Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride

Turaczy, Kevin K.; Liao, Wenjie; Mou, Hansen; Nichols, Nathaniel N.; Liu, Ping; Chen, Jingguang G.

doi:10.1021/acscatal.3c04063

Title: Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride

Journal Article · Mon Oct 23 00:00:00 EDT 2023 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.3c04063· OSTI ID:2267554

Turaczy, Kevin K. ^[1];

^[2]; Mou, Hansen ^[1]; Nichols, Nathaniel N. ^[1];

^[2];

^[2]

Columbia University, New York, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division

It is well established that hydrogen binding energy (HBE) is a key descriptor for hydrogen evolution reaction (HER) activity, and such a relationship is a useful tool for searching efficient and cost-effective HER catalysts. However, in almost all cases, the HBE values are obtained from density functional theory (DFT) calculations. Here in this study, temperature programmed desorption (TPD) was used to experimentally determine the HBE values of metal monolayers supported on molybdenum nitride (Mo₂N), and electrochemical measurements were performed on the same surfaces. Combined DFT and kinetic Monte Carlo (kMC) simulations were used to validate the trend observed with TPD and the electrochemical HER activity. Depositing one monolayer of Pt on Mo₂N led to similar HBE values seen for bulk Pt, and electrochemical measurements showed that monolayer Pt on Mo₂N had similar HER activity to that of bulk Pt. Similar studies were also performed for monolayer Pd on Mo₂N to confirm the correlation. This work also demonstrates that Mo₂N is a promising support to reduce precious metal loading in HER catalysts.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2267554

Report Number(s):: BNL-225118-2023-JAAM

Journal Information:: ACS Catalysis, Vol. 13, Issue 21; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (47)

Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Thermal desorption of gases Redhead, P. A. Vacuum, Vol. 12, Issue 4 https://doi.org/10.1016/0042-207X(62)90978-8	journal	July 1962
Global Hydrogen Review 2022 https://doi.org/10.1787/a15b8442-en	book	October 2022
Challenges and Opportunities in Utilizing MXenes of Carbides and Nitrides as Electrocatalysts Wang, Yan; Nian, Yao; Biswas, Akash N. Advanced Energy Materials, Vol. 11, Issue 3 https://doi.org/10.1002/aenm.202002967	journal	December 2020
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Adsorption and Absorption Energies of Hydrogen with Palladium Schwarzer, Michael; Hertl, Nils; Nitz, Florian The Journal of Physical Chemistry C, Vol. 126, Issue 34 https://doi.org/10.1021/acs.jpcc.2c04567	journal	August 2022
A simulated-TPD study of H2 desorption on metal surfaces Lv, Shuangshuang; Liu, Xiaojing; Shen, Xiangjian Surface Science, Vol. 718 https://doi.org/10.1016/j.susc.2021.122015	journal	April 2022
Adsorption of hydrogen on a Pt(111) surface Christmann, K.; Ertl, G.; Pignet, T. Surface Science, Vol. 54, Issue 2 https://doi.org/10.1016/0039-6028(76)90232-6	journal	February 1976
Monolayer platinum supported on tungsten carbides as low-cost electrocatalysts: opportunities and limitations Esposito, Daniel V.; Chen, Jingguang G. Energy & Environmental Science, Vol. 4, Issue 10 https://doi.org/10.1039/c1ee01851e	journal	January 2011
Trends and Descriptors of Metal-Modified Transition Metal Carbides for Hydrogen Evolution in Alkaline Electrolyte Zhang, Qian; Jiang, Zhao; Tackett, Brian M. ACS Catalysis, Vol. 9, Issue 3 https://doi.org/10.1021/acscatal.8b03990	journal	February 2019
The role of hydrogen and fuel cells in the global energy system Staffell, Iain; Scamman, Daniel; Velazquez Abad, Anthony Energy & Environmental Science, Vol. 12, Issue 2 https://doi.org/10.1039/C8EE01157E	journal	January 2019
Electro-reduction of nitrogen on molybdenum nitride: structure, energetics, and vibrational spectra from DFT Matanović, Ivana; Garzon, Fernando H.; Henson, Neil J. Physical Chemistry Chemical Physics, Vol. 16, Issue 7 https://doi.org/10.1039/c3cp54559h	journal	January 2014
Elastic Scattering Corrections in AES and XPS. II. Estimating Attenuation Lengths and Conditions Required for their Valid Use in Overlayer/Substrate Experiments Cumpson, P. J.; Seah, M. P. Surface and Interface Analysis, Vol. 25, Issue 6 https://doi.org/10.1002/(SICI)1096-9918(199706)25:6<430::AID-SIA254>3.0.CO;2-7	journal	June 1997
Reforming of Oxygenates for H ₂ Production: Correlating Reactivity of Ethylene Glycol and Ethanol on Pt(111) and Ni/Pt(111) with Surface d-Band Center Skoplyak, Orest; Barteau, Mark A.; Chen, Jingguang G. The Journal of Physical Chemistry B, Vol. 110, Issue 4 https://doi.org/10.1021/jp0548927	journal	February 2006
Trends in the Exchange Current for Hydrogen Evolution Nørskov, J. K.; Bligaard, T.; Logadottir, A. Journal of The Electrochemical Society, Vol. 152, Issue 3 https://doi.org/10.1149/1.1856988	journal	January 2005
Crystal structure and high-pressure properties of γ-Mo2N determined by neutron powder diffraction and X-ray diffraction Bull, Craig L.; Kawashima, Tetsuya; McMillan, Paul F. Journal of Solid State Chemistry, Vol. 179, Issue 6 https://doi.org/10.1016/j.jssc.2006.03.011	journal	June 2006
Study on the reaction pathways of steam methane reforming for H2 production Cai, Lei; He, Tianzhi; Xiang, Yanlei Energy, Vol. 207 https://doi.org/10.1016/j.energy.2020.118296	journal	September 2020
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts Tackett, Brian M.; Sheng, Wenchao; Chen, Jingguang G. Joule, Vol. 1, Issue 2 https://doi.org/10.1016/j.joule.2017.07.002	journal	October 2017
Electrocatalysis of the HER in acid and alkaline media Danilovic, Nemanja; Subbaraman, Ram; Strmcnik, Dusan Journal of the Serbian Chemical Society, Vol. 78, Issue 12 https://doi.org/10.2298/JSC131118136D	journal	January 2013
Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes Sheng, Wenchao; Gasteiger, Hubert A.; Shao-Horn, Yang Journal of The Electrochemical Society, Vol. 157, Issue 11 https://doi.org/10.1149/1.3483106	journal	January 2010
Effect of deposition conditions on mechanical stresses and microstructure of sputter-deposited molybdenum and reactively sputter-deposited molybdenum nitride films Shen, Y. G. Materials Science and Engineering: A, Vol. 359, Issue 1-2 https://doi.org/10.1016/S0921-5093(03)00336-8	journal	October 2003
Trends in Electrochemical Stability of Transition Metal Carbides and Their Potential Use As Supports for Low-Cost Electrocatalysts Kimmel, Yannick C.; Xu, Xiaoge; Yu, Weiting ACS Catalysis, Vol. 4, Issue 5 https://doi.org/10.1021/cs500182h	journal	April 2014
Sorption and temperature-programmed desorption of hydrogen from palladium and from palladium on activated carbon Konvalinka, J. Journal of Catalysis, Vol. 48, Issue 1-3 https://doi.org/10.1016/0021-9517(77)90111-7	journal	June 1977
Electronic Structures of NH, NH ₂ , and NH ₃ Higuchi, Jiro The Journal of Chemical Physics, Vol. 24, Issue 3 https://doi.org/10.1063/1.1742542	journal	March 1956
Correlating the hydrogen evolution reaction activity in alkaline electrolytes with the hydrogen binding energy on monometallic surfaces Sheng, Wenchao; Myint, MyatNoeZin; Chen, Jingguang G. Energy & Environmental Science, Vol. 6, Issue 5 https://doi.org/10.1039/c3ee00045a	journal	January 2013
VASP on a GPU: Application to exact-exchange calculations of the stability of elemental boron Hutchinson, M.; Widom, M. Computer Physics Communications, Vol. 183, Issue 7 https://doi.org/10.1016/j.cpc.2012.02.017	journal	July 2012
Surface electronic structure and reactivity of transition and noble metals1Communication presented at the First Francqui Colloquium, Brussels, 19–20 February 1996.1 Ruban, A.; Hammer, B.; Stoltze, P. Journal of Molecular Catalysis A: Chemical, Vol. 115, Issue 3 https://doi.org/10.1016/S1381-1169(96)00348-2	journal	February 1997
Density functional theory studies of transition metal carbides and nitrides as electrocatalysts Tian, Dong; Denny, Steven R.; Li, Kongzhai Chemical Society Reviews, Vol. 50, Issue 22 https://doi.org/10.1039/D1CS00590A	journal	January 2021
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Machine learning prediction and experimental verification of Pt-modified nitride catalysts for ethanol reforming with reduced precious metal loading Denny, Steven R.; Lin, Zhexi; Porter, William N. Applied Catalysis B: Environmental, Vol. 312 https://doi.org/10.1016/j.apcatb.2022.121380	journal	September 2022
Theoretical prediction and experimental verification of low loading of platinum on titanium carbide as low-cost and stable electrocatalysts Kimmel, Yannick C.; Yang, Leerang; Kelly, Thomas G. Journal of Catalysis, Vol. 312 https://doi.org/10.1016/j.jcat.2014.02.002	journal	April 2014
Transition Metal Carbides and Nitrides as Electrode Materials for Low Temperature Fuel Cells Ham, Dong Jin; Lee, Jae Sung Energies, Vol. 2, Issue 4, p. 873-899 https://doi.org/10.3390/en20400873	journal	October 2009
Carbide and Nitride Overlayers on Early Transition Metal Surfaces: Preparation, Characterization, and Reactivities Chen, Jingguang G. Chemical Reviews, Vol. 96, Issue 4 https://doi.org/10.1021/cr950232u	journal	January 1996
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Conversion of NO into N ₂ over γ-Mo ₂ N Altarawneh, Mohammednoor; Jaf, Zainab; Oskierski, Hans The Journal of Physical Chemistry C, Vol. 120, Issue 39 https://doi.org/10.1021/acs.jpcc.6b04107	journal	September 2016
Exploring Metal–Support Interactions To Immobilize Subnanometer Co Clusters on γ–Mo ₂ N: A Highly Selective and Stable Catalyst for CO ₂ Activation Yao, Siyu; Lin, Lili; Liao, Wenjie ACS Catalysis, Vol. 9, Issue 10 https://doi.org/10.1021/acscatal.9b01945	journal	July 2019
Effect of surface carbon on the hydrogen evolution reactivity of tungsten carbide (WC) and Pt-modified WC electrocatalysts Kimmel, Yannick C.; Esposito, Daniel V.; Birkmire, Robert W. International Journal of Hydrogen Energy, Vol. 37, Issue 4 https://doi.org/10.1016/j.ijhydene.2011.11.079	journal	February 2012
Adsorption of hydrogen on palladium single crystal surfaces Conrad, H.; Ertl, G.; Latta, E. E. Surface Science, Vol. 41, Issue 2 https://doi.org/10.1016/0039-6028(74)90060-0	journal	February 1974
Determination of growth modes of ultrathin films from Auger electron spectroscopy : An assessment and commentary Rhead, G. E.; Barthès, M. -G.; Argile, C. Thin Solid Films, Vol. 82, Issue 2 https://doi.org/10.1016/0040-6090(81)90444-2	journal	August 1981
Surface and Subsurface Hydrogen: Adsorption Properties on Transition Metals and Near-Surface Alloys Greeley, Jeff; Mavrikakis, Manos The Journal of Physical Chemistry B, Vol. 109, Issue 8 https://doi.org/10.1021/jp046540q	journal	March 2005
Unraveling Unique Surface Chemistry of Transition Metal Nitrides in Controlling Selective C–O Bond Scission Pathways of Glycerol Lin, Zhexi; Ammal, Salai C.; Denny, Steven R. JACS Au, Vol. 2, Issue 2 https://doi.org/10.1021/jacsau.1c00403	journal	January 2022
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode Nørskov, J. K.; Rossmeisl, J.; Logadottir, A. The Journal of Physical Chemistry B, Vol. 108, Issue 46 https://doi.org/10.1021/jp047349j	journal	November 2004
Accelerating VASP electronic structure calculations using graphic processing units Hacene, Mohamed; Anciaux-Sedrakian, Ani; Rozanska, Xavier Journal of Computational Chemistry, Vol. 33, Issue 32 https://doi.org/10.1002/jcc.23096	journal	August 2012
Platinum-Like Behavior of Tungsten Carbide in Surface Catalysis Levy, R. B.; Boudart, M. Science, Vol. 181, Issue 4099 https://doi.org/10.1126/science.181.4099.547	journal	August 1973
Preparation and catalytic properties of transition metal carbides and nitrides Oyama, S. T. Catalysis Today, Vol. 15, Issue 2 https://doi.org/10.1016/0920-5861(92)80175-M	journal	June 1992
Clean energy and the hydrogen economy Brandon, N. P.; Kurban, Z. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 375, Issue 2098 https://doi.org/10.1098/rsta.2016.0400	journal	June 2017
How to Get Kinetic Parameters Jansen, A. P. J. An Introduction to Kinetic Monte Carlo Simulations of Surface Reactions https://doi.org/10.1007/978-3-642-29488-4_4	book	January 2012

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Title: Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride

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