Hydrogen in Nanocatalysis

Fung, Victor; Hu, Guoxiang; Wu, Zili; Jiang, De-en

doi:10.1021/acs.jpclett.0c01783

Hydrogen in Nanocatalysis

Journal Article · Fri Jul 31 00:00:00 EDT 2020 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.0c01783· OSTI ID:1657894

^[1]; ^[1]; ^[2]; Jiang, De-en ^[3]

Univ. of California, Riverside, CA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of California, Riverside, CA (United States)

Hydrogen is ubiquitous in catalysis. It is involved in many important reactions such as water splitting, N₂ reduction, CO₂ reduction, and alkane activation. In this Perspective, we focus on the hydrogen atom and follow its electron as it interacts with a catalyst or behaves as part of a catalyst from a computational point of view. In this work, we present recent examples in both nanocluster and solid catalysts to elucidate the parameters governing the strength of the hydrogen–surface interactions based on site geometry and electronic structure. We further show the interesting behavior of hydride in nanometal and oxides for catalysis. Overall, the key take-home messages are: (1) the in-the-middle electronegativity and small size of hydrogen give it great versatility in interacting with active sites on nanoparticles and solid surfaces; (2) the strength of hydrogen binding to an active site on a surface is an important descriptor of the chemical and catalytic properties of the surface; (3) the energetics of the hydrogen binding is closely related to the electronic structure of the catalyst; (4) hydrides in nanoclusters and oxides and on surfaces offer unique reactivity for reduction reactions.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1657894

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 17 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (58)

Metal-Dependent Support Effects of Oxyhydride-Supported Ru, Fe, Co Catalysts for Ammonia Synthesis Tang, Ya; Kobayashi, Yoji; Masuda, Naoya Advanced Energy Materials, Vol. 8, Issue 36 https://doi.org/10.1002/aenm.201801772	journal	November 2018
Trends of Alkane Activation on Doped Cobalt (II, III) Oxide from First Principles Fung, Victor; Tao, Franklin Feng; Jiang, De-en ChemCatChem, Vol. 10, Issue 1 https://doi.org/10.1002/cctc.201700960	journal	November 2017
Theory of surface chemistry and reactivity of reducible oxides van Santen, Rutger A.; Tranca, Ionut; Hensen, Emiel J. M. Catalysis Today, Vol. 244 https://doi.org/10.1016/j.cattod.2014.07.009	journal	April 2015
Periodic trends of oxygen vacancy formation and C–H bond activation over transition metal-doped CeO2 (111) surfaces Krcha, Matthew D.; Mayernick, Adam D.; Janik, Michael J. Journal of Catalysis, Vol. 293 https://doi.org/10.1016/j.jcat.2012.06.010	journal	September 2012
Polyhydrido Copper Clusters: Synthetic Advances, Structural Diversity, and Nanocluster-to-Nanoparticle Conversion Dhayal, Rajendra S.; van Zyl, Werner E.; Liu, C. W. Accounts of Chemical Research, Vol. 49, Issue 1 https://doi.org/10.1021/acs.accounts.5b00375	journal	December 2015
Computational Insight into the Covalent Organic–Inorganic Interface Tang, Qing; Jiang, De-en Chemistry of Materials, Vol. 28, Issue 17 https://doi.org/10.1021/acs.chemmater.6b01740	journal	August 2016
Metallic Hydrogen in Atomically Precise Gold Nanoclusters Hu, Guoxiang; Tang, Qing; Lee, Dongil Chemistry of Materials, Vol. 29, Issue 11 https://doi.org/10.1021/acs.chemmater.7b00776	journal	May 2017
Atomically Precise Colloidal Metal Nanoclusters and Nanoparticles: Fundamentals and Opportunities Jin, Rongchao; Zeng, Chenjie; Zhou, Meng Chemical Reviews, Vol. 116, Issue 18 https://doi.org/10.1021/acs.chemrev.5b00703	journal	September 2016
Reactivity and Selectivity Descriptors for the Activation of C–H Bonds in Hydrocarbons and Oxygenates on Metal Oxides Deshlahra, Prashant; Iglesia, Enrique The Journal of Physical Chemistry C, Vol. 120, Issue 30 https://doi.org/10.1021/acs.jpcc.6b04604	journal	July 2016
First Principles Insight into H ₂ Activation and Hydride Species on TiO ₂ Surfaces Hu, Guoxiang; Wu, Zili; Jiang, De-en The Journal of Physical Chemistry C, Vol. 122, Issue 35 https://doi.org/10.1021/acs.jpcc.8b05251	journal	August 2018
Effect of Hydrogen-Induced Metallization on Chemisorption Gao, Yijing; Huang, Runhong; Wang, Jianguo The Journal of Physical Chemistry C, Vol. 123, Issue 24 https://doi.org/10.1021/acs.jpcc.9b04931	journal	May 2019
General Structure–Reactivity Relationship for Oxygen on Transition-Metal Oxides Fung, Victor; Tao, Franklin Feng; Jiang, De-en The Journal of Physical Chemistry Letters, Vol. 8, Issue 10 https://doi.org/10.1021/acs.jpclett.7b00861	journal	May 2017
New Bonding Model of Radical Adsorbate on Lattice Oxygen of Perovskites Fung, Victor; Wu, Zili; Jiang, De-en The Journal of Physical Chemistry Letters, Vol. 9, Issue 21 https://doi.org/10.1021/acs.jpclett.8b02749	journal	October 2018
Correlation of Methane Activation and Oxide Catalyst Reducibility and Its Implications for Oxidative Coupling Kumar, Gaurav; Lau, Sai Lap Jacky; Krcha, Matthew D. ACS Catalysis, Vol. 6, Issue 3 https://doi.org/10.1021/acscatal.5b02657	journal	February 2016
Toward More Complete Descriptors of Reactivity in Catalysis by Solid Acids Deshlahra, Prashant; Iglesia, Enrique ACS Catalysis, Vol. 6, Issue 8 https://doi.org/10.1021/acscatal.6b01402	journal	July 2016
Ru-Loaded C12A7:e ^– Electride as a Catalyst for Ammonia Synthesis Hara, Michikazu; Kitano, Masaaki; Hosono, Hideo ACS Catalysis, Vol. 7, Issue 4 https://doi.org/10.1021/acscatal.6b03357	journal	February 2017
Atomically Precise, Thiolated Copper–Hydride Nanoclusters as Single-Site Hydrogenation Catalysts for Ketones in Mild Conditions Sun, Cunfa; Mammen, Nisha; Kaappa, Sami ACS Nano, Vol. 13, Issue 5 https://doi.org/10.1021/acsnano.9b02052	journal	May 2019
Nature-Derived Approach to Oxygen and Chlorine Dual-Vacancies for Efficient Photocatalysis and Photoelectrochemistry Li, Min; Zhang, Yihe; Li, Xiaowei ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 2 https://doi.org/10.1021/acssuschemeng.7b03847	journal	December 2017
Tunable Ag Micromorphologies Show High Activities for Electrochemical H ₂ Evolution and CO ₂ Electrochemical Reduction Huang, Jing-Fang; Wu, Yi-Ching ACS Sustainable Chemistry & Engineering, Vol. 7, Issue 6 https://doi.org/10.1021/acssuschemeng.9b00116	journal	February 2019
Catalytic Dehydrogenation of Light Alkanes on Metals and Metal Oxides Sattler, Jesper J. H. B.; Ruiz-Martinez, Javier; Santillan-Jimenez, Eduardo Chemical Reviews, Vol. 114, Issue 20 https://doi.org/10.1021/cr5002436	journal	August 2014
C−H Bond Activation and Organometallic Intermediates on Isolated Metal Centers on Oxide Surfaces Coperet, Christophe Chemical Reviews, Vol. 110, Issue 2 https://doi.org/10.1021/cr900122p	journal	February 2010
From Superatomic Au ₂₅ (SR) ₁₈ ⁻ to Superatomic M@Au ₂₄ (SR) ₁₈ ^q Core−Shell Clusters Jiang, De-en; Dai, Sheng Inorganic Chemistry, Vol. 48, Issue 7 https://doi.org/10.1021/ic8024588	journal	April 2009
Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations Dronskowski, Richard; Bloechl, Peter E. The Journal of Physical Chemistry, Vol. 97, Issue 33 https://doi.org/10.1021/j100135a014	journal	August 1993
Controlling Gold Nanoclusters by Diphospine Ligands Chen, Jing; Zhang, Qian-Fan; Bonaccorso, Timary A. Journal of the American Chemical Society, Vol. 136, Issue 1 https://doi.org/10.1021/ja411061e	journal	December 2013
Size-Dependent Catalytic Activity of Supported Vanadium Oxide Species: Oxidative Dehydrogenation of Propane Rozanska, Xavier; Fortrie, Remy; Sauer, Joachim Journal of the American Chemical Society, Vol. 136, Issue 21 https://doi.org/10.1021/ja503130z	journal	May 2014
On the Structure of Thiolate-Protected Au ₂₅ Akola, Jaakko; Walter, Michael; Whetten, Robert L. Journal of the American Chemical Society, Vol. 130, Issue 12 https://doi.org/10.1021/ja800594p	journal	March 2008
Nature of Reactive Hydrogen for Ammonia Synthesis over a Ru/C12A7 Electride Catalyst Kammert, James; Moon, Jisue; Cheng, Yongqiang Journal of the American Chemical Society, Vol. 142, Issue 16 https://doi.org/10.1021/jacs.0c02345	journal	April 2020
A New Class of Atomically Precise, Hydride-Rich Silver Nanoclusters Co-Protected by Phosphines Bootharaju, Megalamane S.; Dey, Raju; Gevers, Lieven E. Journal of the American Chemical Society, Vol. 138, Issue 42 https://doi.org/10.1021/jacs.6b05482	journal	October 2016
The Formation of Ti–H Species at Interface Is Lethal to the Efficiency of TiO ₂ -Based Dye-Sensitized Devices Yan, Yan; Shi, Weidong; Yuan, Zhen Journal of the American Chemical Society, Vol. 139, Issue 5 https://doi.org/10.1021/jacs.6b12324	journal	January 2017
Lattice-Hydride Mechanism in Electrocatalytic CO ₂ Reduction by Structurally Precise Copper-Hydride Nanoclusters Tang, Qing; Lee, Yongjin; Li, Dai-Ying Journal of the American Chemical Society, Vol. 139, Issue 28 https://doi.org/10.1021/jacs.7b05591	journal	July 2017
Hydride-Doped Gold Superatom (Au ₉ H) ²⁺ : Synthesis, Structure, and Transformation Takano, Shinjiro; Hirai, Haru; Muramatsu, Satoru Journal of the American Chemical Society, Vol. 140, Issue 27 https://doi.org/10.1021/jacs.8b03880	journal	June 2018
Low-Temperature Synthesis of Perovskite Oxynitride-Hydrides as Ammonia Synthesis Catalysts Kitano, Masaaki; Kujirai, Jun; Ogasawara, Kiya Journal of the American Chemical Society, Vol. 141, Issue 51 https://doi.org/10.1021/jacs.9b10726	journal	November 2019
Why gold is the noblest of all the metals Hammer, B.; Norskov, J. K. Nature, Vol. 376, Issue 6537 https://doi.org/10.1038/376238a0	journal	July 1995
A molecule-like PtAu24(SC6H13)18 nanocluster as an electrocatalyst for hydrogen production Kwak, Kyuju; Choi, Woojun; Tang, Qing Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14723	journal	March 2017
A selective and efficient electrocatalyst for carbon dioxide reduction Lu, Qi; Rosen, Jonathan; Zhou, Yang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4242	journal	January 2014
Computational high-throughput screening of electrocatalytic materials for hydrogen evolution Greeley, Jeff; Jaramillo, Thomas F.; Bonde, Jacob Nature Materials, Vol. 5, Issue 11, p. 909-913 https://doi.org/10.1038/nmat1752	journal	October 2006
An oxyhydride of BaTiO3 exhibiting hydride exchange and electronic conductivity Kobayashi, Yoji; Hernandez, Olivier J.; Sakaguchi, Tatsunori Nature Materials, Vol. 11, Issue 6 https://doi.org/10.1038/nmat3302	journal	April 2012
Understanding trends in C–H bond activation in heterogeneous catalysis Latimer, Allegra A.; Kulkarni, Ambarish R.; Aljama, Hassan Nature Materials, Vol. 16, Issue 2 https://doi.org/10.1038/nmat4760	journal	October 2016
Machine learning hydrogen adsorption on nanoclusters through structural descriptors Jäger, Marc O. J.; Morooka, Eiaki V.; Federici Canova, Filippo npj Computational Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41524-018-0096-5	journal	July 2018
Identification of stable adsorption sites and diffusion paths on nanocluster surfaces: an automated scanning algorithm Szilvási, Tibor; Chen, Benjamin W. J.; Mavrikakis, Manos npj Computational Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41524-019-0240-x	journal	October 2019
Theory-guided design of catalytic materials using scaling relationships and reactivity descriptors Zhao, Zhi-Jian; Liu, Sihang; Zha, Shenjun Nature Reviews Materials, Vol. 4, Issue 12 https://doi.org/10.1038/s41578-019-0152-x	journal	November 2019
Accelerated discovery of CO2 electrocatalysts using active machine learning Zhong, Miao; Tran, Kevin; Min, Yimeng Nature, Vol. 581, Issue 7807 https://doi.org/10.1038/s41586-020-2242-8	journal	May 2020
The importance of being hydride Esposito, Davide Nature Catalysis, Vol. 1, Issue 12 https://doi.org/10.1038/s41929-018-0208-0	journal	December 2018
Two-dimensional copper nanosheets for electrochemical reduction of carbon monoxide to acetate Luc, Wesley; Fu, Xianbiao; Shi, Jianjian Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0269-8	journal	April 2019
Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis Wang, Yuhang; Wang, Ziyun; Dinh, Cao-Thang Nature Catalysis, Vol. 3, Issue 2 https://doi.org/10.1038/s41929-019-0397-1	journal	December 2019
Mechanistic insights into heterogeneous methane activation Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin Physical Chemistry Chemical Physics, Vol. 19, Issue 5 https://doi.org/10.1039/C6CP08003K	journal	January 2017
Essential role of hydride ion in ruthenium-based ammonia synthesis catalysts Kitano, Masaaki; Inoue, Yasunori; Ishikawa, Hiroki Chemical Science, Vol. 7, Issue 7 https://doi.org/10.1039/C6SC00767H	journal	January 2016
Exploring perovskites for methane activation from first principles Fung, Victor; Polo-Garzon, Felipe; Wu, Zili Catalysis Science & Technology, Vol. 8, Issue 3 https://doi.org/10.1039/C7CY01791J	journal	January 2018
Au ₂₅ (SR) ₁₈ : the captain of the great nanocluster ship Kang, Xi; Chong, Hanbao; Zhu, Manzhou Nanoscale, Vol. 10, Issue 23 https://doi.org/10.1039/C8NR02973C	journal	January 2018
Stronger-than-Pt hydrogen adsorption in a Au ₂₂ nanocluster for the hydrogen evolution reaction Hu, Guoxiang; Wu, Zili; Jiang, De-en Journal of Materials Chemistry A, Vol. 6, Issue 17 https://doi.org/10.1039/C8TA00461G	journal	January 2018
An effective structural descriptor to quantify the reactivity of lattice oxygen in CeO ₂ subnano-clusters Zhou, Chuan; Zhang, Binghu; Hu, P. Physical Chemistry Chemical Physics, Vol. 22, Issue 3 https://doi.org/10.1039/C9CP05805B	journal	January 2020
Formation of hydrocarbons in the electrochemical reduction of carbon dioxide at a copper electrode in aqueous solution Hori, Yoshio; Murata, Akira; Takahashi, Ryutaro Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 85, Issue 8 https://doi.org/10.1039/f19898502309	journal	January 1989
A comparative study of Hamilton and overlap population methods for the analysis of chemical bonding Glassey, Wingfield V.; Hoffmann, Roald The Journal of Chemical Physics, Vol. 113, Issue 5 https://doi.org/10.1063/1.481971	journal	August 2000
A unified view of ligand-protected gold clusters as superatom complexes Walter, M.; Akola, J.; Lopez-Acevedo, O. Proceedings of the National Academy of Sciences, Vol. 105, Issue 27 https://doi.org/10.1073/pnas.0801001105	journal	July 2008
Density functional theory in surface chemistry and catalysis Norskov, J. K.; Abild-Pedersen, F.; Studt, F. Proceedings of the National Academy of Sciences, Vol. 108, Issue 3 https://doi.org/10.1073/pnas.1006652108	journal	January 2011
Hydrogen-induced metallicity of SrTiO 3 (001) surfaces: A density functional theory study Lin, Feng; Wang, Shanying; Zheng, Fawei Physical Review B, Vol. 79, Issue 3 https://doi.org/10.1103/PhysRevB.79.035311	journal	January 2009
Hydrogen-Induced Surface Metallization of SrTiO 3 ( 001 ) D’Angelo, M.; Yukawa, R.; Ozawa, K. Physical Review Letters, Vol. 108, Issue 11 https://doi.org/10.1103/PhysRevLett.108.116802	journal	March 2012
Key role of antibonding electron transfer in bonding on solid surfaces Yu, Liping; Yan, Qimin; Ruzsinszky, Adrienn Physical Review Materials, Vol. 3, Issue 9 https://doi.org/10.1103/PhysRevMaterials.3.092801	journal	September 2019

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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References (58)

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