen evolution reactions (HER and OER). A large number of advanced water-splitting electrocatalysts have been developed through recent understanding of the electrochemical nature and engineering approaches. Specifically, strain engineering offers a novel route to promote the electrocatalytic HER/OER performances for efficient water splitting. Herein, the recent theoretical and experimental progress on applying strain to enhance heterogeneous electrocatalysts for both HER and OER are reviewed and future opportunities are discussed. A brief introduction of the fundamentals of water-splitting reactions, and the rationalization for utilizing mechanical strain to tune an electrocatalyst is given, followed by a discussion of the recent advances on strain-promoted HER and OER, with special emphasis given to combined theoretical and experimental approaches for determining the optimal straining effect for water electrolysis, along with experimental approaches for creating and characterizing strain in nanocatalysts, particularly emerging 2D nanomaterials. Finally, a vision for a future sustainable hydrogen fuel community based on strain-promoted water electrolysis is proposed.

    View details for PubMedID 30773741

  • Accessing the C-C transition state energy on transition metals. Physical chemistry chemical physics : PCCP Aljama, H., Abild-Pedersen, F. 2019

    Abstract

    The search for catalysts that can efficiently convert large hydrocarbons has been an active area of research for decades. To gain insight into those reactions, electronic structure calculations are playing an increasing role but the screening efforts are impeded by the complexity of the reaction networks that can contain hundreds of elementary steps, presenting a large number of computationally expensive transition state barrier calculations. A large number of the sub reactions in the network involve C-C bond dissociation, a step that has been identified as rate determining in many studies. The purpose of this article is to present a methodology that allows for accurate and rapid assessment of transition state energies for C-C bond breaking in any hydrocarbon based on a small number of simple calculations. Our model significantly enhances the capability of expanding the search space for new and efficient catalysts.

    View details for DOI 10.1039/c9cp04897a

    View details for PubMedID 31701972

  • Supported Catalyst Deactivation by Decomposition into Single Atoms Is Suppressed by Increasing Metal Loading. Nature catalysis Goodman, E. D., Johnston-Peck, A. C., Dietze, E. M., Wrasman, C. J., Hoffman, A. S., Abild-Pedersen, F., Bare, S. R., Plessow, P. N., Cargnello, M. 2019; 2

    Abstract

    In the high-temperature environments needed to perform catalytic processes, supported precious metal catalysts severely lose their activity over time. Even brief exposure to high temperatures can lead to significant losses in activity, which forces manufacturers to use large amounts of noble metals to ensure effective catalyst function for a required lifetime. Generally, loss of catalytic activity is attributed to nanoparticle sintering, or processes by which larger particles grow at the expense of smaller ones. Here, by independently controlling particle size and particle loading using colloidal nanocrystals, we reveal the opposite process as a novel deactivation mechanism: nanoparticles rapidly lose activity by high-temperature nanoparticle decomposition into inactive single atoms. This deactivation route is remarkably fast, leading to severe loss of activity in as little as ten minutes. Importantly, this deactivation pathway is strongly dependent on particle density and concentration of support defect sites. A quantitative statistical model explains how for certain reactions, higher particle densities can lead to more stable catalysts.

    View details for DOI 10.1038/s41929-019-0328-1

    View details for PubMedID 32118197

    View details for PubMedCentralID PMC7047889

  • Understanding Structure-Property Relationships of MoO3-Promoted Rh Catalysts for Syngas Conversion to Alcohols. Journal of the American Chemical Society Asundi, A. S., Hoffman, A. S., Bothra, P., Boubnov, A., Vila, F. D., Yang, N., Singh, J. A., Zeng, L., Raiford, J. A., Abild-Pedersen, F., Bare, S. R., Bent, S. F. 2019

    Abstract

    Rh-based catalysts have shown promise for the direct conversion of syngas to higher oxygenates. Although improvements in higher oxygenate yield have been achieved by combining Rh with metal oxide promoters, details of the structure of the promoted catalyst and the role of the promoter in enhancing catalytic performance are not well understood. In this work, we show that MoO3-promoted Rh nanoparticles form a novel catalyst structure in which Mo substitutes into the Rh surface, leading to both a 66-fold increase in turnover frequency and an enhancement in oxygenate yield. By applying a combination of atomically controlled synthesis, in situ characterization, and theoretical calculations, we gain an understanding of the promoter-Rh interactions that govern catalytic performance for MoO3-promoted Rh. We use atomic layer deposition to modify Rh nanoparticles with monolayer-precise amounts of MoO3, with a high degree of control over the structure of the catalyst. Through in situ X-ray absorption spectroscopy, we find that the atomic structure of the catalytic surface under reaction conditions consists of Mo-OH species substituted into the surface of the Rh nanoparticles. Using density functional theory calculations, we identify two roles of MoO3: first, the presence of Mo-OH in the catalyst surface enhances CO dissociation and also stabilizes a methanol synthesis pathway not present in the unpromoted catalyst; and second, hydrogen spillover from Mo-OH sites to adsorbed species on the Rh surface enhances hydrogenation rates of reaction intermediates.

    View details for DOI 10.1021/jacs.9b07460

    View details for PubMedID 31724857

  • Theoretical and Experimental Studies of CoGa Catalysts for the Hydrogenation of CO2 to Methanol CATALYSIS LETTERS Singh, J. A., Cao, A., Schumann, J., Wang, T., Norskov, J. K., Abild-Pedersen, F., Bent, S. F. 2018; 148 (12): 3583–91
  • A Highly Active Molybdenum Phosphide Catalyst for Methanol Synthesis from CO and CO2 ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Duyar, M. S., Tsai, C., Snider, J. L., Singh, J. A., Gallo, A., Yoo, J., Medford, A. J., Abild-Pedersen, F., Studt, F., Kibsgaard, J., Bent, S. F., Norskov, J. K., Jaramillo, T. F. 2018; 57 (46): 15045–50

    Abstract

    Methanol is a major fuel and chemical feedstock currently produced from syngas, a CO/CO2 /H2 mixture. Herein we identify formate binding strength as a key parameter limiting the activity and stability of known catalysts for methanol synthesis in the presence of CO2 . We present a molybdenum phosphide catalyst for CO and CO2 reduction to methanol, which through a weaker interaction with formate, can improve the activity and stability of methanol synthesis catalysts in a wide range of CO/CO2 /H2 feeds.

    View details for PubMedID 30134041

  • Mechanistic Insights into the Synthesis of Higher Alcohols from Syngas on CuCo Alloys ACS CATALYSIS Cao, A., Schumann, J., Wang, T., Zhang, L., Xiao, J., Bothra, P., Liu, Y., Abild-Pedersen, F., Norskov, J. K. 2018; 8 (11): 10148–55
  • Strongly Modified Scaling of CO Hydrogenation in Metal Supported TiO Nanostripes ACS CATALYSIS Sandberg, R. B., Hansen, M. H., Norskov, J. K., Abild-Pedersen, F., Bajdich, M. 2018; 8 (11): 10555–63
  • Tuning Methane Activation Chemistry on Alkaline Earth Metal Oxides by Doping JOURNAL OF PHYSICAL CHEMISTRY C Aljama, H., Norskov, J. K., Abild-Pedersen, F. 2018; 122 (39): 22544–48
  • Low-Temperature Methane Partial Oxidation to Syngas with Modular Nanocrystal Catalysts ACS APPLIED NANO MATERIALS Goodman, E. D., Latimer, A. A., Yang, A., Wu, L., Tahsini, N., Abild-Pedersen, F., Cargnello, M. 2018; 1 (9): 5258–67
  • Understanding and tuning catalytic materials using well-defined nanocrystal precursors Cargnello, M., Willis, J., Goodman, E., Wrasman, C., Yang, A., Abild-Pedersen, F., Bare, S. AMER CHEMICAL SOC. 2018
  • Well-defined nanocrystals catalysts as active phases and premier materials for spectroscopic studies of catalyst restructuring Cargnello, M., Goodman, E., Aitbekova, A., Wrasman, C., Riscoe, A., Yang, A., Abild-Pedersen, F., Bare, S. AMER CHEMICAL SOC. 2018
  • Theoretical Investigation of Methane Oxidation on Pd(111) and Other Metallic Surfaces JOURNAL OF PHYSICAL CHEMISTRY C Yoo, J., Schumann, J., Studt, F., Abild-Pedersen, F., Norskov, J. K. 2018; 122 (28): 16023–32
  • Nature of Lone-Pair-Surface Bonds and Their Scaling Relations INORGANIC CHEMISTRY Kakekhani, A., Roling, L. T., Kulkarni, A., Latimer, A. A., Abroshan, H., Schumann, J., Aljama, H., Siahrostami, S., Ismail-Beigi, S., Abild-Pedersen, F., Norskov, J. K. 2018; 57 (12): 7222–38
  • Structure-Sensitive Scaling Relations: Adsorption Energies from Surface Site Stability CHEMCATCHEM Roling, L. T., Abild-Pedersen, F. 2018; 10 (7): 1643–50
  • Selectivity of Synthesis Gas Conversion to C2+ Oxygenates on fcc(111) Transition-Metal Surfaces ACS CATALYSIS Schumann, J., Medford, A. J., Yoo, J., Zhao, Z., Bothra, P., Cao, A., Studt, F., Abild-Pedersen, F., Norskov, J. K. 2018; 8 (4): 3447–53
  • Selective catalysts for higher alcohol synthesis: A combined DFT and micro-kinetic modeling study Schumann, J., Bothra, P., Abild-Pedersen, F., Norskov, J. AMER CHEMICAL SOC. 2018
  • Mechanistic insights into the synthesis of higher alcohols from syngas on CuCo-alloys Cao, A., Schumann, J., Abild-Pedersen, F., Liu, Y., Norskov, J. AMER CHEMICAL SOC. 2018
  • Understanding activity loss in precious-metal combustion catalysts using well-defined nanocrystals Goodman, E., Riscoe, A., Tahsini, N., Abild-Pedersen, F., Johnston-Peck, A., Cargnello, M. AMER CHEMICAL SOC. 2018
  • Understanding and tuning catalytic materials For methane activation using nanocrystal precursors Cargnello, M., Willis, J., Goodman, E., Wrasman, C., Yang, A., Abild-Pedersen, F. AMER CHEMICAL SOC. 2018
  • Generic approach to access barriers in dehydrogenation reactions COMMUNICATIONS CHEMISTRY Yu, L., Vilella, L., Abild-Pedersen, F. 2018; 1
  • Systematic Structure Property Relationship Studies in Palladium Catalyzed Methane Complete Combustion ACS CATALYSIS Willis, J. J., Gallo, A., Sokaras, D., Aljama, H., Nowak, S. H., Goodman, E. D., Wu, L., Tassone, C. J., Jaramillo, T. F., Abild-Pedersen, F., Cargnello, M. 2017; 7 (11): 7810–21
  • Configurational Energies of Nanoparticles Based on Metal-Metal Coordination JOURNAL OF PHYSICAL CHEMISTRY C Roling, L. T., Li, L., Abild-Pedersen, F. 2017; 121 (41): 23002–10
  • Investigating Catalyst-Support Interactions To Improve the Hydrogen Evolution Reaction Activity of Thiomolybdate [Mo3S13](2-) Nanoclusters ACS CATALYSIS Hellstern, T. R., Kibsgaard, J., Tsai, C., Palm, D. W., King, L. A., Abild-Pedersen, F., Jaramillo, T. F. 2017; 7 (10): 7126–30
  • Rh-MnO Interface Sites Formed by Atomic Layer Deposition Promote Syngas Conversion to Higher Oxygenates ACS CATALYSIS Yang, N., Yoo, J., Schumann, J., Bothra, P., Singh, J. A., Valle, E., Abild-Pedersen, F., Norskov, J. K., Bent, S. F. 2017; 7 (9): 5746–57
  • Theoretical Insights into Methane C-H Bond Activation on Alkaline Metal Oxides JOURNAL OF PHYSICAL CHEMISTRY C Aljama, H., Norskov, J. K., Abild-Pedersen, F. 2017; 121 (30): 16440–46
  • A Theoretical Study of Methanol Oxidation on RuO2(110): Bridging the Pressure Gap ACS CATALYSIS Latimer, A. A., Abild-Pedersen, F., Norskov, J. K. 2017; 7 (7): 4527–34
  • Electrochemical generation of sulfur vacancies in the basal plane of MoS2 for hydrogen evolution NATURE COMMUNICATIONS Tsai, C., Li, H., Park, S., Park, J., Han, H. S., Norskov, J. K., Zheng, X., Abild-Pedersen, F. 2017; 8

    Abstract

    Recently, sulfur (S)-vacancies created on the basal plane of 2H-molybdenum disulfide (MoS2) using argon plasma exposure exhibited higher intrinsic activity for the electrochemical hydrogen evolution reaction than the edge sites and metallic 1T-phase of MoS2 catalysts. However, a more industrially viable alternative to the argon plasma desulfurization process is needed. In this work, we introduce a scalable route towards generating S-vacancies on the MoS2 basal plane using electrochemical desulfurization. Even though sulfur atoms on the basal plane are known to be stable and inert, we find that they can be electrochemically reduced under accessible applied potentials. This can be done on various 2H-MoS2 nanostructures. By changing the applied desulfurization potential, the extent of desulfurization and the resulting activity can be varied. The resulting active sites are stable under extended desulfurization durations and show consistent HER activity.

    View details for DOI 10.1038/ncomms15113

    View details for Web of Science ID 000399985300001

  • Theoretical study on oxidative coupling of methane using MgO Aljama, H., Norskov, J., Abild-Pedersen, F. AMER CHEMICAL SOC. 2017
  • Scaling Relations for Adsorption Energies on Doped Molybdenum Phosphide Surfaces ACS CATALYSIS Fields, M., Tsai, C., Chen, L. D., Abild-Pedersen, F., Norskov, J. K., Chan, K. 2017; 7 (4): 2528-2534
  • Modeling the Migration of Platinum Nanoparticles on Surfaces Using a Kinetic Monte Carlo Approach JOURNAL OF PHYSICAL CHEMISTRY C Li, L., Plessow, P. N., Rieger, M., Sauer, S., Sanchez-Carrera, R. S., Schaefer, A., Abild-Pedersen, F. 2017; 121 (8): 4261–69
  • Understanding trends in C-H bond activation in heterogeneous catalysis NATURE MATERIALS Latimer, A. A., Kulkarni, A. R., Aljama, H., Montoya, J. H., Yoo, J. S., Tsai, C., Abild-Pedersen, F., Studt, F., Norskov, J. K. 2017; 16 (2): 225-229

    Abstract

    While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.

    View details for DOI 10.1038/NMAT4760

    View details for Web of Science ID 000393349800016

  • Mechanistic insights into heterogeneous methane activation. Physical chemistry chemical physics Latimer, A. A., Aljama, H., Kakekhani, A., Yoo, J. S., Kulkarni, A., Tsai, C., Garcia-Melchor, M., Abild-Pedersen, F., Nørskov, J. K. 2017; 19 (5): 3575-3581

    Abstract

    While natural gas is an abundant chemical fuel, its low volumetric energy density has prompted a search for catalysts able to transform methane into more useful chemicals. This search has often been aided through the use of transition state (TS) scaling relationships, which estimate methane activation TS energies as a linear function of a more easily calculated descriptor, such as final state energy, thus avoiding tedious TS energy calculations. It has been shown that methane can be activated via a radical or surface-stabilized pathway, both of which possess a unique TS scaling relationship. Herein, we present a simple model to aid in the prediction of methane activation barriers on heterogeneous catalysts. Analogous to the universal radical TS scaling relationship introduced in a previous publication, we show that a universal TS scaling relationship that transcends catalysts classes also seems to exist for surface-stabilized methane activation if the relevant final state energy is used. We demonstrate that this scaling relationship holds for several reducible and irreducible oxides, promoted metals, and sulfides. By combining the universal scaling relationships for both radical and surface-stabilized methane activation pathways, we show that catalyst reactivity must be considered in addition to catalyst geometry to obtain an accurate estimation for the TS energy. This model can yield fast and accurate predictions of methane activation barriers on a wide range of catalysts, thus accelerating the discovery of more active catalysts for methane conversion.

    View details for DOI 10.1039/c6cp08003k

    View details for PubMedID 28094377

  • Bond Order Conservation Strategies in Catalysis Applied to the NH3 Decomposition Reaction ACS CATALYSIS Yu, L., Abild-Pedersen, F. 2017; 7 (1): 864-871
  • Methanol Partial Oxidation on Ag(111) from First Principles CHEMCATCHEM Aljama, H., Yoo, J. S., Norskov, J. K., Abild-Pedersen, F., Studt, F. 2016; 8 (23): 3621-3625
  • Direct and continuous strain control of catalysts with tunable battery electrode materials SCIENCE Wang, H., Xu, S., Tsai, C., Li, Y., Liu, C., Zhao, J., Liu, Y., Yuan, H., Abild-Pedersen, F., Prinz, F. B., Norskov, J. K., Cui, Y. 2016; 354 (6315): 1031-1036

    Abstract

    We report a method for using battery electrode materials to directly and continuously control the lattice strain of platinum (Pt) catalyst and thus tune its catalytic activity for the oxygen reduction reaction (ORR). Whereas the common approach of using metal overlayers introduces ligand effects in addition to strain, by electrochemically switching between the charging and discharging status of battery electrodes the change in volume can be precisely controlled to induce either compressive or tensile strain on supported catalysts. Lattice compression and tension induced by the lithium cobalt oxide substrate of ~5% were directly observed in individual Pt nanoparticles with aberration-corrected transmission electron microscopy. We observed 90% enhancement or 40% suppression in Pt ORR activity under compression or tension, respectively, which is consistent with theoretical predictions.

    View details for DOI 10.1126/science.aaf7680

    View details for PubMedID 27885028

  • Understanding trends in C-H bond activation in heterogeneous catalysis. Nature materials Latimer, A. A., Kulkarni, A. R., Aljama, H., Montoya, J. H., Yoo, J. S., Tsai, C., Abild-Pedersen, F., Studt, F., Nørskov, J. K. 2016

    Abstract

    While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.

    View details for DOI 10.1038/nmat4760

    View details for PubMedID 27723737

  • Two-Dimensional Materials as Catalysts for Energy Conversion CATALYSIS LETTERS Siahrostami, S., Tsai, C., Karamad, M., Koitz, R., Garcia-Melchor, M., Bajdich, M., Vojvodic, A., Abild-Pedersen, F., Norskov, J. K., Studt, F. 2016; 146 (10): 1917-1921
  • Sintering of Pt Nanoparticles via Volatile PtO2: Simulation and Comparison with Experiments ACS CATALYSIS Plessow, P. N., Abild-Pedersen, F. 2016; 6 (10): 7098–7108
  • Elucidating the electronic structure of supported gold nanoparticles and its relevance to catalysis by means of hard X-ray photoelectron spectroscopy SURFACE SCIENCE Reinecke, B. N., Kuhl, K. P., Ogasawara, H., Li, L., Voss, J., Abild-Pedersen, F., Nilsson, A., Jaramillo, T. F. 2016; 650: 24-33
  • Dynamical Observation and Detailed Description of Catalysts under Strong Metal-Support Interaction NANO LETTERS Zhang, S., Plessow, P. N., Willis, J. J., Dai, S., Xu, M., Graham, G. W., Cargnello, M., Abild-Pedersen, F., Pan, X. 2016; 16 (7): 4528-4534

    Abstract

    Understanding the structures of catalysts under realistic conditions with atomic precision is crucial to design better materials for challenging transformations. Under reducing conditions, certain reducible supports migrate onto supported metallic particles and create strong metal-support states that drastically change the reactivity of the systems. The details of this process are still unclear and preclude its thorough exploitation. Here, we report an atomic description of a palladium/titania (Pd/TiO2) system by combining state-of-the-art in situ transmission electron microscopy and density functional theory (DFT) calculations with structurally defined materials, in which we visualize the formation of the overlayers at the atomic scale under atmospheric pressure and high temperature. We show that an amorphous reduced titania layer is formed at low temperatures, and that crystallization of the layer into either mono- or bilayer structures is dictated by the reaction environment and predicted by theory. Furthermore, it occurs in combination with a dramatic reshaping of the metallic surface facets.

    View details for DOI 10.1021/acs.nanolett.6b01769

    View details for Web of Science ID 000379794200081

    View details for PubMedID 27280326

  • Modeling the Interface of Platinum and alpha-Quartz(001): Implications for Sintering JOURNAL OF PHYSICAL CHEMISTRY C Plessow, P. N., Sanchez-Carrera, R. S., Li, L., Rieger, M., Sauer, S., Schaefer, A., Abild-Pedersen, F. 2016; 120 (19): 10340-10350
  • Trends in the Thermodynamic Stability of Ultrathin Supported Oxide Films JOURNAL OF PHYSICAL CHEMISTRY C Plessow, P. N., Bajdich, M., Greene, J., Vojvodic, A., Abild-Pedersen, F. 2016; 120 (19): 10351–60
  • Chemical and Phase Evolution of Amorphous Molybdenum Sulfide Catalysts for Electrochemical Hydrogen Production. ACS nano Lee, S. C., Benck, J. D., Tsai, C., Park, J., Koh, A. L., Abild-Pedersen, F., Jaramillo, T. F., Sinclair, R. 2016; 10 (1): 624-632

    Abstract

    Amorphous MoSx is a highly active, earth-abundant catalyst for the electrochemical hydrogen evolution reaction. Previous studies have revealed that this material initially has a composition of MoS3, but after electrochemical activation, the surface is reduced to form an active phase resembling MoS2 in composition and chemical state. However, structural changes in the MoSx catalyst and the mechanism of the activation process remain poorly understood. In this study, we employ transmission electron microscopy (TEM) to image amorphous MoSx catalysts activated under two hydrogen-rich conditions: ex situ in an electrochemical cell and in situ in an environmental TEM. For the first time, we directly observe the formation of crystalline domains in the MoSx catalyst after both activation procedures as well as spatially localized changes in the chemical state detected via electron energy loss spectroscopy. Using density functional theory calculations, we investigate the mechanisms for this phase transformation and find that the presence of hydrogen is critical for enabling the restructuring process. Our results suggest that the surface of the amorphous MoSx catalyst is dynamic: while the initial catalyst activation forms the primary active surface of amorphous MoS2, continued transformation to the crystalline phase during electrochemical operation could contribute to catalyst deactivation. These results have important implications for the application of this highly active electrocatalyst for sustainable H2 generation.

    View details for DOI 10.1021/acsnano.5b05652

    View details for PubMedID 26624225

  • Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies NATURE MATERIALS Li, H., Tsai, C., Koh, A. L., Cai, L., Contryman, A. W., Fragapane, A. H., Zhao, J., Han, H. S., Manoharan, H. C., Abild-Pedersen, F., Norskov, J. K., Zheng, X. 2016; 15 (1): 48-?

    Abstract

    As a promising non-precious catalyst for the hydrogen evolution reaction (HER; refs ,,,,), molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.

    View details for DOI 10.1038/NMAT4465

    View details for Web of Science ID 000366690600019

    View details for PubMedID 26552057

  • Theoretical insights into the hydrogen evolution activity of layered transition metal dichalcogenides SURFACE SCIENCE Tsai, C., Chan, K., Norskov, J. K., Abild-Pedersen, F. 2015; 640: 133-140
  • Surface Tension Effects on the Reactivity of Metal Nanoparticles JOURNAL OF PHYSICAL CHEMISTRY LETTERS Li, L., Abild-Pedersen, F., Greeley, J., Norskov, J. K. 2015; 6 (19): 3797-3801

    Abstract

    We present calculated adsorption energies of oxygen on gold and platinum clusters with up to 923 atoms (3 nm diameter) using density functional theory. We find that surface tension of the clusters induces a compression, which weakens the bonding of adsorbates compared with the bonding on extended surfaces. The effect is largest for close-packed surfaces and almost nonexistent on the more reactive steps and edges. The effect is largest at low coverage and decreases, even changing sign, at higher coverages where the strain changes from compressive to tensile. Quantum size effects also influence adsorption energies but only below a critical size of 1.5 nm for platinum and 2.5 nm for gold. We develop a model to describe the strain-induced size effects on adsorption energies, which is able to describe the influence of surface structure, adsorbate, metal, and coverage.

    View details for DOI 10.1021/acs.jpclett.5b01746

    View details for Web of Science ID 000362391000004

  • Predicting Promoter-Induced Bond Activation on Solid Catalysts Using Elementary Bond Orders JOURNAL OF PHYSICAL CHEMISTRY LETTERS Tsai, C., Latimer, A. A., Yoo, J. S., Studt, F., Abild-Pedersen, F. 2015; 6 (18): 3670-3674

    Abstract

    In this Letter, we examine bond activation induced by nonmetal surface promoters in the context of dehydrogenation reactions. We use C-H bond activation in methane dehydrogenation on transition metals as an example to understand the origin of the promoting or poisoning effect of nonmetals. The electronic structure of the surface and the bond order of the promoter are found to establish all trends in bond activation. On the basis of these results, we develop a predictive model that successfully describes the energetics of C-H, O-H, and N-H bond activation across a range of reactions. For a given reaction step, a single data point determines whether a nonmetal will promote bond activation or poison the surface and by how much. We show how our model leads to general insights that can be directly used to predict bond activation energetics on transition metal sulfides and oxides, which can be perceived as promoted surfaces. These results can then be directly used in studies on full catalytic pathways.

    View details for DOI 10.1021/acs.jpclett.5b01792

    View details for Web of Science ID 000361858800025

  • From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis JOURNAL OF CATALYSIS Medford, A. J., Vojvodic, A., Hummelshoj, J. S., Voss, J., Abild-Pedersen, F., Studt, F., Bligaard, T., Nilsson, A., Norskov, J. K. 2015; 328: 36-42
  • Hydrogenation of CO2 to methanol and CO on Cu/ZnO/Al2O3: Is there a common intermediate or not? JOURNAL OF CATALYSIS Kunkes, E. L., Studt, F., Abild-Pedersen, F., Schloegl, R., Behrens, M. 2015; 328: 43–48
  • Toward Controlled Growth of Helicity-Specific Carbon Nanotubes JOURNAL OF PHYSICAL CHEMISTRY LETTERS Santos, E. J., Norskov, J. K., Harutyunyan, A. R., Abild-Pedersen, F. 2015; 6 (12): 2232-2237

    Abstract

    The underlying mechanisms for the nucleation of carbon nanotubes as well as their helicity, remain elusive. Here, using van der Waals dispersion force calculations implemented within density functional theory, we study the cap formation, believed to be responsible for the chirality of surface-catalyzed carbon nanotubes. We find the energetics associated with growth along different facets to be independent of the surface orientation and that the growth across an edge along the axis of the metal particle leads to a perfect honeycomb lattice in a curved geometry. The formation of defects in the graphene matrix, which bend the carbon plane, requires that two or more graphene embryos with significantly different growth axis merge. Such scenario is only possible at the front- or back-end of the metal particle where growth symmetry is broken. The graphene embryos reconstruct their hexagonal structure into pentagons, heptagons, and octagons counterpart to accommodate the tube curvature.

    View details for DOI 10.1021/acs.jpclett.5b00880

    View details for Web of Science ID 000356758100013

  • Examining the Linearity of Transition State Scaling Relations JOURNAL OF PHYSICAL CHEMISTRY C Plessow, P. N., Abild-Pedersen, F. 2015; 119 (19): 10448-10453
  • The Mechanism of CO and CO2 Hydrogenation to Methanol over Cu-Based Catalysts CHEMCATCHEM Studt, F., Behrens, M., Kunkes, E. L., Thomas, N., Zander, S., Tarasov, A., Schumann, J., Frei, E., Varley, J. B., Abild-Pedersen, F., Norskov, J. K., Schloegl, R. 2015; 7 (7): 1105-1111
  • Catalyst design principles: An application to the steam reforming of methane Abild-Pedersen, F., Bligaard, T., Studt, F., Norskov, J. AMER CHEMICAL SOC. 2015
  • Transition-metal doped edge sites in vertically aligned MoS2 catalysts for enhanced hydrogen evolution NANO RESEARCH Wang, H., Tsai, C., Kong, D., Chan, K., Abild-Pedersen, F., Norskov, J. K., Cui, Y. 2015; 8 (2): 566-575
  • On the role of the surface oxygen species during A-H (A = C, N, O) bond activation: a density functional theory study. Chemical communications Yoo, J. S., Khan, T. S., Abild-Pedersen, F., Nørskov, J. K., Studt, F. 2015; 51 (13): 2621-2624

    Abstract

    During A-H (A = C, N, O) bond cleavage on O* or OH* pre-covered (111) surfaces, the oxygen species play the role of modifying the reaction energy by changing the species involved in the initial and final states of the reaction.

    View details for DOI 10.1039/c4cc08658a

    View details for PubMedID 25571859

  • Rational design of MoS2 catalysts: tuning the structure and activity via transition metal doping CATALYSIS SCIENCE & TECHNOLOGY Tsai, C., Chan, K., Norskov, J. K., Abild-Pedersen, F. 2015; 5 (1): 246-253

    View details for DOI 10.1039/c4cy01162g

    View details for Web of Science ID 000348358200027

  • Designing an improved transition metal phosphide catalyst for hydrogen evolution using experimental and theoretical trends ENERGY & ENVIRONMENTAL SCIENCE Kibsgaard, J., Tsai, C., Chan, K., Benck, J. D., Norskov, J. K., Abild-Pedersen, F., Jaramillo, T. F. 2015; 8 (10): 3022-3029

    View details for DOI 10.1039/c5ee02179k

    View details for Web of Science ID 000362351700024

  • Operando Characterization of an Amorphous Molybdenum Sulfide Nanoparticle Catalyst during the Hydrogen Evolution Reaction JOURNAL OF PHYSICAL CHEMISTRY C Casalongue, H. G., Benck, J. D., Tsai, C., Karlsson, R. K., Kaya, S., Ng, M. L., Pettersson, L. G., Abild-Pedersen, F., Norskov, J. K., Ogasawara, H., Jaramillo, T. F., Nilsson, A. 2014; 118 (50): 29252-29259

    View details for DOI 10.1021/jp505394e

    View details for Web of Science ID 000346759300037

  • Understanding the Reactivity of Layered Transition-Metal Sulfides: A Single Electronic Descriptor for Structure and Adsorption JOURNAL OF PHYSICAL CHEMISTRY LETTERS Tsai, C., Chan, K., Norskov, J. K., Abild-Pedersen, F. 2014; 5 (21): 3884-3889

    Abstract

    Density functional theory is used to investigate the adsorption and structural properties of layered transition-metal sulfide (TMS) catalysts. We considered both the (101̅0) M-edge and (1̅010) S-edge terminations for a wide range of pure and doped TMSs, determined their sulfur coverage under realistic operating conditions (i.e, steady-state structures), and calculated an extensive set of chemisorption energies for several important reactions. On the basis of these results, we show that the d-band center, εd, of the edge-most metal site at 0 ML sulfur coverage is a general electronic descriptor for both structure and adsorption energies, which are known to describe catalytic activity. A negative linear correlation between adsorbate-S binding and S-metal binding allows εd to describe the adsorption of species on both metal and sulfur sites. Our results provide a significant simplification in the understanding of structure-activity relationships in TMSs and provides guidelines for the rational design and large-scale screening of these catalysts for various processes.

    View details for DOI 10.1021/jz5020532

    View details for Web of Science ID 000344579500041

  • Energetics of the Water-Gas-Shift Reaction on the Active Sites of the Industrially Used Cu/ZnO/Al2O3 Catalyst CATALYSIS LETTERS Studt, F., Behrens, M., Abild-Pedersen, F. 2014; 144 (11): 1973–77
  • Insights into carbon nanotube nucleation: Cap formation governed by catalyst interfacial step flow SCIENTIFIC REPORTS Rao, R., Sharma, R., Abild-Pedersen, F., Norskov, J. K., Harutyunyan, A. R. 2014; 4

    Abstract

    In order to accommodate an increasing demand for carbon nanotubes (CNTs) with desirable characteristics one has to understand the origin of helicity of their structures. Here, through in situ microscopy we demonstrate that the nucleation of a carbon nanotube is initiated by the formation of the carbon cap. Nucleation begins with the formation of a graphene embryo that is bound between opposite step-edges on the nickel catalyst surface. The embryo grows larger as the step-edges migrate along the surface, leading to the formation of a curved carbon cap when the steps flow across the edges of adjacent facets. Further motion of the steps away from the catalyst tip with attached rims of the carbon cap generates the wall of the nanotube. Density Functional Theory calculations bring further insight into the process, showing that step flow occurs by surface self diffusion of the nickel atoms via a step-edge attachment-detachment mechanism. Since the cap forms first in the sequence of stages involved in growth, we suggest that it originates the helicity of the nanotube. Therefore, the angular distribution of catalyst facets could be exploited as a new parameter for controlling the curvature of the cap and, presumably, the helicity of the nanotube.

    View details for DOI 10.1038/srep06510

    View details for Web of Science ID 000343083200001

    View details for PubMedID 25308821

    View details for PubMedCentralID PMC4194440

  • Implications of uncertainty on computationally predicted rates and trends in catalytic ammonia synthesis Medford, A. J., Wellendorff, J., Vojvodic, A., Abild-Pedersen, F., Studt, F., Jacobsen, K., Bligaard, T., Norskov, J. K. AMER CHEMICAL SOC. 2014
  • Inherent Enhancement of Electronic Emission from Hexaboride Heterostructure PHYSICAL REVIEW APPLIED Voss, J., Vojvodic, A., Chou, S. H., Howe, R. T., Abild-Pedersen, F. 2014; 2 (2)
  • Catalysis. Assessing the reliability of calculated catalytic ammonia synthesis rates. Science Medford, A. J., Wellendorff, J., Vojvodic, A., Studt, F., Abild-Pedersen, F., Jacobsen, K. W., Bligaard, T., Nørskov, J. K. 2014; 345 (6193): 197-200

    Abstract

    We introduce a general method for estimating the uncertainty in calculated materials properties based on density functional theory calculations. We illustrate the approach for a calculation of the catalytic rate of ammonia synthesis over a range of transition-metal catalysts. The correlation between errors in density functional theory calculations is shown to play an important role in reducing the predicted error on calculated rates. Uncertainties depend strongly on reaction conditions and catalyst material, and the relative rates between different catalysts are considerably better described than the absolute rates. We introduce an approach for incorporating uncertainty when searching for improved catalysts by evaluating the probability that a given catalyst is better than a known standard.

    View details for DOI 10.1126/science.1253486

    View details for PubMedID 25013071

  • Active edge sites in MoSe2 and WSe2 catalysts for the hydrogen evolution reaction: a density functional study. Physical chemistry chemical physics Tsai, C., Chan, K., Abild-Pedersen, F., Nørskov, J. K. 2014; 16 (26): 13156-13164

    Abstract

    MoSe2 and WSe2 nanofilms and nanosheets have recently been shown to be active for electrochemical H2 evolution (HER). In this work, we used periodic density functional theory to investigate the origin of the catalytic activity on these materials. We determined the relevant structures of the Mo/W-edges and the Se-edges under HER conditions and their differential hydrogen adsorption free energies. The Mo-edge on MoSe2 and the Se-edge on both MoSe2 and WSe2 are found to be the predominantly active facets for these catalysts, with activity predicted to be comparable to or better than MoS2. On the other hand, the (0001) basal planes are found to be inert. We further explain the enhanced activity at the edges in terms of localized edge states, which provide insight into the trends in HER activity seen between the two catalysts. Our results thus suggest that an optimal catalyst design should maximize the exposure of edge sites. Comparisons are also made between the transition metal selenide catalysts and their sulfide counterparts in order to understand the consequences of having either Mo/W or Se/S atoms. It is found that linear scaling relations describe the S/Se binding onto the edge and the H binding onto the S/Se.

    View details for DOI 10.1039/c4cp01237b

    View details for PubMedID 24866567

  • DFT Study of Atomically-Modified Alkali-Earth Metal Oxide Films on Tungsten JOURNAL OF PHYSICAL CHEMISTRY C Chou, S. H., Voss, J., Vojvodic, A., Howe, R. T., Abild-Pedersen, F. 2014; 118 (21): 11303-11309

    View details for DOI 10.1021/jp4120578

    View details for Web of Science ID 000336771700017

  • Exploring the limits: A low-pressure, low-temperature Haber-Bosch process CHEMICAL PHYSICS LETTERS Vojvodic, A., Medford, A. J., Studt, F., Abild-Pedersen, F., Khan, T. S., Bligaard, T., Norskov, J. K. 2014; 598: 108-112
  • Theoretical Analysis of Transition-Metal Catalysts for Formic Acid Decomposition ACS CATALYSIS Yoo, J. S., Abild-Pedersen, F., Norskov, J. K., Studt, F. 2014; 4 (4): 1226-1233

    View details for DOI 10.1021/cs400664z

    View details for Web of Science ID 000338807100024

  • Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol NATURE CHEMISTRY Studt, F., Sharafutdinov, I., Abild-Pedersen, F., Elkjaer, C. F., Hummelshoj, J. S., Dahl, S., Chorkendorff, I., Norskov, J. K. 2014; 6 (4): 320-324

    Abstract

    The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni5Ga3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al2O3 catalysts revealed the same or better methanol synthesis activity, as well as considerably lower production of CO. We suggest that this is a first step towards the development of small-scale low-pressure devices for CO2 reduction to methanol.

    View details for DOI 10.1038/NCHEM.1873

    View details for Web of Science ID 000333396200022

    View details for PubMedID 24651199

  • Finite-size effects on gold and platinum clusters Li, L., Larsen, A. H., Romero, N. A., Abild-Pedersen, F., Greeley, J. P., Norskov, J. K. AMER CHEMICAL SOC. 2014
  • Effects of d-band shape on the surface reactivity of transition-metal alloys PHYSICAL REVIEW B Xin, H., Vojvodic, A., Voss, J., Norskov, J. K., Abild-Pedersen, F. 2014; 89 (11)
  • Tuning the MoS2 Edge-Site Activity for Hydrogen Evolution via Support Interactions. Nano letters Tsai, C., Abild-Pedersen, F., Nørskov, J. K. 2014; 14 (3): 1381-1387

    Abstract

    The hydrogen evolution reaction (HER) on supported MoS2 catalysts is investigated using periodic density functional theory, employing the new BEEF-vdW functional that explicitly takes long-range van der Waals (vdW) forces into account. We find that the support interactions involving vdW forces leads to significant changes in the hydrogen binding energy, resulting in several orders of magnitude difference in HER activity. It is generally seen for the Mo-edge that strong adhesion of the catalyst onto the support leads to weakening in the hydrogen binding. This presents a way to optimally tune the hydrogen binding on MoS2 and explains the lower than expected exchange current densities of supported MoS2 in electrochemical H2 evolution studies.

    View details for DOI 10.1021/nl404444k

    View details for PubMedID 24499163

  • Activity and Selectivity Trends in Synthesis Gas Conversion to Higher Alcohols TOPICS IN CATALYSIS Medford, A. J., Lausche, A. C., Abild-Pedersen, F., Temel, B., Schjodt, N. C., Norskov, J. K., Studt, F. 2014; 57 (1-4): 135-142
  • In silico search for novel methane steam reforming catalysts NEW JOURNAL OF PHYSICS Xu, Y., Lausche, A. C., Wang, S., Khan, T. S., Abild-Pedersen, F., Studt, F., Norskov, J. K., Bligaard, T. 2013; 15
  • On the effect of coverage-dependent adsorbate-adsorbate interactions for CO methanation on transition metal surfaces JOURNAL OF CATALYSIS Lausche, A. C., Medford, A. J., Khan, T. S., Xu, Y., Bligaard, T., Abild-Pedersen, F., Norskov, J. K., Studt, F. 2013; 307: 275-282
  • Density functional theory studies of transition metal nanoparticles in catalysis Greeley, J., Rankin, R., Zeng, Z., Chun, H., Clayborne, A., Li, L., Abild-Pedersen, F., Norskov, J., Larsen, A., Kleis, J., Jacobsen, K., Romero, N. AMER CHEMICAL SOC. 2013
  • Interlayer Carbon Bond Formation Induced by Hydrogen Adsorption in Few-Layer Supported Graphene PHYSICAL REVIEW LETTERS Rajasekaran, S., Abild-Pedersen, F., Ogasawara, H., Nilsson, A., Kaya, S. 2013; 111 (8)

    Abstract

    We report on the hydrogen adsorption induced phase transition of a few layer graphene (1 to 4 layers) to a diamondlike structure on Pt(111) based on core level x-ray spectroscopy, temperature programed desorption, infrared spectroscopy, and density functional theory total energy calculations. The surface adsorption of hydrogen induces a hybridization change of carbon from the sp^{2} to the sp^{3} bond symmetry, which propagates through the graphene layers, resulting in interlayer carbon bond formation. The structure is stabilized through the termination of interfacial sp^{3} carbon atoms by the substrate. The structural transformation occurs as a consequence of high adsorption energy.

    View details for DOI 10.1103/PhysRevLett.111.085503

    View details for Web of Science ID 000323388200016

    View details for PubMedID 24010453

  • Stability of Pt-Modified Cu(111) in the Presence of Oxygen and Its Implication on the Overall Electronic Structure JOURNAL OF PHYSICAL CHEMISTRY C Oberg, H., Anniyev, T., Vojvodic, A., Kaya, S., Ogasawara, H., Friebel, D., Miller, D. J., Nordlund, D., Bergmann, U., Ljungberg, M. P., Abild-Pedersen, F., Nilsson, A., Pettersson, L. G. 2013; 117 (32): 16371-16380

    View details for DOI 10.1021/jp400486r

    View details for Web of Science ID 000323301100012

  • Analysis of sulfur-induced selectivity changes for anhydrous methanol dehydrogenation on Ni(100) surfaces SURFACE SCIENCE Lausche, A. C., Abild-Pedersen, F., Madix, R. J., Norskov, J. K., Studt, F. 2013; 613: 58-62
  • Thermionic current densities from first principles. journal of chemical physics Voss, J., Vojvodic, A., Chou, S. H., Howe, R. T., Bargatin, I., Abild-Pedersen, F. 2013; 138 (20): 204701-?

    Abstract

    We present a density functional theory-based method for calculating thermionic emission currents from a cathode into vacuum using a non-equilibrium Green's function approach. It does not require semi-classical approximations or crude simplifications of the electronic structure used in previous methods and thus provides quantitative predictions of thermionic emission for adsorbate-coated surfaces. The obtained results match well with experimental measurements of temperature-dependent current densities. Our approach can thus enable computational design of composite electrode materials.

    View details for DOI 10.1063/1.4805002

    View details for PubMedID 23742494

  • Comment on "Using Photoelectron Spectroscopy and Quantum Mechanics to Determine d-Band Energies of Metals for Catalytic Applications" JOURNAL OF PHYSICAL CHEMISTRY C Abild-Pedersen, F., Nilsson, A., Norskov, J. K. 2013; 117 (13): 6914-6915

    View details for DOI 10.1021/jp312595p

    View details for Web of Science ID 000317317600050

  • Bronsted-Evans-Polanyi Relationship for Transition Metal Carbide and Transition Metal Oxide Surfaces JOURNAL OF PHYSICAL CHEMISTRY C Vines, F., Vojvodic, A., Abild-Pedersen, F., Illas, F. 2013; 117 (8): 4168–71

    View details for DOI 10.1021/jp312671z

    View details for Web of Science ID 000318211800055

  • Electronic Origin of the Surface Reactivity of Transition-Metal-Doped TiO2(110) JOURNAL OF PHYSICAL CHEMISTRY C Garcia-Mota, M., Vojvodic, A., Abild-Pedersen, F., Norskov, J. K. 2013; 117 (1): 460-465

    View details for DOI 10.1021/jp310667r

    View details for Web of Science ID 000313220700059

  • Investigation of Catalytic Finite-Size-Effects of Platinum Metal Clusters JOURNAL OF PHYSICAL CHEMISTRY LETTERS Li, L., Larsen, A. H., Romero, N. A., Morozov, V. A., Glinsvad, C., Abild-Pedersen, F., Greeley, J., Jacobsen, K. W., Norskov, J. K. 2013; 4 (1): 222-226

    Abstract

    In this paper, we use density functional theory (DFT) calculations on highly parallel computing resources to study size-dependent changes in the chemical and electronic properties of platinum (Pt) for a number of fixed freestanding clusters ranging from 13 to 1415 atoms, or 0.7-3.5 nm in diameter. We find that the surface catalytic properties of the clusters converge to the single crystal limit for clusters with as few as 147 atoms (1.6 nm). Recently published results for gold (Au) clusters showed analogous convergence with size. However, this convergence happened at larger sizes, because the Au d-states do not contribute to the density of states around the Fermi-level, and the observed level fluctuations were not significantly damped until the cluster reached ca. 560 atoms (2.7 nm) in size.

    View details for DOI 10.1021/jz3018286

    View details for Web of Science ID 000313142000032

  • CO and CO2 Hydrogenation to Methanol Calculated Using the BEEF-vdW Functional CATALYSIS LETTERS Studt, F., Abild-Pedersen, F., Varley, J. B., Norskov, J. K. 2013; 143 (1): 71-73
  • Energetics of Oxygen Adatoms, Hydroxyl Species and Water Dissociation on Pt(111) JOURNAL OF PHYSICAL CHEMISTRY C Karp, E. M., Campbell, C. T., Studt, F., Abild-Pedersen, F., Nerskov, J. K. 2012; 116 (49): 25772-25776

    View details for DOI 10.1021/jp3066794

    View details for Web of Science ID 000312176100015

  • Elementary steps of syngas reactions on Mo2C(0 0 1): Adsorption thermochemistry and bond dissociation (vol 290, pg 108, 2012) JOURNAL OF CATALYSIS Medford, A. J., Vojvodic, A., Studt, F., Abild-Pedersen, F., Norskov, J. K. 2012; 296: 175-175
  • An orbital-overlap model for minimal work functions of cesiated metal surfaces JOURNAL OF PHYSICS-CONDENSED MATTER Chou, S. H., Voss, J., Bargatin, I., Vojvodic, A., Howe, R. T., Abild-Pedersen, F. 2012; 24 (44)

    Abstract

    We introduce a model for the effect of cesium adsorbates on the work function of transition metal surfaces. The model builds on the classical point-dipole equation by adding exponential terms that characterize the degree of orbital overlap between the 6s states of neighboring cesium adsorbates and its effect on the strength and orientation of electric dipoles along the adsorbate-substrate interface. The new model improves upon earlier models in terms of agreement with the work function-coverage curves obtained via first-principles calculations based on density functional theory. All the cesiated metal surfaces have optimal coverages between 0.6 and 0.8 monolayers, in accordance with experimental data. Of all the cesiated metal surfaces that we have considered, tungsten has the lowest minimum work function, also in accordance with experiments.

    View details for DOI 10.1088/0953-8984/24/44/445007

    View details for Web of Science ID 000310571100009

    View details for PubMedID 23018485

  • Volcano Relations for Oxidation of Hydrogen Halides over Rutile Oxide Surfaces CHEMCATCHEM Toftelund, A., Man, I. C., Hansen, H. A., Abild-Pedersen, F., Bligaard, T., Rossmeisl, J., Studt, F. 2012; 4 (11): 1856–61
  • CO hydrogenation to methanol on Cu-Ni catalysts: Theory and experiment JOURNAL OF CATALYSIS Studt, F., Abild-Pedersen, F., Wu, Q., Jensen, A. D., Temel, B., Grunwaldt, J., Norskov, J. K. 2012; 293: 51-60
  • Reversible graphene-metal contact through hydrogenation PHYSICAL REVIEW B Rajasekaran, S., Kaya, S., Abild-Pedersen, F., Anniyev, T., Yang, F., Stacchiola, D., Ogasawara, H., Nilsson, A. 2012; 86 (7)
  • Application of a new informatics tool in heterogeneous catalysis: Analysis of methanol dehydrogenation on transition metal catalysts for the production of anhydrous formaldehyde JOURNAL OF CATALYSIS Lausche, A. C., Hummelshoj, J. S., Abild-Pedersen, F., Studt, F., Norskov, J. K. 2012; 291: 133-137
  • Elementary steps of syngas reactions on Mo2C(001): Adsorption thermochemistry and bond dissociation JOURNAL OF CATALYSIS Medford, A. J., Vojvodic, A., Studt, F., Abild-Pedersen, F., Norskov, J. K. 2012; 290: 108-117
  • The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts SCIENCE Behrens, M., Studt, F., Kasatkin, I., Kuehl, S., Haevecker, M., Abild-Pedersen, F., Zander, S., Girgsdies, F., Kurr, P., Kniep, B., Tovar, M., Fischer, R. W., Norskov, J. K., Schloegl, R. 2012; 336 (6083): 893-897

    Abstract

    One of the main stumbling blocks in developing rational design strategies for heterogeneous catalysis is that the complexity of the catalysts impairs efforts to characterize their active sites. We show how to identify the crucial atomic structure motif for the industrial Cu/ZnO/Al(2)O(3) methanol synthesis catalyst by using a combination of experimental evidence from bulk, surface-sensitive, and imaging methods collected on real high-performance catalytic systems in combination with density functional theory calculations. The active site consists of Cu steps decorated with Zn atoms, all stabilized by a series of well-defined bulk defects and surface species that need to be present jointly for the system to work.

    View details for DOI 10.1126/science.1219831

    View details for Web of Science ID 000304145600059

    View details for PubMedID 22517324

  • CatApp: A web application for surface chemistry and heterogeneous catalysis 11th International Biorelated Polymer Symposium / 243rd National Spring Meeting of the American-Chemical-Society (ACS) Hummelshoj, J. S., Abild-Pedersen, F., Studt, F., Bligaard, T., Norskov, J. K. AMER CHEMICAL SOC. 2012
  • Scaling relations applied to synthetic fuel production Wang, S., Khan, T. S., Jones, G., Andersson, M. P., Falsig, H., Grabow, L. C., Abild-Pedersen, F., Studt, F., Norskov, J. K., Bligaard, T. AMER CHEMICAL SOC. 2012
  • Catalyst design on the computer Norskov, J. K., Bligaard, T., Studt, F., Abild-Pedersen, F. AMER CHEMICAL SOC. 2012
  • A theoretical evaluation of possible transition metal electro-catalysts for N-2 reduction PHYSICAL CHEMISTRY CHEMICAL PHYSICS Skulason, E., Bligaard, T., Gudmundsdottir, S., Studt, F., Rossmeisl, J., Abild-Pedersen, F., Vegge, T., Jonsson, H., Norskov, J. K. 2012; 14 (3): 1235-1245

    Abstract

    Theoretical studies of the possibility of forming ammonia electrochemically at ambient temperature and pressure are presented. Density functional theory calculations were used in combination with the computational standard hydrogen electrode to calculate the free energy profile for the reduction of N(2) admolecules and N adatoms on several close-packed and stepped transition metal surfaces in contact with an acidic electrolyte. Trends in the catalytic activity were calculated for a range of transition metal surfaces and applied potentials under the assumption that the activation energy barrier scales with the free energy difference in each elementary step. The most active surfaces, on top of the volcano diagrams, are Mo, Fe, Rh, and Ru, but hydrogen gas formation will be a competing reaction reducing the faradaic efficiency for ammonia production. Since the early transition metal surfaces such as Sc, Y, Ti, and Zr bind N-adatoms more strongly than H-adatoms, a significant production of ammonia compared with hydrogen gas can be expected on those metal electrodes when a bias of -1 V to -1.5 V vs. SHE is applied. Defect-free surfaces of the early transition metals are catalytically more active than their stepped counterparts.

    View details for DOI 10.1039/c1cp22271f

    View details for Web of Science ID 000299271800015

  • CatApp: A Web Application for Surface Chemistry and Heterogeneous Catalysis ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Hummelshoj, J. S., Abild-Pedersen, F., Studt, F., Bligaard, T., Norskov, J. K. 2012; 51 (1): 272-274

    View details for DOI 10.1002/anie.201107947

    View details for Web of Science ID 000298598500049

    View details for PubMedID 22162297

  • Scaling relationships for adsorption energies of C-2 hydrocarbons on transition metal surfaces CHEMICAL ENGINEERING SCIENCE Jones, G., Studt, F., Abild-Pedersen, F., Norskov, J. K., Bligaard, T. 2011; 66 (24): 6318-6323
  • Scaling relations applied to synthetic fuel production 242nd National Meeting of the American-Chemical-Society (ACS) Wang, S., Jones, G., Andersson, M. P., Falsig, H., Grabow, L. C., Abild-Pedersen, F., Studt, F., Norskov, J. K., Bligaard, T. AMER CHEMICAL SOC. 2011
  • On the activity and selectivity of syngas conversion processes 242nd National Meeting of the American-Chemical-Society (ACS) Studt, F., Abild-Pedersen, F., Norskov, J. K. AMER CHEMICAL SOC. 2011
  • Structure effects on the energetics of the electrochemical reduction of CO2 by copper surfaces SURFACE SCIENCE Durand, W. J., Peterson, A. A., Studt, F., Abild-Pedersen, F., Norskov, J. K. 2011; 605 (15-16): 1354-1359
  • Br(A)over-tilde,nsted-Evans-Polanyi relations for transition-metal oxides from density functional theory 241st National Meeting and Exposition of the American-Chemical-Society (ACS) Vojvodic, A., Calle-Vallejo, F., Abild-Pedersen, F., Guo, W., Wang, S., Toftelund, A., Studt, F., Martinez, J. I., Shen, J., Man, I. C., Rossmeisl, J., Bligaard, T., Norskov, J. K. AMER CHEMICAL SOC. 2011
  • Understanding selectivity in syngas reactions 241st National Meeting and Exposition of the American-Chemical-Society (ACS) Norskov, J. K., Studt, F., Abild-Pedersen, F. AMER CHEMICAL SOC. 2011
  • Universal Bronsted-Evans-Polanyi Relations for C-C, C-O, C-N, N-O, N-N, and O-O Dissociation Reactions CATALYSIS LETTERS Wang, S., Temel, B., Shen, J., Jones, G., Grabow, L. C., Studt, F., Bligaard, T., Abild-Pedersen, F., Christensen, C. H., Norskov, J. K. 2011; 141 (3): 370-373
  • First-principles investigations of Ni3Al(111) and NiAl(110) surfaces at metal dusting conditions SURFACE SCIENCE Saadi, S., Hinnemann, B., Appel, C. C., Helveg, S., Abild-Pedersen, F., Norskov, J. K. 2011; 605 (5-6): 582-592
  • Density functional theory in surface chemistry and catalysis PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Norskov, J. K., Abild-Pedersen, F., Studt, F., Bligaard, T. 2011; 108 (3): 937-943

    Abstract

    Recent advances in the understanding of reactivity trends for chemistry at transition-metal surfaces have enabled in silico design of heterogeneous catalysts in a few cases. The current status of the field is discussed with an emphasis on the role of coupling theory and experiment and future challenges.

    View details for DOI 10.1073/pnas.1006652108

    View details for Web of Science ID 000286310300013

    View details for PubMedID 21220337

    View details for PubMedCentralID PMC3024687

  • Descriptor-Based Analysis Applied to HCN Synthesis from NH3 and CH4 ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Grabow, L. C., Studt, F., Abild-Pedersen, F., Petzold, V., Kleis, J., Bligaard, T., Norskov, J. K. 2011; 50 (20): 4601-4605

    View details for DOI 10.1002/anie.201100353

    View details for Web of Science ID 000290663600007

    View details for PubMedID 21500324

  • How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels ENERGY & ENVIRONMENTAL SCIENCE Peterson, A. A., Abild-Pedersen, F., Studt, F., Rossmeisl, J., Norskov, J. K. 2010; 3 (9): 1311-1315

    View details for DOI 10.1039/c0ee00071j

    View details for Web of Science ID 000282334000016

  • On the Role of Metal Step-Edges in Graphene Growth JOURNAL OF PHYSICAL CHEMISTRY C Saadi, S., Abild-Pedersen, F., Helveg, S., Sehested, J., Hinnemann, B., Appel, C. C., Norskov, J. K. 2010; 114 (25): 11221-11227

    View details for DOI 10.1021/jp1033596

    View details for Web of Science ID 000278982300031

  • Self Blocking of CO Dissociation on a Stepped Ruthenium Surface TOPICS IN CATALYSIS Vendelbo, S. B., Johansson, M., Mowbray, D. J., Andersson, M. P., Abild-Pedersen, F., Nielsen, J. H., Norskov, J. K., Chorkendorff, I. 2010; 53 (5-6): 357-364
  • Electrochemical chlorine evolution at rutile oxide (110) surfaces PHYSICAL CHEMISTRY CHEMICAL PHYSICS Hansen, H. A., Man, I. C., Studt, F., Abild-Pedersen, F., Bligaard, T., Rossmeisl, J. 2010; 12 (1): 283–90

    Abstract

    Based on density functional theory (DFT) calculations we study the electrochemical chlorine evolution reaction on rutile (110) oxide surfaces. First we construct the Pourbaix surface diagram for IrO(2) and RuO(2), and from this we find the chlorine evolution reaction intermediates and identify the lowest overpotential at which all elementary reaction steps in the chlorine evolution reaction are downhill in free energy. This condition is then used as a measure for catalytic activity. Linear scaling relations between the binding energies of the intermediates and the oxygen binding energies at cus-sites are established for MO(2) (M being Ir, Ru, Pt, Ti). The linear relations form the basis for constructing a generalized surface phase diagram where two parameters, the potential and the binding energy of oxygen, are needed to determine the surface composition. We calculate the catalytic activity as function of the oxygen binding energy, giving rise to a Sabatier volcano. By combining the surface phase diagram and the volcano describing the catalytic activity, we find that the reaction mechanism differs depending on catalyst material. The flexibility in reaction path means that the chlorine evolution activity is high for a wide range of oxygen binding energies. We find that the required overpotential for chlorine evolution is lower than the overpotential necessary for oxygen evolution.

    View details for DOI 10.1039/b917459a

    View details for Web of Science ID 000272589000032

    View details for PubMedID 20024470

  • Volcano Relation for the Deacon Process over Transition-Metal Oxides CHEMCATCHEM Studt, F., Abild-Pedersen, F., Hansen, H. A., Man, I. C., Rossmeisl, J., Bligaard, T. 2010; 2 (1): 98–102
  • CATALYSIS Bond control in surface reactions NATURE Norskov, J. K., Abild-Pedersen, F. 2009; 461 (7268): 1223–25

    View details for DOI 10.1038/4611223a

    View details for Web of Science ID 000271190800035

    View details for PubMedID 19865160

  • First-principles investigations of the Ni3Sn alloy at steam reforming conditions SURFACE SCIENCE Saadi, S., Hinnemann, B., Helveg, S., Appel, C. C., Abild-Pedersen, F., Norskov, J. K. 2009; 603 (5): 762-770
  • Trends for Methane Oxidation at Solid Oxide Fuel Cell Conditions JOURNAL OF THE ELECTROCHEMICAL SOCIETY Kleis, J., Jones, G., Abild-Pedersen, F., Tripkovic, V., Bligaard, T., Rossmeisl, J. 2009; 156 (12): B1447–B1456

    View details for DOI 10.1149/1.3230622

    View details for Web of Science ID 000271218900024

  • Virtual materials design using databases of calculated materials properties. Computational Science and Discovery Munter, T. R., Landis, D. D., Abild-Pedersen, F., Jones, G., Bligaard, T. 2009; 2: 27
  • The nature of the active site in heterogeneous metal catalysis CHEMICAL SOCIETY REVIEWS Norskov, J. K., Bligaard, T., Hvolbaek, B., Abild-Pedersen, F., Chorkendorff, I., Christensen, C. H. 2008; 37 (10): 2163-2171

    Abstract

    This tutorial review, of relevance for the surface science and heterogeneous catalysis communities, provides a molecular-level discussion of the nature of the active sites in metal catalysis. Fundamental concepts such as "Brønsted-Evans-Polanyi relations" and "volcano curves" are introduced, and are used to establish a strict partitioning between the so-called "electronic" and "geometrical" effects. This partitioning is subsequently employed as the basis for defining the concept "degree of structure sensitivity" which can be used when analyzing the structure sensitivity of catalytic reactions.

    View details for DOI 10.1039/b800260f

    View details for Web of Science ID 000259505600003

    View details for PubMedID 18818819

  • First principles calculations and experimental insight into methane steam reforming over transition metal catalysts JOURNAL OF CATALYSIS Jones, G., Jakobsen, J. G., Shim, S. S., Kleis, J., Andersson, M. P., Rossmeisl, J., Abild-Pedersen, F., Bligaard, T., Helveg, S., Hinnemann, B., Rostrup-Nielsen, J. R., Chorkendorff, I., Sehested, J., Norskov, J. K. 2008; 259 (1): 147-160
  • Identification of non-precious metal alloy catalysts for selective hydrogenation of acetylene SCIENCE Studt, F., Abild-Pedersen, F., Bligaard, T., Sorensen, R. Z., Christensen, C. H., Norskov, J. K. 2008; 320 (5881): 1320-1322

    Abstract

    The removal of trace acetylene from ethylene is performed industrially by palladium hydrogenation catalysts (often modified with silver) that avoid the hydrogenation of ethylene to ethane. In an effort to identify catalysts based on less expensive and more available metals, density functional calculations were performed that identified relations in heats of adsorption of hydrocarbon molecules and fragments on metal surfaces. This analysis not only verified the facility of known catalysts but identified nickel-zinc alloys as alternatives. Experimental studies demonstrated that these alloys dispersed on an oxide support were selective for acetylene hydrogenation at low pressures.

    View details for DOI 10.1126/science.1156660

    View details for Web of Science ID 000256441100039

    View details for PubMedID 18535238

  • Structure sensitivity of the methanation reaction: H-2-induced CO dissociation on nickel surfaces JOURNAL OF CATALYSIS Andersson, M. P., Abild-Pedersen, E., Remediakis, I. N., Bligaard, T., Jones, G., Engbwk, J., Lytken, O., Horch, S., Nielsen, J. H., Sehested, J., Rostrup-Nielsen, J. R., Norskov, J. K., Chorkendorff, I. 2008; 255 (1): 6-19
  • Using scaling relations to understand trends in the catalytic activity of transition metals 2nd Workshop on Theory Meets Industry Jones, G., Bligaard, T., Abild-Pedersen, F., Norskov, J. K. IOP PUBLISHING LTD. 2008

    Abstract

    A method is developed to estimate the potential energy diagram for a full catalytic reaction for a range of late transition metals on the basis of a calculation (or an experimental determination) for a single metal. The method, which employs scaling relations between adsorption energies, is illustrated by calculating the potential energy diagram for the methanation reaction and ammonia synthesis for 11 different metals on the basis of results calculated for Ru. It is also shown that considering the free energy diagram for the reactions, under typical industrial conditions, provides additional insight into reactivity trends.

    View details for DOI 10.1088/0953-8984/20/6/064239

    View details for Web of Science ID 000252927300040

    View details for PubMedID 21693900

  • On the Role of Surface Modifications of Palladium Catalysts in the Selective Hydrogenation of Acetylene International Symposium on Creation and Control of Advanced Selective Catalysis Studt, F., Abild-Pedersen, F., Bligaard, T., Sorensen, R. Z., Christensen, C. H., Norskov, J. K. WILEY-V C H VERLAG GMBH. 2008: 9299–9302

    View details for DOI 10.1002/anie.200802844

    View details for Web of Science ID 000261445900023

    View details for PubMedID 18833559

  • Scaling relationships for adsorption energies on transition metal oxide, sulfide, and nitride surfaces ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Fernandez, E. M., Moses, P. G., Toftelund, A., Hansen, H. A., Martinez, J. I., Abild-Pedersen, F., Kleis, J., Hinnemann, B., Rossmeisl, J., Bligaard, T., Norskov, J. K. 2008; 47 (25): 4683-4686

    View details for DOI 10.1002/anie.200705739

    View details for Web of Science ID 000256894600012

    View details for PubMedID 18484577

  • Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces PHYSICAL REVIEW LETTERS Abild-Pedersen, F., Greeley, J., Studt, F., Rossmeisl, J., Munter, T. R., Moses, P. G., Skulason, E., Bligaard, T., Norskov, J. K. 2007; 99 (1)

    Abstract

    Density functional theory calculations are presented for CHx, x=0,1,2,3, NHx, x=0,1,2, OHx, x=0,1, and SHx, x=0,1 adsorption on a range of close-packed and stepped transition-metal surfaces. We find that the adsorption energy of any of the molecules considered scales approximately with the adsorption energy of the central, C, N, O, or S atom, the scaling constant depending only on x. A model is proposed to understand this behavior. The scaling model is developed into a general framework for estimating the reaction energies for hydrogenation and dehydrogenation reactions.

    View details for DOI 10.1103/PhysRevLett.99.016105

    View details for Web of Science ID 000247819900029

    View details for PubMedID 17678168

  • CO adsorption energies on metals with correction for high coordination adsorption sites - A density functional study SURFACE SCIENCE Abild-Pedersen, F., Andersson, M. P. 2007; 601 (7): 1747–53
  • Carbide induced reconstruction of monatomic steps on Ni(111) - A density functional study SURFACE SCIENCE Andersson, M. P., Abild-Pedersen, F. 2007; 601 (3): 649–55
  • Mechanisms for catalytic carbon nanofiber growth studied by ab initio density functional theory calculations PHYSICAL REVIEW B Abild-Pedersen, F., Norskov, J. K., Rostrup-Nielsen, J. R., Sehested, J., Helveg, S. 2006; 73 (11)
  • Understanding the effect of steps, strain, poisons, and alloying: Methane activation on Ni surfaces CATALYSIS LETTERS Abild-Pedersen, F., Greeley, J., Norskov, J. K. 2005; 105 (1-2): 9-13
  • Methane activation on Ni(111): Effects of poisons and step defects SURFACE SCIENCE Abild-Pedersen, F., Lytken, O., Engbaek, J., Nielsen, G., Chorkendorff, I., Norskov, J. K. 2005; 590 (2-3): 127-137
  • DFT study of formaldehyde and methanol synthesis from CO and H-2 on Ni(111) JOURNAL OF PHYSICAL CHEMISTRY B Remediakis, I. N., Abild-Pedersen, F., Norskov, J. K. 2004; 108 (38): 14535-14540

    View details for DOI 10.1021/jp0493374

    View details for Web of Science ID 000223922500044

  • Atomic-scale imaging of carbon nanofibre growth NATURE Helveg, S., Lopez-Cartes, C., Sehested, J., Hansen, P. L., Clausen, B. S., Rostrup-Nielsen, J. R., Abild-Pedersen, F., Norskov, J. K. 2004; 427 (6973): 426-429

    Abstract

    The synthesis of carbon nanotubes with predefined structure and functionality plays a central role in the field of nanotechnology, whereas the inhibition of carbon growth is needed to prevent a breakdown of industrial catalysts for hydrogen and synthesis gas production. The growth of carbon nanotubes and nanofibres has therefore been widely studied. Recent advances in in situ techniques now open up the possibility of studying gas-solid interactions at the atomic level. Here we present time-resolved, high-resolution in situ transmission electron microscope observations of the formation of carbon nanofibres from methane decomposition over supported nickel nanocrystals. Carbon nanofibres are observed to develop through a reaction-induced reshaping of the nickel nanocrystals. Specifically, the nucleation and growth of graphene layers are found to be assisted by a dynamic formation and restructuring of mono-atomic step edges at the nickel surface. Density-functional theory calculations indicate that the observations are consistent with a growth mechanism involving surface diffusion of carbon and nickel atoms. The finding that metallic step edges act as spatiotemporal dynamic growth sites may be important for understanding other types of catalytic reactions and nanomaterial syntheses.

    View details for DOI 10.1038/nature02278

    View details for Web of Science ID 000188470500038

    View details for PubMedID 14749826