Adam Nielander

All Publications

• Stabilization of molybdenum in CMP: Operando insights into distinct inhibitor adsorption pathways JOURNAL OF ELECTROANALYTICAL CHEMISTRY Choi, S., Lee, D., Kreider, M. E., Nielander, A. C., Stevens, M., Park, D., Hong, I., Park, K., Bae, K., Kim, H., Yoon, B., Kim, S., Jaramillo, T. F., Lee, K. 2025; 996

  View details for DOI 10.1016/j.jelechem.2025.119377

  View details for Web of Science ID 001549855500001

• Controlling Chloride Crossover in Bipolar Membrane Water Electrolysis. ACS electrochemistry Rochow, M. F., Marin, D. H., Cassady, H. J., Hannagan, R. T., Yan, K., Perryman, J. T., Nielander, A. C., Jaramillo, T. F., Hickner, M. A. 2025; 1 (9): 1812-1820

  Abstract

  Bipolar membranes (BPMs) are increasingly recognized as a promising electrolyte option for water electrolysis, attributable to their distinctive properties derived from the membrane's layered structure, which consists of an anion exchange (AEL) and a cation exchange layer (CEL). This study investigates four different BPMs and the influence they have on the performance of a water electrolysis cell under two different feed configurations: (1) a symmetric deionized water feed to both anode and cathode compartments and (2) an asymmetric feed with a 0.5 mol/L NaCl catholyte feed and a deionized water anolyte feed. The BPMs were also investigated for total chlorine (Cl) species (e.g., Cl-, Cl2, HOCl, and ClO-) in the anolyte due to Cl- crossover from the catholyte during water electrolysis with the asymmetric feed, at an applied current density of 250 mA/cm2. The best-performing BPM with the asymmetric feed was an E98-05 (CEL)/FAS-50 (AEL) membrane with a TiO2 water dissociation catalyst at the BPM junction. This membrane had the lowest measured Cl species crossover and lowest cell voltage at a given current density under asymmetric conditions compared to the other BPMs studied. It was also found that under asymmetric conditions the CEL facing the catholyte feed determined the amount of total Cl species crossover due to anion exclusion (Donnan exclusion) of the CEL, reducing the amount of Cl- in the CEL where it crossed over to the AEL and the anolyte compartment.

  View details for DOI 10.1021/acselectrochem.5c00175

  View details for PubMedID 40927531

  View details for PubMedCentralID PMC12415932

• Chemistry of Materials Underpinning Photoelectrochemical Solar Fuel Production CHEMICAL REVIEWS Schichtl, Z. G., Carvalho, O., Tan, J., Saund, S. S., Ghoshal, D., Wilder, L. M., Gish, M. K., Nielander, A. C., Stevens, M., Greenaway, A. L. 2025

  Abstract

  Since its inception, photoelectrochemistry has sought to power the generation of fuels, particularly hydrogen, using energy from sunlight. Efficient and durable photoelectrodes, however, remain elusive. Here we review the current state of the art, focusing our discussion on advances in photoelectrodes made in the past decade. We open by briefly discussing fundamental photoelectrochemical concepts and implications for photoelectrode function. We next review a broad range of semiconductor photoelectrodes broken down by material class (oxides, nitrides, chalcogenides, and mature photovoltaic semiconductors), identifying intrinsic properties and discussing their influence on performance. We then identify innovative in situ and operando techniques to directly probe the photoelectrode|electrolyte interface, enabling direct assessment of structure-property relationships for catalytic surfaces in active reaction environments. We close by considering more complex photoelectrochemical fuel-forming reactions (carbon dioxide and nitrogen reduction, as well as alternative oxidation reactions), where product selectivity imposes additional criteria on electrochemical driving force and photoelectrode architecture. By contextualizing recent literature within a fundamental framework, we seek to provide direction for continued progress toward achieving efficient and stable fuel-forming photoelectrodes.

  View details for DOI 10.1021/acs.chemrev.4c00258

  View details for Web of Science ID 001482456300001

  View details for PubMedID 40327786

• CO₂ Oxidative Ethane Dehydrogenation on CeO₂/SiO₂-Supported NiFe₃ Catalysts CHEMCATCHEM Spurlock, R., Erdem, E., Lee, S., Chen, J., Gallo, A., Nielander, A. C., Jaramillo, T. F. 2025

  View details for DOI 10.1002/cctc.202402030

  View details for Web of Science ID 001477129300001

• In Situ Neutron Reflectometry Reveals the Interfacial Microenvironment Driving Electrochemical Ammonia Synthesis. Journal of the American Chemical Society Niemann, V. A., Doucet, M., Benedek, P., Deissler, N. H., Mygind, J. B., Lee, S. W., Rios Amador, I., Willoughby, W. L., Chorkendorff, I., Nielander, A. C., Tarpeh, W. A., Jaramillo, T. F. 2025

  Abstract

  Electrified interfaces are critical to the performance of energy systems and often demonstrate substantial complexity under operating conditions. A nanoscale understanding of the interfacial microenvironment, i.e., the solid-electrolyte interphase (SEI), in lithium-mediated nitrogen reduction (Li-N2R) is key for realizing efficient ammonia (NH3) production. Herein, we used time-resolved neutron reflectometry (NR) to observe SEI formation under Li-N2R conditions. We found that the LiBF4-based electrolyte provided a substantially more well-defined SEI layer than previous SEI NR interrogations that used LiClO4, highlighting the underlying chemistry that dictates electrolyte design and enabling new NR-based studies. Using in situ NR, we found that the LiBF4-derived SEI under Li-N2R conditions comprises a thick, diffuse outer layer and a thin, compact inner layer at low current cycling (<2 mA/cm2), revealing a structure which ex situ studies have not been able to probe. Increased current cycling and sustained current cycling led to the merging of the layers into a single-layer SEI. We used isotope contrast methods with d6-EtOH and d8-THF to drive time-resolved tracking of SEI growth at low current cycling, revealing that the proton donor modifies the inner layer, and the solvent modifies the outer layer. Li dendritic growth was observed in the absence of a proton donor. Neutron absorption also indicated the presence of boron in the SEI, underscoring the value of neutron-based interrogation. Our results inform Li-based systems and reaction microenvironments, and these methods can be applied broadly to interfacial energy technologies.

  View details for DOI 10.1021/jacs.4c16636

  View details for PubMedID 40172240

• Temperature-dependent solid electrolyte interphase reactions drive performance in lithium-mediated nitrogen reduction to ammonia JOULE Benedek, P., Cornejo-Carrillo, Y. E., O'Rafferty, A. H., Niemann, V. A., Lee, S., Mcshane, E. J., Cargnello, M., Niel, A. C., Jaramillo, T. F. 2025; 9 (3)

  View details for DOI 10.1016/j.joule.2024.101810

  View details for Web of Science ID 001450564700001

• Multimodal In Situ Characterization Uncovers Unexpected Stability of a Cobalt Electrocatalyst for Acidic Sustainable Energy Technologies. Journal of the American Chemical Society Aleman, A. M., Crago, C. F., Kamat, G. A., Mule, A. S., Avilés Acosta, J. E., Matthews, J. E., Keyes, N., Hannagan, R. T., Nielander, A. C., Stevens, M. B., Jaramillo, T. F. 2025

  Abstract

  An accelerated development of durable and affordable sustainable energy technologies is often hindered by a limited understanding of how nonprecious materials within these systems degrade. In acidic proton exchange membrane fuel cells and water electrolyzers, metallic cobalt (Co) is considered an unstable component that is often combined with precious metals or other stabilizers. To understand the mechanisms behind Co instability, we employ an experimental platform that quantifies dissolution with on-line inductively coupled plasma mass spectrometry and product formation with electrochemical mass spectrometry during electrochemical testing, along with ex situ characterization. Under varied conditions (electrocatalysis, time, gas-type saturation, and ion concentration), windows of Co stability are observed that are different than predicted with classical chemical thermodynamics, suggesting new stabilization and degradation mechanisms than previously understood. Notably, Co is active for the hydrogen evolution reaction (HER), with prolonged stability that is ∼300 mV greater than thermodynamically projected. Additionally, in an oxygenated environment, Co concurrently performs the HER and the oxygen reduction reaction (ORR) yet undergoes different morphology changes and dissolution mechanisms. Interestingly, at open-circuit voltage, there is a 22× decrease in dissolution in an oxygen-free environment, proposing a route to decrease Co losses during device shutdown protocols. Lastly, under more extreme operating conditions, Co becomes stable after a substantial amount of dissolution, suggesting that high concentrations of Co2+ ions in the microenvironment induce the formation of a stable CoHO2 surface. Altogether, these results can be leveraged to improve the design and development of more robust and cost-effective sustainable energy technologies, as well as promote strategic strategies for prolonged material utilization.

  View details for DOI 10.1021/jacs.4c16707

  View details for PubMedID 40079839

• On-line Inductively Coupled Plasma Mass Spectrometry Reveals Material Degradation Dynamics of Au and Cu Catalysts during Electrochemical CO2 Reduction. Journal of the American Chemical Society Yan, K., Lee, S. W., Yap, K. M., Mule, A. S., Hannagan, R. T., Matthews, J. E., Kamat, G. A., Lee, D. U., Stevens, M. B., Nielander, A. C., Jaramillo, T. F. 2025

  Abstract

  A significant challenge in commercializing electrochemical CO2 reduction (CO2R) is achieving catalyst durability. In this study, online inductively coupled mass spectrometry (ICP-MS) was used to investigate catalyst degradation via nanoparticle detachment and/or dissolution into metal ions under CO2R operating conditions in 0.1 M KHCO3. We developed an experimental framework with ex situ characterization to validate the online ICP-MS method for in situ evaluation of degradation from metal foils. By varying the applied potential and microenvironment (CO2 vs N2-saturated electrolyte), we gained insights into the degradation of Au and Cu foils under CO2R and hydrogen evolution reaction (HER) conditions. While both Au and Cu foils were observed to be stable to dissolution in these regimes, degradation via nanoparticle detachment from the foil surface at the femtogram scale was observed as a function of reaction conditions, providing new insights into material degradation mechanisms. When applying potential steps at -0.1 and -1.0 V vs the reversible hydrogen electrode (RHE), Au was found to degrade via nanoparticle detachment under CO2R operating conditions more than under HER conditions, while Cu was found to degrade via nanoparticle detachment in similar amounts during both reactions. Au lost ∼1.8× more mass and ∼7.5× more nanoparticles than Cu under CO2R operating conditions. This study demonstrates the use of online ICP-MS to gain insight into the degradation of Au and Cu, the importance of studying unconventional degradation mechanisms such as nanoparticle detachment, and that online ICP-MS can be further utilized to gain fundamental understanding of catalyst durability for a variety of reaction systems.

  View details for DOI 10.1021/jacs.4c13233

  View details for PubMedID 39871661

• Structural Transformation and Degradation of Cu Oxide Nanocatalysts during Electrochemical CO2 Reduction. Journal of the American Chemical Society Lee, S. H., Avilés Acosta, J. E., Lee, D., Larson, D. M., Li, H., Chen, J., Lee, J., Erdem, E., Lee, D. U., Blair, S. J., Gallo, A., Zheng, H., Nielander, A. C., Tassone, C. J., Jaramillo, T. F., Drisdell, W. S. 2025

  Abstract

  The electrochemical CO2 reduction reaction (CO2RR) holds enormous potential as a carbon-neutral route to the sustainable production of fuels and platform chemicals. The durability for long-term operation is currently inadequate for commercialization, however, and the underlying deactivation process remains elusive. A fundamental understanding of the degradation mechanism of electrocatalysts, which can dictate the overall device performance, is needed. In this work, we report the structural dynamics and degradation pathway of Cu oxide nanoparticles (CuOx NPs) during the CO2RR by using in situ small-angle X-ray scattering (SAXS) and X-ray absorption spectroscopy (XAS). The in situ SAXS reveals a reduction in the size of NPs when subjected to a potential at which no reaction products are detected. At potentials where the CO2RR starts to occur, CuOx NPs are agglomerated through a particle migration and coalescence process in the early stage of the reaction, followed by Ostwald ripening (OR) as the dominant degradation mechanism for the remainder of the reaction. As the applied potential becomes more negative, the OR process becomes more dominant, and for the most negative applied potential, OR dominates for the entire reaction time. The morphological changes are linked to a gradual decrease in the formation rate for multicarbon products (C2H4 and ethanol). Other reaction parameters, including reaction intermediates and local high pH, induce changes in the agglomeration process and final morphology of the CuOx NPs electrode, supported by post-mortem ex situ microscopic analysis. The in situ XAS analysis suggests that the CuOx NPs reduced into the metallic state before the structural transformation was observed. The introduction of high surface area carbon supports with ionomer coating mitigates the degree of structural transformation and detachment of the CuOx NPs electrode. These findings show the dynamic nature of Cu nanocatalysts during the CO2RR and can serve as a rational guideline toward a stable catalyst system under electrochemical conditions.

  View details for DOI 10.1021/jacs.4c14720

  View details for PubMedID 39815387

• <i>Operando</i> Surface-Enhanced Infrared Spectroscopy Connects Interfacial Dynamics with Reaction Kinetics During Electrochemical CO₂ Reduction on Copper ACS CATALYSIS Matthews, J. E., Acosta, J., Lee, S., Oh, D., Lin, T. Y., Yap, K. M. K., Chen, J., Jang, J., Lee, D., Nielander, A. C., Jaramillo, T. F. 2024

  View details for DOI 10.1021/acscatal.4c05532

  View details for Web of Science ID 001380955800001

• Electrodialysis and nitrate reduction (EDNR) to enable distributed ammonia manufacturing from wastewaters ENERGY & ENVIRONMENTAL SCIENCE Guo, J., Liu, M. J., Laguna, C., Miller, D. M., Williams, K. S., Clark, B. D., Munoz, C., Blair, S. J., Nielander, A. C., Jaramillo, T. F., Tarpeh, W. A. 2024

  View details for DOI 10.1039/d4ee03002h

  View details for Web of Science ID 001338143700001

• CO₂ Conversion to Butene via a Tandem Photovoltaic-Electrochemical/Photothermocatalytic Process: A Co-design Approach to Coupled Microenvironments ACS ENERGY LETTERS Yap, K. M. K., Aitbekova, A., Salazar, M., Kistler, T. A., Pabon, M., Su, M. P., Watkins, N. B., Lee, S., Agbo, P., Weber, A. Z., Peters, J. C., Agapie, T., Nielander, A. C., Atwater, H. A., Jaramillo, T. F., Bell, A. T. 2024

  View details for DOI 10.1021/acsenergylett.4c01866

  View details for Web of Science ID 001292243900001

• Author Correction: Alkali cation-induced cathodic corrosion in Cu electrocatalysts. Nature communications Liu, S., Li, Y., Wang, D., Xi, S., Xu, H., Wang, Y., Li, X., Zang, W., Liu, W., Su, M., Yan, K., Nielander, A. C., Wong, A. B., Lu, J., Jaramillo, T. F., Wang, L., Canepa, P., He, Q. 2024; 15 (1): 6092

  View details for DOI 10.1038/s41467-024-50241-z

  View details for PubMedID 39030201

  View details for PubMedCentralID PMC11259566

• Sub-volt conversion of activated biochar and water for H2 2 production near equilibrium via biochar-assisted water electrolysis CELL REPORTS PHYSICAL SCIENCE Kani, N. C., Chauhan, R., Olusegun, S. A., Sharan, I., Katiyar, A., House, D. W., Lee, S., Jairamsingh, A., Bhawnani, R. R., Choi, D., Nielander, A. C., Jaramillo, T. F., Lee, H., Oroskar, A., Srivastava, V. C., Sinha, S., Gauthier, J. A., Singh, M. R. 2024; 5 (6)

  View details for DOI 10.1016/j.xcrp.2024.102013

  View details for Web of Science ID 001293785400001

• Alkali cation-induced cathodic corrosion in Cu electrocatalysts. Nature communications Liu, S., Li, Y., Wang, D., Xi, S., Xu, H., Wang, Y., Li, X., Zang, W., Liu, W., Su, M., Yan, K., Nielander, A. C., Wong, A. B., Lu, J., Jaramillo, T. F., Wang, L., Canepa, P., He, Q. 2024; 15 (1): 5080

  Abstract

  The reconstruction of Cu catalysts during electrochemical reduction of CO2 is a widely known but poorly understood phenomenon. Herein, we examine the structural evolution of Cu nanocubes under CO2 reduction reaction and its relevant reaction conditions using identical location transmission electron microscopy, cyclic voltammetry, in situ X-ray absorption fine structure spectroscopy and ab initio molecular dynamics simulation. Our results suggest that Cu catalysts reconstruct via a hitherto unexplored yet critical pathway - alkali cation-induced cathodic corrosion, when the electrode potential is more negative than an onset value (e.g., -0.4 VRHE when using 0.1 M KHCO3). Having alkali cations in the electrolyte is critical for such a process. Consequently, Cu catalysts will inevitably undergo surface reconstructions during a typical process of CO2 reduction reaction, resulting in dynamic catalyst morphologies. While having these reconstructions does not necessarily preclude stable electrocatalytic reactions, they will indeed prohibit long-term selectivity and activity enhancement by controlling the morphology of Cu pre-catalysts. Alternatively, by operating Cu catalysts at less negative potentials in the CO electrochemical reduction, we show that Cu nanocubes can provide a much more stable selectivity advantage over spherical Cu nanoparticles.

  View details for DOI 10.1038/s41467-024-49492-7

  View details for PubMedID 38871724

  View details for PubMedCentralID 7810728

• Absolute band-edge energies are over-emphasized in the design of photoelectrochemical materials NATURE CATALYSIS Kaufman, A. J., Nielander, A. C., Meyer, G. J., Maldonado, S., Ardo, S., Boettcher, S. W. 2024; 7 (6): 615-623

  View details for DOI 10.1038/s41929-024-01161-0

  View details for Web of Science ID 001255620300014

• Modeling diurnal and annual ethylene generation from solar-driven electrochemical CO₂ reduction devices ENERGY & ENVIRONMENTAL SCIENCE Yap, K. M. K., Wei, W. J., Pabon, M., King, A. J., Bui, J. C., Wei, L., Lee, S., Weber, A. Z., Bell, A. T., Nielander, A. C., Jaramillo, T. F. 2024

  View details for DOI 10.1039/d4ee00545g

  View details for Web of Science ID 001176280900001

• Multi-scale physics of bipolar membranes in electrochemical processes NATURE CHEMICAL ENGINEERING Bui, J. C., Lees, E. W., Marin, D. H., Stovall, T., Chen, L., Kusoglu, A., Nielander, A. C., Jaramillo, T. F., Boettcher, S. W., Bell, A. T., Weber, A. Z. 2024; 1 (1): 45-60

  View details for DOI 10.1038/s44286-023-00009-x

  View details for Web of Science ID 001550568800008

• Protocol for assembling and operating bipolar membrane water electrolyzers. STAR protocols Rios Amador, I., Hannagan, R. T., Marin, D. H., Perryman, J. T., Rémy, C., Hubert, M. A., Lindquist, G. A., Chen, L., Stevens, M. B., Boettcher, S. W., Nielander, A. C., Jaramillo, T. F. 2023; 4 (4): 102606

  Abstract

  Renewable energy-driven bipolar membrane water electrolyzers (BPMWEs) are a promising technology for sustainable production of hydrogen from seawater and other impure water sources. Here, we present a protocol for assembling BPMWEs and operating them in a range of water feedstocks, including ultra-pure deionized water and seawater. We describe steps for membrane electrode assembly preparation, electrolyzer assembly, and electrochemical evaluation. For complete details on the use and execution of this protocol, please refer to Marin et al. (2023).1.

  View details for DOI 10.1016/j.xpro.2023.102606

  View details for PubMedID 37924520

• Calcium-mediated nitrogen reduction for electrochemical ammonia synthesis. Nature materials Fu, X., Niemann, V. A., Zhou, Y., Li, S., Zhang, K., Pedersen, J. B., Saccoccio, M., Andersen, S. Z., Enemark-Rasmussen, K., Benedek, P., Xu, A., Deissler, N. H., Mygind, J. B., Nielander, A. C., Kibsgaard, J., Vesborg, P. C., Norskov, J. K., Jaramillo, T. F., Chorkendorff, I. 2023

  Abstract

  Ammonia (NH3) is a key commodity chemical for the agricultural, textile and pharmaceutical industries, but its production via the Haber-Bosch process is carbon-intensive and centralized. Alternatively, an electrochemical method could enable decentralized, ambient NH3 production that can be paired with renewable energy. The first verified electrochemical method for NH3 synthesis was a process mediated by lithium (Li) in organic electrolytes. So far, however, elements other than Li remain unexplored in this process for potential benefits in efficiency, reaction rates, device design, abundance and stability. In our demonstration of a Li-free system, we found that calcium can mediate the reduction of nitrogen for NH3 synthesis. We verified the calcium-mediated process using a rigorous protocol and achieved an NH3 Faradaic efficiency of 40±2% using calcium tetrakis(hexafluoroisopropyloxy)borate (Ca[B(hfip)4]2) as the electrolyte. Our results offer the possibility of using abundant materials for the electrochemical production of NH3, a critical chemical precursor and promising energy vector.

  View details for DOI 10.1038/s41563-023-01702-1

  View details for PubMedID 37884670

• Quantifying Influence of the Solid-Electrolyte Interphase in Ammonia Electrosynthesis ACS ENERGY LETTERS Mcshane, E. J., Niemann, V. A., Benedek, P., Fu, X., Nielander, A. C., Chorkendorff, I., Jaramillo, T. F., Cargnello, M. 2023

  View details for DOI 10.1021/acsenergylett.3c01534

  View details for Web of Science ID 001062617200001

• Development of a versatile electrochemical cell for in situ grazing-incidence X-ray diffraction during non-aqueous electrochemical nitrogen reduction. Journal of synchrotron radiation Blair, S. J., Nielander, A. C., Stone, K. H., Kreider, M. E., Niemann, V. A., Benedek, P., McShane, E. J., Gallo, A., Jaramillo, T. F. 2023

  Abstract

  In situ techniques are essential to understanding the behavior of electrocatalysts under operating conditions. When employed, in situ synchrotron grazing-incidence X-ray diffraction (GI-XRD) can provide time-resolved structural information of materials formed at the electrode surface. In situ cells, however, often require epoxy resins to secure electrodes, do not enable electrolyte flow, or exhibit limited chemical compatibility, hindering the study of non-aqueous electrochemical systems. Here, a versatile electrochemical cell for air-free in situ synchrotron GI-XRD during non-aqueous Li-mediated electrochemical N2 reduction (Li-N2R) has been designed. This cell not only fulfills the stringent material requirements necessary to study this system but is also readily extendable to other electrochemical systems. Under conditions relevant to non-aqueous Li-N2R, the formation of Li metal, LiOH and Li2O as well as a peak consistent with the alpha-phase of Li3N was observed, thus demonstrating the functionality of this cell toward developing a mechanistic understanding of complicated electrochemical systems.

  View details for DOI 10.1107/S1600577523006331

  View details for PubMedID 37594864

• Combined, time-resolved, in situ neutron reflectometry and X-ray diffraction analysis of dynamic SEI formation during electrochemical N-2 reduction ENERGY & ENVIRONMENTAL SCIENCE Blair, S. J., Doucet, M., Niemann, V. A., Stone, K. H., Kreider, M. E., Browning, J. F., Halbert, C. E., Wang, H., Benedek, P., McShane, E. J., Nielander, A. C., Gallo, A., Jaramillo, T. F. 2023

  View details for DOI 10.1039/d2ee03694k

  View details for Web of Science ID 001018487700001

• A framework for understanding efficient diurnal CO2 reduction using Si and GaAs photocathodes CHEM CATALYSIS Yap, K. M. K., Lee, S., Steiner, M. A., Acosta, J., Kang, D., Kim, D., Warren, E. L., Nielander, A. C., Jaramillo, T. F. 2023; 3 (6)

  View details for DOI 10.1016/j.checat.2023.100641

  View details for Web of Science ID 001023692400001

• Co-designing Electrocatalytic Systems with Separations To Improve the Sustainability of Reactive Nitrogen Management ACS CATALYSIS Niemann, V. A., Benedek, P., Guo, J., Xu, Y., Blair, S. J., Corson, E. R., Nielander, A. C., Jaramillo, T. F., Tarpeh, W. A. 2023; 13 (9): 6268-6279

  View details for DOI 10.1021/acscatal.3c00933

  View details for Web of Science ID 000983745600001

• Hydrogen production with seawater-resilient bipolar membrane electrolyzers JOULE Marin, D. H., Perryman, J. T., Hubert, M. A., Lindquist, G. A., Chen, L., Aleman, A. M., Kamat, G. A., Niemann, V. A., Stevens, M., Regmi, Y. N., Boettcher, S. W., Nielander, A. C., Jaramillo, T. F. 2023; 7 (4): 765-781

  View details for DOI 10.1016/j.joule.2023.03.005

  View details for Web of Science ID 000988108000001

• Insights into Active Sites and Mechanisms of Benzyl Alcohol Oxidation on Nickel-Iron Oxyhydroxide Electrodes ACS CATALYSIS Wei, L., Hossain, M., Boyd, M. J., Aviles-Acosta, J., Kreider, M. E., Nielander, A. C., Stevens, M., Jaramillo, T. F., Bajdich, M., Hahn, C. 2023: 4272-4282

  View details for DOI 10.1021/acscatal.2c05656

  View details for Web of Science ID 000953973700001

• Reliable reporting of Faradaic efficiencies for electrocatalysis research. Nature communications Kempler, P. A., Nielander, A. C. 2023; 14 (1): 1158

  View details for DOI 10.1038/s41467-023-36880-8

  View details for PubMedID 36859528

• A Versatile Li0.5FePO4 Reference Electrode for Nonaqueous Electrochemical Conversion Technologies ACS ENERGY LETTERS McShane, E. J., Benedek, P., Niemann, V. A., Blair, S. J., Kamat, G. A., Nielander, A. C., Jaramillo, T. F., Cargnello, M. 2022: 230-235

  View details for DOI 10.1021/acsenergylett.2c02190

  View details for Web of Science ID 000891330700001

• Origins of wear-induced tungsten corrosion defects in semiconductor manufacturing during tungsten chemical mechanical polishing APPLIED SURFACE SCIENCE Choi, S., Kreider, M. E., Nielander, A. C., Stevens, M., Kamat, G., Koo, J., Bae, K., Kim, H., Yoon, I., Yoon, B., Hwang, K., Lee, D., Jaramillo, T. F. 2022; 598

  View details for DOI 10.1016/j.apsusc.2022.153767

  View details for Web of Science ID 000818529100002

• Lithium-Mediated Electrochemical Nitrogen Reduction: Tracking Electrode-Electrolyte Interfaces via Time-Resolved Neutron Reflectometry ACS ENERGY LETTERS Blair, S. J., Doucet, M., Browning, J. F., Stone, K., Wang, H., Halbert, C., Acosta, J., Zeledon, J., Nielander, A. C., Gallo, A., Jaramillo, T. F. 2022; 7 (6): 1939-1946

  View details for DOI 10.1021/acsenergylett.1c02833

  View details for Web of Science ID 000810534300001

• Characterizing Sustained Solar-to-Hydrogen Electrocatalysis at Low Cell Potentials Enabled by Crude Glycerol Oxidation ACS APPLIED ENERGY MATERIALS Schichtl, Z. G., Conlin, S. K., Mehrabi, H., Nielander, A. C., Coridan, R. H. 2022; 5 (3): 3863-3875

  View details for DOI 10.1021/acsaem.2c00377

  View details for Web of Science ID 000812979700001

• Demonstration of photoreactor platform for on-sun unassisted photoelectrochemical hydrogen generation with tandem III-V photoelectrodes CHEM CATALYSIS Ben-Naim, M., Aldridge, C. W., Steiner, M. A., Nielander, A. C., Deustch, T. G., Young, J. L., Jaramillo, T. F. 2022; 2 (1): 195-209

  View details for DOI 10.1016/j.checat.2021.12.013

  View details for Web of Science ID 000901338900018

• Engineering Surface Architectures for Improved Durability in III-V Photocathodes. ACS applied materials & interfaces Ben-Naim, M., Aldridge, C. W., Steiner, M. A., Britto, R. J., Nielander, A. C., King, L. A., Deutsch, T. G., Young, J. L., Jaramillo, T. F. 1800

  Abstract

  GaInP2 has shown promise as the wide bandgap top junction in tandem absorber photoelectrochemical (PEC) water splitting devices. Among previously reported dual-junction PEC devices with a GaInP2 top cell, those with the highest performance incorporate an AlInP2 window layer (WL) to reduce surface recombination and a thin GaInP2 capping layer (CL) to protect the WL from corrosion in electrolytes. However, the stability of these III-V systems is limited, and durability continues to be a major challenge broadly in the field of PEC water splitting. This work provides a systematic investigation into the durability of GaInP2 systems, examining the impacts of the window layer and capping layer among single junction pn-GaInP2 photocathodes coated with an MoS2 catalytic and protective layer. The photocathode with both a CL and WL demonstrates the highest PEC performance and longest lifetime, producing a significant current for >125 h. In situ optical imaging and post-test characterization illustrate the progression of macroscopic degradation and chemical state. The surface architecture combining an MoS2 catalyst, CL, and WL can be translated to dual-junction PEC devices with GaInP2 or other III-V top junctions to enable more efficient and stable PEC systems.

  View details for DOI 10.1021/acsami.1c18938

  View details for PubMedID 35005903

• Addressing the Stability Gap in Photoelectrochemistry: Molybdenum Disulfide Protective Catalysts for Tandem III-V Unassisted Solar Water Splitting ACS ENERGY LETTERS Ben-Naim, M., Britto, R. J., Aldridge, C. W., Mow, R., Steiner, M. A., Nielander, A. C., King, L. A., Friedman, D. J., Deutsch, T. G., Young, J. L., Jaramillo, T. F. 2020; 5 (8): 2631–40

  View details for DOI 10.1021/acsenergylett.0c01132

  View details for Web of Science ID 000562954100024

• A cyclic electrochemical strategy to produce acetylene from CO2, CH4, or alternative carbon sources SUSTAINABLE ENERGY & FUELS McEnaney, J. M., Rohr, B. A., Nielander, A. C., Singh, A. R., King, L. A., Norskov, J. K., Jaramillo, T. F. 2020; 4 (6): 2752–59

  View details for DOI 10.1039/c9se00799g

  View details for Web of Science ID 000539290400013

• A Combined Theory-Experiment Analysis of the Surface Species in Lithium-Mediated NH3 Electrosynthesis CHEMELECTROCHEM Schwalbe, J. A., Statt, M. J., Chosy, C., Singh, A. R., Rohr, B. A., Nielander, A. C., Andersen, S. Z., McEnaney, J. M., Baker, J. G., Jaramillo, T. F., Norskov, J. K., Cargnello, M. 2020; 7 (7): 1513

  View details for DOI 10.1002/celc.202000265

  View details for Web of Science ID 000525948800001

• Electrolyte Engineering for Efficient Electrochemical Nitrate Reduction to Ammonia on a Titanium Electrode ACS SUSTAINABLE CHEMISTRY & ENGINEERING McEnaney, J. M., Blair, S. J., Nielander, A. C., Schwalbe, J. A., Koshy, D. M., Cargnello, M., Jaramillo, T. F. 2020; 8 (7): 2672–81

  View details for DOI 10.1021/acssuschemeng.9b05983

  View details for Web of Science ID 000516665500010

• A Combined Theory-Experiment Analysis of the Surface Species in Lithium-Mediated NH3 Electrosynthesis CHEMELECTROCHEM Schwalbe, J. A., Statt, M. J., Chosy, C., Singh, A. R., Rohr, B. A., Nielander, A. C., Andersen, S. Z., McEnaney, J. M., Baker, J. G., Jaramillo, T. F., Norskov, J. K., Cargnello, M. 2020

  View details for DOI 10.1002/celc.201902124

  View details for Web of Science ID 000510258500001

• A Spin Coating Method To Deposit Iridium-Based Catalysts onto Silicon for Water Oxidation Photoanodes. ACS applied materials & interfaces Ben-Naim, M. n., Palm, D. W., Strickler, A. L., Nielander, A. C., Sanchez, J. n., King, L. A., Higgins, D. C., Jaramillo, T. F. 2020

  Abstract

  Silicon has shown promise for use as a small band gap (1.1 eV) absorber material in photoelectrochemical (PEC) water splitting. However, the limited stability of silicon in acidic electrolyte requires the use of protection strategies coupled with catalysts. Herein, spin coating is used as a versatile method to directly coat silicon photoanodes with an IrO x oxygen evolution reaction (OER) catalyst, reducing the processing complexity compared to conventional fabrication schemes. Biphasic strontium chloride/iridium oxide (SrCl2:IrO x ) catalysts are also developed, and both catalysts form photoactive junctions with silicon and demonstrate high photoanode activity. The iridium oxide photoanode displays a photocurrent onset at 1.06 V vs reversible hydrogen electrode (RHE), while the SrCl2:IrO x photoanode onsets earlier at 0.96 V vs RHE. The differing potentials are consistent with the observed photovoltages of 0.43 and 0.53 V for the IrO x and SrCl2:IrO x , respectively. By measuring the oxidation of a reversible redox couple, Fe(CN)63-/4-, we compare the charge carrier extraction of the devices and show that the addition of SrCl2 to the IrO x catalyst improves the silicon-electrolyte interface compared to pure IrO x . However, the durability of the strontium-containing photoanode remains a challenge, with its photocurrent density decreasing by 90% over 4 h. The IrO x photoanode, on the other hand, maintained a stable photocurrent density over this timescale. Characterization of the as-prepared and post-tested material structure via Auger electron spectroscopy identifies catalyst film cracking and delamination as the primary failure modes. We propose that improvements to catalyst adhesion should further the viability of spin coating as a technique for photoanode preparation.

  View details for DOI 10.1021/acsami.9b20099

  View details for PubMedID 31971770

• Readily Constructed Glass Piston Pump for Gas Recirculation. ACS omega Nielander, A. C., Blair, S. J., McEnaney, J. M., Schwalbe, J. A., Adams, T. n., Taheri, S. n., Wang, L. n., Yang, S. n., Cargnello, M. n., Jaramillo, T. F. 2020; 5 (27): 16455–59

  Abstract

  The recirculation of gases in a sealed reactor system is a broadly useful method in catalytic and electrocatalytic studies. It is especially relevant when a reactant gas reacts slowly with respect to residence time in a catalytic reaction zone and when mass transport control through the reaction zone is necessary. This need is well illustrated in the field of electrocatalytic N2 reduction, where the need for recirculation of 15N2 has recently become more apparent. Herein, we describe the design, fabrication, use, and specifications of a lubricant-free, readily constructed recirculating pump fabricated entirely from glass and inert polymer (poly(ether ether ketone) (PEEK), poly(tetrafluoroethylene) (PTFE)) components. Using these glass and polymer components ensures chemical compatibility between the piston pump and a wide range of chemical environments, including strongly acidic and organic electrolytes often employed in studies of electrocatalytic N2 reduction. The lubricant-free nature of the pump and the presence of components made exclusively of glass and PEEK/PTFE mitigate contamination concerns associated with recirculating gases saturated with corrosive or reactive vapors for extended periods. The gas recirculating glass pump achieved a flow rate of >500 mL min-1 N2 against atmospheric pressure at 15 W peak power input and >100 mL min-1 N2 against a differential pressure of +6 in. H2O (∼15 mbar) at 10 W peak power input.

  View details for DOI 10.1021/acsomega.0c00742

  View details for PubMedID 32685809

  View details for PubMedCentralID PMC7364576

• Promoting reliable electrocatalytic N2 reduction Nielander, A., McEnaney, J., Blair, S., Schwalbe, J., Baker, J., Jaramillo, T. AMER CHEMICAL SOC. 2019

  View details for Web of Science ID 000525055502400

• Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area NATURE CATALYSIS Wang, L., Nitopi, S., Wong, A. B., Snider, J. L., Nielander, A. C., Morales-Guio, C. G., Orazov, M., Higgins, D. C., Hahn, C., Jaramillo, T. F. 2019; 2 (8): 702–8

  View details for DOI 10.1038/s41929-019-0301-z

  View details for Web of Science ID 000481511400011

• Electro-Oxidation of Methane on Platinum under Ambient Conditions ACS CATALYSIS Boyd, M. J., Latimer, A. A., Dickens, C. F., Nielander, A. C., Hahn, C., Norskov, J. K., Higgins, D. C., Jaramillo, T. F. 2019; 9 (8): 7578–87

  View details for DOI 10.1021/acscatal.9b01207

  View details for Web of Science ID 000480503700098

• A Versatile Method for Ammonia Detection in a Range of Relevant Electrolytes via Direct Nuclear Magnetic Resonance Techniques ACS CATALYSIS Nielander, A. C., McEnaney, J. M., Schwalbe, J. A., Baker, J. G., Blair, S. J., Wang, L., Pelton, J. G., Andersen, S. Z., Enemark-Rasmussen, K., Colic, V., Yang, S., Bent, S. F., Cargnello, M., Kibsgaard, J., Vesborg, P. C. K., Chorkendorff, I., Jaramillo, T. F. 2019; 9 (7): 5797–5802

  View details for DOI 10.1021/acscatal.9b00358

  View details for Web of Science ID 000474812400001

• A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements. Nature Andersen, S. Z., Colic, V., Yang, S., Schwalbe, J. A., Nielander, A. C., McEnaney, J. M., Enemark-Rasmussen, K., Baker, J. G., Singh, A. R., Rohr, B. A., Statt, M. J., Blair, S. J., Mezzavilla, S., Kibsgaard, J., Vesborg, P. C., Cargnello, M., Bent, S. F., Jaramillo, T. F., Stephens, I. E., Norskov, J. K., Chorkendorff, I. 2019

  Abstract

  The electrochemical synthesis of ammonia from nitrogen under mild conditions and using renewable electricity is in principle an attractive alternative1-4 to the demanding, energy-intense Haber-Bosch process, which dominates industrial ammonia production. However, the electrochemical alternative faces considerable scientific and technical challenges5,6 and most experimental studies reported thus far achieve only low selectivities and conversions. In fact, the amount of ammonia produced is usually so small that it is difficult to firmly attribute it to electrochemical nitrogen fixation7-9 and exclude contamination due to ammonia that is either present in air, human breath or ion-conducting membranes9, or generated from labile nitrogen-containing compounds (for example, nitrates, amines, nitrites and nitrogen oxides) that are typically present in the nitrogen gas stream10, in the atmosphere or even the catalyst itself. Although these many and varied sources of potential experimental artefacts are beginning to be recognized and dealt with11,12, concerted efforts to develop effective electrochemical nitrogen reduction processes would benefit from benchmarking protocols for the reaction and from a standardized set of control experiments to identify and then eliminate or quantify contamination sources. Here we put forward such a rigorous procedure that, by making essential use of 15N2, allows us to reliably detect and quantify the electroreduction of N2 to NH3. We demonstrate experimentally the significance of various sources of contamination and show how to remove labile nitrogen-containing compounds present in the N2 gas and how to perform quantitative isotope measurements with cycling of 15N2 gas to reduce both contamination and the cost of isotope measurements. Following this protocol, we obtain negative results when using the most promising pure metal catalysts in aqueous media, and successfully confirm and quantify ammonia synthesis using lithium electrodeposition in tetrahydrofuran13.

  View details for DOI 10.1038/s41586-019-1260-x

  View details for PubMedID 31117118

• Quantitative protocol for the electroreduction of N2 to NH3 under ambient conditions Stephens, I., Andersen, S., Colic, V., Yang, S., Schwalbe, J., Nielander, A., McEnaney, J., Enemark-Rasmussen, K., Baker, J., Singh, A., Rohr, B., Blair, S., Mezzavilla, S., Kibsgaard, J., Vesborg, P., Cargnello, M., Bent, S., Jaramillo, T., Norskov, J., Chorkendorff, I. AMER CHEMICAL SOC. 2019

  View details for Web of Science ID 000478860505876

• Proton control in electrochemical ammonia synthesis Schwalbe, J., Singh, A., Rohr, B., Statt, M., Nielander, A., McEnaney, J., Andersen, S., Colic, V., Yang, S., Chorkendorff, I., Jaramillo, T., Norskov, J., Cargnello, M. AMER CHEMICAL SOC. 2019

  View details for Web of Science ID 000478860505877

• Nanostructuring Strategies To Increase the Photoelectrochemical Water Splitting Activity of Silicon Photocathodes ACS APPLIED NANO MATERIALS Hellstern, T. R., Nielander, A. C., Chakthranont, P., King, L. A., Willis, J. J., Xu, S., MacIsaac, C., Hahn, C., Bent, S. F., Prinz, F. B., Jaramillo, T. F. 2019; 2 (1): 6–11

  View details for DOI 10.1021/acsanm.8b01966

  View details for Web of Science ID 000464491500002

• Author Correction: A rigorous electrochemical ammonia synthesis protocol with quantitative isotope measurements. Nature Andersen, S. Z., Čolić, V. n., Yang, S. n., Schwalbe, J. A., Nielander, A. C., McEnaney, J. M., Enemark-Rasmussen, K. n., Baker, J. G., Singh, A. R., Rohr, B. A., Statt, M. J., Blair, S. J., Mezzavilla, S. n., Kibsgaard, J. n., Vesborg, P. C., Cargnello, M. n., Bent, S. F., Jaramillo, T. F., Stephens, I. E., Nørskov, J. K., Chorkendorff, I. n. 2019

  Abstract

  An Amendment to this paper has been published and can be accessed via a link at the top of the paper.

  View details for DOI 10.1038/s41586-019-1625-1

  View details for PubMedID 31554972

• Electrochemical cycling strategy for selective and sustainable C2H2 production from CO2 or CH4 at atmospheric pressure using H2O McEnaney, J., Rohr, B., Nielander, A., Singh, A., Norskov, J., Jaramillo, T. AMER CHEMICAL SOC. 2018

  View details for Web of Science ID 000435539900178

• Exploring electrocatalytic N2 activation under mild synthetic conditions Nielander, A., McEnaney, J., Jaramillo, T. AMER CHEMICAL SOC. 2017

  View details for Web of Science ID 000430569103422

• Lightly Fluorinated Graphene as a Protective Layer for n-Type Si(111) Photoanodes in Aqueous Electrolytes NANO LETTERS Nielander, A. C., Thompson, A. C., Roske, C. W., Maslyn, J. A., Hao, Y., Plymale, N. T., Hone, J., Lewis, N. S. 2016; 16 (7): 4082-4086

  View details for DOI 10.1021/acs.nanolett.6b00773

  View details for Web of Science ID 000379794200018

• Photoelectrochemical Behavior of n-Type GaAs(100) Electrodes Coated by a Single Layer of Graphene JOURNAL OF PHYSICAL CHEMISTRY C Yang, F., Nielander, A. C., Grimm, R. L., Lewis, N. S. 2016; 120 (13): 6989-6995

  View details for DOI 10.1021/acs.jpcc.6b00232

  View details for Web of Science ID 000373862700009

• Stable Solar-Driven Water Oxidation to O-2(g) by Ni-Oxide-Coated Silicon Photoanodes JOURNAL OF PHYSICAL CHEMISTRY LETTERS Sun, K., McDowell, M. T., Nielander, A. C., Hu, S., Shaner, M. R., Yang, F., Brunschwig, B. S., Lewis, N. S. 2015; 6 (4): 592-598

  View details for DOI 10.1021/jz5026195

  View details for Web of Science ID 000349942500018

• A taxonomy for solar fuels generators ENERGY & ENVIRONMENTAL SCIENCE Nielander, A. C., Shaner, M. R., Papadantonakis, K. M., Francis, S. A., Lewis, N. S. 2015; 8 (1): 16-25

  View details for DOI 10.1039/c4ee02251c

  View details for Web of Science ID 000346563600002

• Interface engineering of the photoelectrochemical performance of Ni-oxide-coated n-Si photoanodes by atomic-layer deposition of ultrathin films of cobalt oxide ENERGY & ENVIRONMENTAL SCIENCE Zhou, X., Liu, R., Sun, K., Friedrich, D., McDowell, M. T., Yang, F., Omelchenko, S. T., Saadi, F. H., Nielander, A. C., Yalamanchili, S., Papadantonakis, K. M., Brunschwig, B. S., Lewis, N. S. 2015; 8 (9): 2644-2649

  View details for DOI 10.1039/c5ee01687h

  View details for Web of Science ID 000360456600008

• Methods for comparing the performance of energy-conversion systems for use in solar fuels and solar electricity generation ENERGY & ENVIRONMENTAL SCIENCE Coridan, R. H., Nielander, A. C., Francis, S. A., McDowell, M. T., Dix, V., Chatman, S. M., Lewis, N. S. 2015; 8 (10): 2886-2901

  View details for DOI 10.1039/c5ee00777a

  View details for Web of Science ID 000362351700006

• Photoelectrochemical Behavior of n-Type Si(111) Electrodes Coated With a Single Layer of Graphene JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Nielander, A. C., Bierman, M. J., Petrone, N., Strandwitz, N. C., Ardo, S., Yang, F., Hone, J., Lewis, N. S. 2013; 135 (46): 17246-17249

  View details for DOI 10.1021/ja407462g

  View details for Web of Science ID 000327413300003

• Photoelectrochemical Behavior of n-type Si(100) Electrodes Coated with Thin Films of Manganese Oxide Grown by Atomic Layer Deposition JOURNAL OF PHYSICAL CHEMISTRY C Strandwitz, N. C., Comstock, D. J., Grimm, R. L., Nichols-Nielander, A. C., Elam, J., Lewis, N. S. 2013; 117 (10): 4931-4936

  View details for DOI 10.1021/jp311207x

  View details for Web of Science ID 000316308400006

• Hyperdistorted Tungsten Allyl Complexes and Their Stereoselective Deprotonation to Form Dihapto-Coordinated Dienes ORGANOMETALLICS Harrison, D. P., Nichols-Nielander, A. C., Zottig, V. E., Strausberg, L., Salomon, R. J., Trindle, C. O., Sabat, M., Gunnoe, T., Iovan, D. A., Myers, W. H., Harman, W. 2011; 30 (9): 2587-2597

  View details for DOI 10.1021/om200183m

  View details for Web of Science ID 000290001900019

• Epoxidation, Cyclopropanation, and Electrophilic Addition Reactions at the meta Position of Phenol and meta-Cresol ORGANOMETALLICS Zottig, V. E., Todd, M. A., Nichols-Nielander, A. C., Harrison, D. P., Sabat, M., Myers, W. H., Harman, W. 2010; 29 (21): 4793-4803

  View details for DOI 10.1021/om901017d

  View details for Web of Science ID 000283572100021

• Tungsten-Promoted Pyridine Ring Scission: The Selective Formation of eta(2)-Cyanine and eta(2)-Merocyanine Complexes and Their Derivatives ORGANOMETALLICS Harrison, D. P., Kosturko, G. W., Ramdeen, V. M., Nichols-Nielander, A. C., Payne, S. J., Sabat, M., Myers, W. H., Harman, W. 2010; 29 (8): 1909-1915

  View details for DOI 10.1021/om1001777

  View details for Web of Science ID 000276692100009

• Efficient Synthesis of an eta(2)-Pyridine Complex and a Preliminary Investigation of the Bound Heterocycle's Reactivity JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Harrison, D. P., Welch, K. D., Nichols-Nielander, A. C., Sabat, M., Myers, W. H., Harman, W. 2008; 130 (50): 16844-+

  View details for DOI 10.1021/ja807521d

  View details for Web of Science ID 000263320400010