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Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride
Abstract
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.
- Authors:
-
[2];
[2];
[2]
- Columbia University, New York, NY (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 2267554
- Report Number(s):
- BNL-225118-2023-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 13; Journal Issue: 21; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 08 HYDROGEN; hydrogen evolution reaction; HER; hydrogen binding energy; HBE; density functional theory; DFT; temperature-programmed desorption; TPD; transition metal nitride; TMN
Citation Formats
Turaczy, Kevin K., Liao, Wenjie, Mou, Hansen, Nichols, Nathaniel N., Liu, Ping, and Chen, Jingguang G. Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride. United States: N. p., 2023.
Web. doi:10.1021/acscatal.3c04063.
Turaczy, Kevin K., Liao, Wenjie, Mou, Hansen, Nichols, Nathaniel N., Liu, Ping, & Chen, Jingguang G. Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride. United States. https://doi.org/10.1021/acscatal.3c04063
Turaczy, Kevin K., Liao, Wenjie, Mou, Hansen, Nichols, Nathaniel N., Liu, Ping, and Chen, Jingguang G. Mon .
"Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride". United States. https://doi.org/10.1021/acscatal.3c04063.
@article{osti_2267554,
title = {Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride},
author = {Turaczy, Kevin K. and Liao, Wenjie and Mou, Hansen and Nichols, Nathaniel N. and Liu, Ping and Chen, Jingguang G.},
abstractNote = {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.},
doi = {10.1021/acscatal.3c04063},
journal = {ACS Catalysis},
number = 21,
volume = 13,
place = {United States},
year = {Mon Oct 23 00:00:00 EDT 2023},
month = {Mon Oct 23 00:00:00 EDT 2023}
}
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Works referenced in this record:
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Challenges and Opportunities in Utilizing MXenes of Carbides and Nitrides as Electrocatalysts
journal, December 2020
- Wang, Yan; Nian, Yao; Biswas, Akash N.
- Advanced Energy Materials, Vol. 11, Issue 3
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Adsorption and Absorption Energies of Hydrogen with Palladium
journal, August 2022
- Schwarzer, Michael; Hertl, Nils; Nitz, Florian
- The Journal of Physical Chemistry C, Vol. 126, Issue 34
A simulated-TPD study of H2 desorption on metal surfaces
journal, April 2022
- Lv, Shuangshuang; Liu, Xiaojing; Shen, Xiangjian
- Surface Science, Vol. 718
Adsorption of hydrogen on a Pt(111) surface
journal, February 1976
- Christmann, K.; Ertl, G.; Pignet, T.
- Surface Science, Vol. 54, Issue 2
Monolayer platinum supported on tungsten carbides as low-cost electrocatalysts: opportunities and limitations
journal, January 2011
- Esposito, Daniel V.; Chen, Jingguang G.
- Energy & Environmental Science, Vol. 4, Issue 10
Trends and Descriptors of Metal-Modified Transition Metal Carbides for Hydrogen Evolution in Alkaline Electrolyte
journal, February 2019
- Zhang, Qian; Jiang, Zhao; Tackett, Brian M.
- ACS Catalysis, Vol. 9, Issue 3
The role of hydrogen and fuel cells in the global energy system
journal, January 2019
- Staffell, Iain; Scamman, Daniel; Velazquez Abad, Anthony
- Energy & Environmental Science, Vol. 12, Issue 2
Electro-reduction of nitrogen on molybdenum nitride: structure, energetics, and vibrational spectra from DFT
journal, January 2014
- Matanović, Ivana; Garzon, Fernando H.; Henson, Neil J.
- Physical Chemistry Chemical Physics, Vol. 16, Issue 7
Elastic Scattering Corrections in AES and XPS. II. Estimating Attenuation Lengths and Conditions Required for their Valid Use in Overlayer/Substrate Experiments
journal, June 1997
- Cumpson, P. J.; Seah, M. P.
- Surface and Interface Analysis, Vol. 25, Issue 6
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
journal, February 2006
- Skoplyak, Orest; Barteau, Mark A.; Chen, Jingguang G.
- The Journal of Physical Chemistry B, Vol. 110, Issue 4
Trends in the Exchange Current for Hydrogen Evolution
journal, January 2005
- Nørskov, J. K.; Bligaard, T.; Logadottir, A.
- Journal of The Electrochemical Society, Vol. 152, Issue 3
Crystal structure and high-pressure properties of γ-Mo2N determined by neutron powder diffraction and X-ray diffraction
journal, June 2006
- Bull, Craig L.; Kawashima, Tetsuya; McMillan, Paul F.
- Journal of Solid State Chemistry, Vol. 179, Issue 6
Study on the reaction pathways of steam methane reforming for H2 production
journal, September 2020
- Cai, Lei; He, Tianzhi; Xiang, Yanlei
- Energy, Vol. 207
Opportunities and Challenges in Utilizing Metal-Modified Transition Metal Carbides as Low-Cost Electrocatalysts
journal, October 2017
- Tackett, Brian M.; Sheng, Wenchao; Chen, Jingguang G.
- Joule, Vol. 1, Issue 2
Electrocatalysis of the HER in acid and alkaline media
journal, January 2013
- Danilovic, Nemanja; Subbaraman, Ram; Strmcnik, Dusan
- Journal of the Serbian Chemical Society, Vol. 78, Issue 12
Hydrogen Oxidation and Evolution Reaction Kinetics on Platinum: Acid vs Alkaline Electrolytes
journal, January 2010
- Sheng, Wenchao; Gasteiger, Hubert A.; Shao-Horn, Yang
- Journal of The Electrochemical Society, Vol. 157, Issue 11
Effect of deposition conditions on mechanical stresses and microstructure of sputter-deposited molybdenum and reactively sputter-deposited molybdenum nitride films
journal, October 2003
- Shen, Y. G.
- Materials Science and Engineering: A, Vol. 359, Issue 1-2
Trends in Electrochemical Stability of Transition Metal Carbides and Their Potential Use As Supports for Low-Cost Electrocatalysts
journal, April 2014
- Kimmel, Yannick C.; Xu, Xiaoge; Yu, Weiting
- ACS Catalysis, Vol. 4, Issue 5
Sorption and temperature-programmed desorption of hydrogen from palladium and from palladium on activated carbon
journal, June 1977
- Konvalinka, J.
- Journal of Catalysis, Vol. 48, Issue 1-3
Electronic Structures of NH, NH 2 , and NH 3
journal, March 1956
- Higuchi, Jiro
- The Journal of Chemical Physics, Vol. 24, Issue 3
Correlating the hydrogen evolution reaction activity in alkaline electrolytes with the hydrogen binding energy on monometallic surfaces
journal, January 2013
- Sheng, Wenchao; Myint, MyatNoeZin; Chen, Jingguang G.
- Energy & Environmental Science, Vol. 6, Issue 5
VASP on a GPU: Application to exact-exchange calculations of the stability of elemental boron
journal, July 2012
- Hutchinson, M.; Widom, M.
- Computer Physics Communications, Vol. 183, Issue 7
Surface electronic structure and reactivity of transition and noble metals1Communication presented at the First Francqui Colloquium, Brussels, 19–20 February 1996.1
journal, February 1997
- Ruban, A.; Hammer, B.; Stoltze, P.
- Journal of Molecular Catalysis A: Chemical, Vol. 115, Issue 3
Density functional theory studies of transition metal carbides and nitrides as electrocatalysts
journal, January 2021
- Tian, Dong; Denny, Steven R.; Li, Kongzhai
- Chemical Society Reviews, Vol. 50, Issue 22
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Machine learning prediction and experimental verification of Pt-modified nitride catalysts for ethanol reforming with reduced precious metal loading
journal, September 2022
- Denny, Steven R.; Lin, Zhexi; Porter, William N.
- Applied Catalysis B: Environmental, Vol. 312
Theoretical prediction and experimental verification of low loading of platinum on titanium carbide as low-cost and stable electrocatalysts
journal, April 2014
- Kimmel, Yannick C.; Yang, Leerang; Kelly, Thomas G.
- Journal of Catalysis, Vol. 312
Transition Metal Carbides and Nitrides as Electrode Materials for Low Temperature Fuel Cells
journal, October 2009
- Ham, Dong Jin; Lee, Jae Sung
- Energies, Vol. 2, Issue 4, p. 873-899
Carbide and Nitride Overlayers on Early Transition Metal Surfaces: Preparation, Characterization, and Reactivities
journal, January 1996
- Chen, Jingguang G.
- Chemical Reviews, Vol. 96, Issue 4
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Conversion of NO into N 2 over γ-Mo 2 N
journal, September 2016
- Altarawneh, Mohammednoor; Jaf, Zainab; Oskierski, Hans
- The Journal of Physical Chemistry C, Vol. 120, Issue 39
Exploring Metal–Support Interactions To Immobilize Subnanometer Co Clusters on γ–Mo 2 N: A Highly Selective and Stable Catalyst for CO 2 Activation
journal, July 2019
- Yao, Siyu; Lin, Lili; Liao, Wenjie
- ACS Catalysis, Vol. 9, Issue 10
Effect of surface carbon on the hydrogen evolution reactivity of tungsten carbide (WC) and Pt-modified WC electrocatalysts
journal, February 2012
- Kimmel, Yannick C.; Esposito, Daniel V.; Birkmire, Robert W.
- International Journal of Hydrogen Energy, Vol. 37, Issue 4
Adsorption of hydrogen on palladium single crystal surfaces
journal, February 1974
- Conrad, H.; Ertl, G.; Latta, E. E.
- Surface Science, Vol. 41, Issue 2
Determination of growth modes of ultrathin films from Auger electron spectroscopy : An assessment and commentary
journal, August 1981
- Rhead, G. E.; Barthès, M. -G.; Argile, C.
- Thin Solid Films, Vol. 82, Issue 2
Surface and Subsurface Hydrogen: Adsorption Properties on Transition Metals and Near-Surface Alloys
journal, March 2005
- Greeley, Jeff; Mavrikakis, Manos
- The Journal of Physical Chemistry B, Vol. 109, Issue 8
Unraveling Unique Surface Chemistry of Transition Metal Nitrides in Controlling Selective C–O Bond Scission Pathways of Glycerol
journal, January 2022
- Lin, Zhexi; Ammal, Salai C.; Denny, Steven R.
- JACS Au, Vol. 2, Issue 2
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Accelerating VASP electronic structure calculations using graphic processing units
journal, August 2012
- Hacene, Mohamed; Anciaux-Sedrakian, Ani; Rozanska, Xavier
- Journal of Computational Chemistry, Vol. 33, Issue 32
Platinum-Like Behavior of Tungsten Carbide in Surface Catalysis
journal, August 1973
- Levy, R. B.; Boudart, M.
- Science, Vol. 181, Issue 4099
Preparation and catalytic properties of transition metal carbides and nitrides
journal, June 1992
- Oyama, S. T.
- Catalysis Today, Vol. 15, Issue 2
Clean energy and the hydrogen economy
journal, June 2017
- Brandon, N. P.; Kurban, Z.
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 375, Issue 2098
How to Get Kinetic Parameters
book, January 2012
- Jansen, A. P. J.
- An Introduction to Kinetic Monte Carlo Simulations of Surface Reactions