Unraveling Electronic Trends in O* and OH* Surface Adsorption in the MO2 Transition-Metal Oxide Series

Comer, Benjamin M.; Li, Jiang; Abild-Pedersen, Frank; Bajdich, Michal; Winther, Kirsten T.

doi:10.1021/acs.jpcc.2c02381

Unraveling Electronic Trends in O* and OH* Surface Adsorption in the MO₂ Transition-Metal Oxide Series

Journal Article · Wed Apr 27 00:00:00 EDT 2022 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.2c02381· OSTI ID:1875698

Comer, Benjamin M. ^[1]; ^[1]; ^[2]; ^[2]; ^[2]

Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

Understanding the bond strength of O* and OH* intermediates to metal-oxide surfaces is key to predicting the catalytic activity in oxygen-based electrochemistry. Here, we uncover highly non-linear trends in O* and OH* adsorption energies across the 3d, 4d, and 5d series of MO₂ transition-metal (TM) oxide surfaces computed within Hubbard-U corrected density functional theory (DFT + U). Investigating the electronic structure with crystal orbital Hamiltonian populations (COHP) of the relevant metal–oxygen bonds reveals that the spin-dependent coupling strength between metal-d and oxygen-2p atomic orbitals together with the extent of filling of bonding and anti-bonding orbitals are the primary contributors to the adsorption energy. Importantly, we show that the integrated COHP obtained purely from bulk calculations is a highly accurate descriptor for surface adsorption energetics that captures trends across the group 5–12 TM oxide series within 0.19–0.36 eV. Our results suggest a pathway to prediction of adsorption energies for an arbitrary metal–ligand catalyst system.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231

OSTI ID:: 1875698

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 18 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Modern Heterogeneous Catalysis Santen, Rutger A. https://doi.org/10.1002/9783527810253	book	February 2017
Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces Man, Isabela C.; Su, Hai‐Yan; Calle‐Vallejo, Federico ChemCatChem, Vol. 3, Issue 7 https://doi.org/10.1002/cctc.201000397	journal	March 2011
Trends in Oxygen Electrocatalysis of 3 d ‐Layered (Oxy)(Hydro)Oxides Zhao, Zhenghang; Schlexer Lamoureux, Philomena; Kulkarni, Ambarish ChemCatChem, Vol. 11, Issue 15 https://doi.org/10.1002/cctc.201900846	journal	June 2019
LOBSTER: A tool to extract chemical bonding from plane-wave based DFT: Tool to Extract Chemical Bonding Maintz, Stefan; Deringer, Volker L.; Tchougréeff, Andrei L. Journal of Computational Chemistry, Vol. 37, Issue 11 https://doi.org/10.1002/jcc.24300	journal	February 2016
LOBSTER : Local orbital projections, atomic charges, and chemical‐bonding analysis from projector‐augmented‐wave‐based density‐functional theory Nelson, Ryky; Ertural, Christina; George, Janine Journal of Computational Chemistry, Vol. 41, Issue 21 https://doi.org/10.1002/jcc.26353	journal	June 2020
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
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
Electrolysis of water on oxide surfaces Rossmeisl, J.; Qu, Z. -W.; Zhu, H. Journal of Electroanalytical Chemistry, Vol. 607, Issue 1-2 https://doi.org/10.1016/j.jelechem.2006.11.008	journal	September 2007
An electronic structure descriptor for oxygen reactivity at metal and metal-oxide surfaces Dickens, Colin F.; Montoya, Joseph H.; Kulkarni, Ambarish R. Surface Science, Vol. 681 https://doi.org/10.1016/j.susc.2018.11.019	journal	March 2019
Electrocatalysis by oxides — Attempt at a unifying approach Trasatti, Sergio Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 111, Issue 1 https://doi.org/10.1016/s0022-0728(80)80084-2	journal	July 1980
The origin of ideas on a Hydrogen Economy and its solution to the decay of the environment Bockris, J. International Journal of Hydrogen Energy, Vol. 27, Issue 7-8 https://doi.org/10.1016/s0360-3199(01)00154-9	journal	August 2002
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
Mineralogical Applications of Crystal Field Theory Burns, Roger G. Cambridge University Press https://doi.org/10.1017/CBO9780511524899	book	January 2009
Statistical Analysis of Coordination Environments in Oxides Waroquiers, David; Gonze, Xavier; Rignanese, Gian-Marco Chemistry of Materials, Vol. 29, Issue 19 https://doi.org/10.1021/acs.chemmater.7b02766	journal	September 2017
Understanding Catalytic Activity Trends in the Oxygen Reduction Reaction Kulkarni, Ambarish; Siahrostami, Samira; Patel, Anjli Chemical Reviews, Vol. 118, Issue 5 https://doi.org/10.1021/acs.chemrev.7b00488	journal	December 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
Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan ACS Catalysis, Vol. 2, Issue 8 https://doi.org/10.1021/cs300227s	journal	July 2012
Why Is Bulk Thermochemistry a Good Descriptor for the Electrocatalytic Activity of Transition Metal Oxides? Calle-Vallejo, Federico; Díaz-Morales, Oscar A.; Kolb, Manuel J. ACS Catalysis, Vol. 5, Issue 2 https://doi.org/10.1021/cs5016657	journal	January 2015
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
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
Crystal Orbital Hamilton Population (COHP) Analysis As Projected from Plane-Wave Basis Sets Deringer, Volker L.; Tchougréeff, Andrei L.; Dronskowski, Richard The Journal of Physical Chemistry A, Vol. 115, Issue 21 https://doi.org/10.1021/jp202489s	journal	June 2011
Electronic Origin of the Surface Reactivity of Transition-Metal-Doped TiO ₂ (110) García-Mota, Mónica; Vojvodic, Aleksandra; Abild-Pedersen, Frank The Journal of Physical Chemistry C, Vol. 117, Issue 1 https://doi.org/10.1021/jp310667r	journal	December 2012
Catalysis-Hub.org, an open electronic structure database for surface reactions Winther, Kirsten T.; Hoffmann, Max J.; Boes, Jacob R. Scientific Data, Vol. 6, Issue 1 https://doi.org/10.1038/s41597-019-0081-y	journal	May 2019
Understanding of metal-insulator transition in VO2 based on experimental and theoretical investigations of magnetic features Zhang, R.; Fu, Q. S.; Yin, C. Y. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-35490-5	journal	November 2018
Number of outer electrons as descriptor for adsorption processes on transition metals and their oxides Calle-Vallejo, Federico; Inoglu, Nilay G.; Su, Hai-Yan Chemical Science, Vol. 4, Issue 3 https://doi.org/10.1039/c2sc21601a	journal	January 2013
Crystal and Ligand Field Models of Solid Catalysts Dowden, D. A. Catalysis Reviews, Vol. 5, Issue 1 https://doi.org/10.1080/01614947208076863	journal	January 1972
The Inorganic Crystal Structure Database (ICSD)—Present and Future Hellenbrandt, Mariette Crystallography Reviews, Vol. 10, Issue 1 https://doi.org/10.1080/08893110410001664882	journal	January 2004
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/physrevb.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/physrevb.49.14251	journal	May 1994
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
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
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/physrevb.59.1758	journal	January 1999
Evaluating optimal U for 3 d transition-metal oxides within the SCAN+ U framework Long, Olivia Y.; Sai Gautam, Gopalakrishnan; Carter, Emily A. Physical Review Materials, Vol. 4, Issue 4 https://doi.org/10.1103/physrevmaterials.4.045401	journal	April 2020
A Perovskite Oxide Optimized for Oxygen Evolution Catalysis from Molecular Orbital Principles Suntivich, J.; May, K. J.; Gasteiger, H. A. Science, Vol. 334, Issue 6061 https://doi.org/10.1126/science.1212858	journal	October 2011
Optimizing Perovskites for the Water-Splitting Reaction Vojvodic, A.; Norskov, J. K. Science, Vol. 334, Issue 6061 https://doi.org/10.1126/science.1215081	journal	December 2011
Combining theory and experiment in electrocatalysis: Insights into materials design Seh, Zhi Wei; Kibsgaard, Jakob; Dickens, Colin F. Science, Vol. 355, Issue 6321 https://doi.org/10.1126/science.aad4998	journal	January 2017

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Unraveling Electronic Trends in O* and OH* Surface Adsorption in the MO2 Transition-Metal Oxide Series

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Unraveling Electronic Trends in O* and OH* Surface Adsorption in the MO₂ Transition-Metal Oxide Series