All Publications

  • Enhanced energy delivery of direct-write fabricated reactive materials with energetic graphene oxide COMBUSTION AND FLAME Wang, H., Jiang, Y., Wang, Y., Baek, J., Zheng, X., Zachariah, M. R. 2024; 260
  • Synergistic effects of mixing and strain in high entropy spinel oxides for oxygen evolution reaction. Nature communications Baek, J., Hossain, M. D., Mukherjee, P., Lee, J., Winther, K. T., Leem, J., Jiang, Y., Chueh, W. C., Bajdich, M., Zheng, X. 2023; 14 (1): 5936


    Developing stable and efficient electrocatalysts is vital for boosting oxygen evolution reaction (OER) rates in sustainable hydrogen production. High-entropy oxides (HEOs) consist of five or more metal cations, providing opportunities to tune their catalytic properties toward high OER efficiency. This work combines theoretical and experimental studies to scrutinize the OER activity and stability for spinel-type HEOs. Density functional theory confirms that randomly mixed metal sites show thermodynamic stability, with intermediate adsorption energies displaying wider distributions due to mixing-induced equatorial strain in active metal-oxygen bonds. The rapid sol-flame method is employed to synthesize HEO, comprising five 3d-transition metal cations, which exhibits superior OER activity and durability under alkaline conditions, outperforming lower-entropy oxides, even with partial surface oxidations. The study highlights that the enhanced activity of HEO is primarily attributed to the mixing of multiple elements, leading to strain effects near the active site, as well as surface composition and coverage.

    View details for DOI 10.1038/s41467-023-41359-7

    View details for PubMedID 37741823

    View details for PubMedCentralID PMC10517924

  • Exfoliated Magnesium Diboride (MgB2) Nanosheets as Solid Fuels. Nano letters Jiang, Y., Ka, D., Huynh, A. H., Baek, J., Ning, R., Yu, S. J., Zheng, X. 2023


    Magnesium diboride (MgB2) has been explored as an alternative fuel to boron (B) due to its high energy density and the additive effect of magnesium (Mg) to promote B combustion. However, the primary oxidation of MgB2 does not occur unless it decomposes at a high temperature (830 °C), which makes ignition difficult and the reaction slow. Recently, two-dimensional (2D) exfoliated MgB2 nanosheets have attracted increasing attention due to their unique properties and potential applications in various fields. In this study, we investigate the potential of 2D exfoliated MgB2 nanosheets as solid fuels for overcoming the challenges of MgB2 combustion. We analyzed their oxidation behavior and energetic performance through material characterization and combustion tests under slow- and fast-heating conditions and compared their performance with those of bulk MgB2, B nanoparticles, and a B/Mg nanoparticle mixture. This study highlights the potential of MgB2 nanosheets as promising solid fuels with superior energetic properties.

    View details for DOI 10.1021/acs.nanolett.3c01910

    View details for PubMedID 37656036

  • Enhanced H2O2 Upcycling into Hydroxyl Radicals with GO/Ni:FeOOH-Coated Silicon Nanowire Photocatalysts for Wastewater Treatment. Nano letters Ning, R., Kim, S., Sun, E., Jiang, Y., Baek, J., Li, Y., Robinson, A., Vallez, L., Zheng, X. 2023


    There remains continued interest in improving the advanced water oxidation process [e.g., ultraviolet (UV)/hydrogen peroxide (H2O2)] for more efficient and environmentally friendly wastewater treatment. Here, we report the design, fabrication, and performance of graphene oxide (GO, on top)/nickel-doped iron oxyhydroxide (Ni:FeOOH, shell)/silicon nanowires (SiNWs, core) as a new multifunctional photocatalyst for the degradation of common pollutants like polystyrene and methylene blue through enhancing the hydroxyl radical (•OH) production rate of the UV/H2O2 system. The photocatalyst combines the advantages of a large surface area and light absorption characteristics of SiNWs with heterogeneous photo-Fenton active Ni:FeOOH and photocatalytically active/charge separator GO. In addition, the built-in electric field of GO/Ni:FeOOH/SiNWs facilitates the charge separation of electrons to GO and holes to Ni:FeOOH, thus boosting the photocatalytic performance. Our photocatalyst increases the •OH yield by 5.7 times compared with that of a blank H2O2 solution sample and also extends the light absorption spectrum to include visible light irradiation.

    View details for DOI 10.1021/acs.nanolett.3c00696

    View details for PubMedID 37459426

  • Author Correction: Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide. Nature communications Baek, J., Jin, Q., Johnson, N. S., Jiang, Y., Ning, R., Mehta, A., Siahrostami, S., Zheng, X. 2022; 13 (1): 7685

    View details for DOI 10.1038/s41467-022-35478-w

    View details for PubMedID 36509777

  • Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide. Nature communications Baek, J., Jin, Q., Johnson, N. S., Jiang, Y., Ning, R., Mehta, A., Siahrostami, S., Zheng, X. 2022; 13 (1): 7256


    Electrochemical two-electron water oxidation reaction (2e-WOR) has drawn significant attention as a promising process to achieve the continuous on-site production of hydrogen peroxide (H2O2). However, compared to the cathodic H2O2 generation, the anodic 2e-WOR is more challenging to establish catalysts due to the severe oxidizing environment. In this study, we combine density functional theory (DFT) calculations with experiments to discover a stable and efficient perovskite catalyst for the anodic 2e-WOR. Our theoretical screening efforts identify LaAlO3 perovskite as a stable, active, and selective candidate for catalyzing 2e-WOR. Our experimental results verify that LaAlO3 achieves an overpotential of 510mV at 10mAcm-2 in 4M K2CO3/KHCO3, lower than those of many reported metal oxide catalysts. In addition, LaAlO3 maintains a stable H2O2 Faradaic efficiency with only a 3% decrease after 3h at 2.7V vs. RHE. This computation-experiment synergistic approach introduces another effective direction to discover promising catalysts for the harsh anodic 2e-WOR towards H2O2.

    View details for DOI 10.1038/s41467-022-34884-4

    View details for PubMedID 36433962

  • Perfluoroalkyl-Functionalized Graphene Oxide as a Multifunctional Additive for Promoting the Energetic Performance of Aluminum. ACS nano Jiang, Y., Wang, H., Baek, J., Ka, D., Huynh, A. H., Wang, Y., Zachariah, M. R., Zheng, X. 2022


    Aluminum (Al) is a widely used metal fuel for energetic applications ranging from space propulsion and exploration, and materials processing, to power generation for nano- and microdevices due to its high energy density and earth abundance. Recently, the ignition and combustion performance of Al particles were found to be improved by graphene-based additives, such as graphene oxide (GO) and graphene fluoride (GF), as their reactions provide heat to accelerate Al oxidation, gas to reduce particle agglomeration, and fluorine-containing species to remove Al2O3. However, GF is not only expensive but also hydrophobic with poor mixing compatibility with Al particles. Herein, we report a multifunctional graphene-based additive for Al combustion, i.e., perfluoroalkyl-functionalized graphene oxide (CFGO), which integrates the benefits of GO and GF in one material. We compared the effects of CFGO to GO and GF on the ignition and combustion properties of nAl particles using thermogravimetric analysis, differential scanning calorimetry, temperature-jump ignition), Xe flash ignition, and constant-volume combustion test. These experiments confirm that CFGO generates fluorine-containing species, heat, and gases, which collectively lower the ignition threshold, augment the energy release rate, and reduce the combustion product agglomeration of nanosized Al particles, outperforming both GO and GF as additives. This work shows the great potential of using multifunctionalized graphene as an integrated additive for enhancing the ignition and combustion of metals.

    View details for DOI 10.1021/acsnano.2c05271

    View details for PubMedID 36099637

  • Ignition and combustion of Perfluoroalkyl-functionalized aluminum nanoparticles and nanothermite COMBUSTION AND FLAME Jiang, Y., Wang, Y., Baek, J., Wang, H., Gottfried, J. L., Wu, C., Shi, X., Zachariah, M. R., Zheng, X. 2022; 242
  • Efficient and Stable Acidic Water Oxidation Enabled by Low-Concentration, High-Valence Iridium Sites ACS ENERGY LETTERS Shi, X., Peng, H., Hersbach, T. P., Jiang, Y., Zeng, Y., Baek, J., Winther, K. T., Sokaras, D., Zheng, X., Bajdich, M. 2022
  • Effect of Fluoroalkylsilane Surface Functionalization on Boron Combustion. ACS applied materials & interfaces Baek, J., Jiang, Y., Demko, A. R., Jimenez-Thomas, A. R., Vallez, L., Ka, D., Xia, Y., Zheng, X. 2022


    Boron has been regarded as a promising high-energy fuel due to its high volumetric and gravimetric heating values. However, it remains challenging for boron to attain its theoretical heat of combustion because of the existence of its native boron oxide layer and its high melting and boiling temperatures that delay ignition and inhibit complete combustion. Boron combustion is known to be enhanced by physically adding fluorine-containing chemicals, such as fluoropolymer or metal fluorides, to remove surface boron oxides. Herein, we chemically functionalize the surface of boron particles with three different fluoroalkylsilanes: FPTS-B (F3-B), FOTS-B (F13-B), and FDTS-B (F17-B). We evaluated the ignition and combustion properties of those three functionalized boron particles as well as pristine ones. The boron particles functionalized with the longest fluorocarbon chain (F17) exhibit the most powerful energetic performance, the highest heat of combustion, and the strongest BO2 emission among all samples. These results suggest that the surface functionalization with fluoroalkylsilanes is an efficient strategy to enhance boron ignition and combustion.

    View details for DOI 10.1021/acsami.2c00347

    View details for PubMedID 35467848

  • Enhancing Mechanical and Combustion Performance of Boron/Polymer Composites via Boron Particle Functionalization. ACS applied materials & interfaces Jiang, Y., Dincer Yilmaz, N. E., Barker, K. P., Baek, J., Xia, Y., Zheng, X. 2021


    High-speed air-breathing propulsion systems, such as solid fuel ramjets (SFRJ), are important for space exploration and national security. The development of SFRJ requires high-performance solid fuels with excellent mechanical and combustion properties. One of the current solid fuel candidates is composed of high-energy particles (e.g., boron (B)) and polymeric binder (e.g., hydroxyl-terminated polybutadiene (HTPB)). However, the opposite polarities of the boron surface and HTPB lead to poor B particle dispersion and distribution within HTPB. Herein, we demonstrate that the surface functionalization of B particles with nonpolar oleoyl chloride greatly improves the dispersion and distribution of B particles within HTPB. The improved particle dispersion is quantitatively visualized through X-ray computed tomography imaging, and the particle/matrix interaction is evaluated by dynamic mechanical analysis. The surface-functionalized B particles can be uniformly dispersed up to 40 wt % in HTPB, the highest mass loading reported to date. The surface-functionalized B (40 wt %)/HTPB composite exhibits a 63.3% higher Young's modulus, 87.5% higher tensile strength, 16.2% higher toughness, and 16.8% higher heat of combustion than pristine B (40 wt %)/HTPB. The surface functionalization of B particles provides an effective strategy for improving the efficacy and safety of B/HTPB solid fuels for future high-speed air-breathing vehicles.

    View details for DOI 10.1021/acsami.1c06727

    View details for PubMedID 34110148