Electrostatic Origins of Linear Scaling Relationships at Bifunctional Metal/Oxide Interfaces: A Case Study of Au Nanoparticles on Doped MgO Substrates

Choksi, Tej; Majumdar, Paulami; Greeley, Jeffrey P.

doi:10.1002/anie.201808246

Title: Electrostatic Origins of Linear Scaling Relationships at Bifunctional Metal/Oxide Interfaces: A Case Study of Au Nanoparticles on Doped MgO Substrates

Journal Article · Wed Sep 12 00:00:00 EDT 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201808246· OSTI ID:1543475

Choksi, Tej ^[1]; Majumdar, Paulami ^[1];

^[1]

Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering

Linear scaling relationships (SRs), which relate binding energies of adsorbates across a space of catalyst surfaces, have been extensively explored for metal and oxide surfaces, but little is known about their properties at interfaces between metal nanoparticles and oxide supports, which are ubiquitous in heterogeneous catalysis. Using periodic DFT calculations, scaling principles are extended to bifunctional Au/oxide interfaces. Adopting a Au nanorod on doped MgO (100) as a model, SRs for species participating in water gas shift, methanol synthesis, and oxidation reactions are reported. SR slopes are not constrained by the bond order conservation rule postulated for metals, oxides, and zeolites, potentially permitting greater flexibility in catalyst design strategies. Finally, the deviation from bond counting, along with the physical origin of scaling behavior at interfaces, are explored using a conceptual framework involving electrostatic interactions at the Au/oxide interface.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1543475

Journal Information:: Angewandte Chemie (International Edition), Vol. 57, Issue 47; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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References (45)

O ₂ activation at the Au/MgO(001) interface boundary facilitates CO oxidation Duan, Zhiyao; Henkelman, Graeme Physical Chemistry Chemical Physics, Vol. 18, Issue 7 https://doi.org/10.1039/C5CP05558J	journal	January 2016
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
Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces Fernández, Eva M.; Moses, Poul G.; Toftelund, Anja Angewandte Chemie, Vol. 120, Issue 25 https://doi.org/10.1002/ange.200705739	journal	June 2008
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
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Methanol–Alkene Reactions in Zeotype Acid Catalysts: Insights from a Descriptor-Based Approach and Microkinetic Modeling Brogaard, Rasmus Y.; Wang, Chuan-Ming; Studt, Felix ACS Catalysis, Vol. 4, Issue 12 https://doi.org/10.1021/cs5014267	journal	November 2014
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
Catalysis by Doped Oxides McFarland, Eric W.; Metiu, Horia Chemical Reviews, Vol. 113, Issue 6 https://doi.org/10.1021/cr300418s	journal	December 2012
Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2 Graciani, J.; Mudiyanselage, K.; Xu, F. Science, Vol. 345, Issue 6196 https://doi.org/10.1126/science.1253057	journal	July 2014
Theoretical Heterogeneous Catalysis: Scaling Relationships and Computational Catalyst Design Greeley, Jeffrey Annual Review of Chemical and Biomolecular Engineering, Vol. 7, Issue 1 https://doi.org/10.1146/annurev-chembioeng-080615-034413	journal	June 2016
Universality in Heterogeneous Catalysis Nørskov, J. K.; Bligaard, T.; Logadottir, A. Journal of Catalysis, Vol. 209, Issue 2 https://doi.org/10.1006/jcat.2002.3615	journal	July 2002
Computational catalyst screening: Scaling, bond-order and catalysis Abild-Pedersen, Frank Catalysis Today, Vol. 272 https://doi.org/10.1016/j.cattod.2015.08.056	journal	September 2016
Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO ₂ Reduction to CO Hansen, Heine A.; Varley, Joel B.; Peterson, Andrew A. The Journal of Physical Chemistry Letters, Vol. 4, Issue 3 https://doi.org/10.1021/jz3021155	journal	January 2013
Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol Studt, Felix; Sharafutdinov, Irek; Abild-Pedersen, Frank Nature Chemistry, Vol. 6, Issue 4 https://doi.org/10.1038/nchem.1873	journal	March 2014
Scaling Relationships for Molecular Adsorption and Dissociation in Lewis Acid Zeolites Bukowski, Brandon C.; Greeley, Jeffrey The Journal of Physical Chemistry C, Vol. 120, Issue 12 https://doi.org/10.1021/acs.jpcc.6b01157	journal	March 2016
Adsorption Energy Correlations at the Metal–Support Boundary Mehta, Prateek; Greeley, Jeffrey; Delgass, W. Nicholas ACS Catalysis, Vol. 7, Issue 7 https://doi.org/10.1021/acscatal.7b00979	journal	June 2017
Ab initio molecular dynamics for open-shell transition metals Kresse, G.; Hafner, J. Physical Review B, Vol. 48, Issue 17 https://doi.org/10.1103/PhysRevB.48.13115	journal	November 1993
Importance of metal-oxide interfaces in heterogeneous catalysis: A combined DFT, microkinetic, and experimental study of water-gas shift on Au/MgO Zhao, Zhi-Jian; Li, Zhenglong; Cui, Yanran Journal of Catalysis, Vol. 345 https://doi.org/10.1016/j.jcat.2016.11.008	journal	January 2017
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
Relaxed core projector-augmented-wave method Marsman, M.; Kresse, G. The Journal of Chemical Physics, Vol. 125, Issue 10 https://doi.org/10.1063/1.2338035	journal	September 2006
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
Scaling Properties of Adsorption Energies for Hydrogen-Containing Molecules on Transition-Metal Surfaces Abild-Pedersen, F.; Greeley, J.; Studt, F. Physical Review Letters, Vol. 99, Issue 1 https://doi.org/10.1103/PhysRevLett.99.016105	journal	July 2007
Trends in methanol decomposition on transition metal alloy clusters from scaling and Brønsted–Evans–Polanyi relationships Mehmood, Faisal; Rankin, Rees B.; Greeley, Jeffrey Physical Chemistry Chemical Physics, Vol. 14, Issue 24 https://doi.org/10.1039/c2cp00052k	journal	January 2012
A fast and robust algorithm for Bader decomposition of charge density Henkelman, Graeme; Arnaldsson, Andri; Jónsson, Hannes Computational Materials Science, Vol. 36, Issue 3 https://doi.org/10.1016/j.commatsci.2005.04.010	journal	June 2006
How Doped MoS ₂ Breaks Transition-Metal Scaling Relations for CO ₂ Electrochemical Reduction Hong, Xin; Chan, Karen; Tsai, Charlie ACS Catalysis, Vol. 6, Issue 7 https://doi.org/10.1021/acscatal.6b00619	journal	June 2016
Scaling Relationships for Binding Energies of Transition Metal Complexes Wang, Ying; Montoya, Joseph H.; Tsai, Charlie Catalysis Letters, Vol. 146, Issue 2 https://doi.org/10.1007/s10562-015-1667-4	journal	December 2015
Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces Fernández, Eva M.; Moses, Poul G.; Toftelund, Anja Angewandte Chemie International Edition, Vol. 47, Issue 25 https://doi.org/10.1002/anie.200705739	journal	June 2008
Analyzing the Case for Bifunctional Catalysis Andersen, Mie; Medford, Andrew J.; Nørskov, Jens K. Angewandte Chemie International Edition, Vol. 55, Issue 17 https://doi.org/10.1002/anie.201601049	journal	March 2016
New design paradigm for heterogeneous catalysts Vojvodic, Aleksandra; Nørskov, Jens K. National Science Review, Vol. 2, Issue 2 https://doi.org/10.1093/nsr/nwv023	journal	April 2015
Tuning the surface metal work function by deposition of ultrathin oxide films: Density functional calculations Giordano, Livia; Cinquini, Fabrizio; Pacchioni, Gianfranco Physical Review B, Vol. 73, Issue 4 https://doi.org/10.1103/PhysRevB.73.045414	journal	January 2006
The Theory of Intermolecular Forces Stone, Anthony Oxford University Press https://doi.org/10.1093/acprof:oso/9780199672394.001.0001	book	January 2013
Towards the computational design of solid catalysts Nørskov, J.; Bligaard, T.; Rossmeisl, J. Nature Chemistry, Vol. 1, Issue 1, p. 37-46 https://doi.org/10.1038/nchem.121	journal	April 2009
Nature of Lone-Pair–Surface Bonds and Their Scaling Relations Kakekhani, Arvin; Roling, Luke T.; Kulkarni, Ambarish Inorganic Chemistry, Vol. 57, Issue 12 https://doi.org/10.1021/acs.inorgchem.8b00902	journal	June 2018
Analyzing the Case for Bifunctional Catalysis Andersen, Mie; Medford, Andrew J.; Nørskov, Jens K. Angewandte Chemie, Vol. 128, Issue 17 https://doi.org/10.1002/ange.201601049	journal	March 2016
Active Role of Oxide Support during CO Oxidation at $A u / M g O$ Molina, L. M.; Hammer, B. Physical Review Letters, Vol. 90, Issue 20 https://doi.org/10.1103/PhysRevLett.90.206102	journal	May 2003
Surface Dipoles and Electron Transfer at the Metal Oxide–Metal Interface: A 2PPE Study of Size-Selected Metal Oxide Clusters Supported on Cu(111) Yang, Yixiong; Zhou, Jia; Nakayama, Miki The Journal of Physical Chemistry C, Vol. 118, Issue 25 https://doi.org/10.1021/jp503646u	journal	June 2014
Scaling relations between adsorption energies for computational screening and design of catalysts Montemore, Matthew M.; Medlin, J. Will Catal. Sci. Technol., Vol. 4, Issue 11 https://doi.org/10.1039/C4CY00335G	journal	January 2014
Breaking scaling relations to achieve low-temperature ammonia synthesis through LiH-mediated nitrogen transfer and hydrogenation Wang, Peikun; Chang, Fei; Gao, Wenbo Nature Chemistry, Vol. 9, Issue 1 https://doi.org/10.1038/nchem.2595	journal	August 2016
Establishing and Understanding Adsorption–Energy Scaling Relations with Negative Slopes Su, Hai-Yan; Sun, Keju; Wang, Wei-Qi The Journal of Physical Chemistry Letters, Vol. 7, Issue 24 https://doi.org/10.1021/acs.jpclett.6b02430	journal	November 2016
How covalence breaks adsorption-energy scaling relations and solvation restores them Calle-Vallejo, Federico; Krabbe, Alexander; García-Lastra, Juan M. Chemical Science, Vol. 8, Issue 1 https://doi.org/10.1039/C6SC02123A	journal	January 2017
Size and Support Effects for the Water–Gas Shift Catalysis over Gold Nanoparticles Supported on Model Al ₂ O ₃ and TiO ₂ Shekhar, Mayank; Wang, Jun; Lee, Wen-Sheng Journal of the American Chemical Society, Vol. 134, Issue 10 https://doi.org/10.1021/ja210083d	journal	February 2012
Alloys of platinum and early transition metals as oxygen reduction electrocatalysts Greeley, J.; Stephens, I. E. L.; Bondarenko, A. S. Nature Chemistry, Vol. 1, Issue 7, p. 552-556 https://doi.org/10.1038/nchem.367	journal	September 2009
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets Chen, Ruyi; Cui, Qirui; Liao, Liyang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23414-3	journal	May 2021
High-resolution X-ray luminescence extension imaging Ou, Xiangyu; Qin, Xian; Huang, Bolong Nature, Vol. 590, Issue 7846 https://doi.org/10.1038/s41586-021-03251-6	journal	February 2021
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-58835-5	journal	February 2020

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Strategies to break linear scaling relationships Pérez-Ramírez, Javier; López, Núria Nature Catalysis, Vol. 2, Issue 11 https://doi.org/10.1038/s41929-019-0376-6	journal	October 2019
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