Charting C–C coupling pathways in electrochemical CO 2 reduction on Cu(111) using embedded correlated wavefunction theory

Zhao, Qing; Martirez, John Mark P.; Carter, Emily A.

doi:10.1073/pnas.2202931119

Title: Charting C–C coupling pathways in electrochemical CO ₂ reduction on Cu(111) using embedded correlated wavefunction theory

Journal Article · Fri Oct 28 00:00:00 EDT 2022 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.2202931119· OSTI ID:1895198

Zhao, Qing ^[1];

^[2];

^[3]

Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ 08544-5263
Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095-1592
Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ 08544-5263, Department of Chemical and Biomolecular Engineering, University of California, Los Angeles, CA 90095-1592, Andlinger Center for Energy and the Environment, Princeton University, Princeton, NJ 08544-5263

The electrochemical CO₂ reduction reaction (CO₂RR) powered by excess zero-carbon-emission electricity to produce especially multicarbon (C₂₊) products could contribute to a carbon-neutral to carbon-negative economy. Foundational to the rational design of efficient, selective CO₂RR electrocatalysts is mechanistic analysis of the best metal catalyst thus far identified, namely, copper (Cu), via quantum mechanical computations to complement experiments. Here, we apply embedded correlated wavefunction (ECW) theory, which regionally corrects the electron exchange-correlation error in density functional theory (DFT) approximations, to examine multiple C–C coupling steps involving adsorbed CO (*CO) and its hydrogenated derivatives on the most ubiquitous facet, Cu(111). We predict that two adsorbed hydrogenated CO species, either *COH or *CHO, are necessary precursors for C–C bond formation. The three kinetically feasible pathways involving these species yield all three possible products: *COH–CHO, *COH–*COH, and *OCH–*OCH. The most kinetically favorable path forms *COH–CHO. In contrast, standard DFT approximations arrive at qualitatively different conclusions, namely, that only *CO and *COH will prevail on the surface and their C–C coupling paths produce only *COH–*COH and *CO–*CO, with a preference for the first product. Furthermore, this work demonstrates the importance of applying qualitatively and quantitatively accurate quantum mechanical method to simulate electrochemistry in order ultimately to shed light on ways to enhance selectivity toward C₂₊ product formation via CO₂RR electrocatalysts.

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Research Organization:: Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1895198

Alternate ID(s):: OSTI ID: 1962800; OSTI ID: 1963053

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 119 Journal Issue: 44; ISSN 0027-8424

Publisher:: Proceedings of the National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (86)

Theoretical Considerations on the Electroreduction of CO to C ₂ Species on Cu(100) Electrodes Calle-Vallejo, Federico; Koper, Marc T. M. Angewandte Chemie International Edition, Vol. 52, Issue 28 https://doi.org/10.1002/anie.201301470	journal	June 2013
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
Atomistic Mechanisms Underlying Selectivities in C ₁ and C ₂ Products from Electrochemical Reduction of CO on Cu(111) Xiao, Hai; Cheng, Tao; Goddard, William A. Journal of the American Chemical Society, Vol. 139, Issue 1 https://doi.org/10.1021/jacs.6b06846	journal	December 2016
A quantum theory of molecular structure and its applications Bader, Richard F. W. Chemical Reviews, Vol. 91, Issue 5 https://doi.org/10.1021/cr00005a013	journal	July 1991
Facet Dependence of CO ₂ Reduction Paths on Cu Electrodes Luo, Wenjia; Nie, Xiaowa; Janik, Michael J. ACS Catalysis, Vol. 6, Issue 1 https://doi.org/10.1021/acscatal.5b01967	journal	December 2015
Highly Electrocatalytic Ethylene Production from CO ₂ on Nanodefective Cu Nanosheets Zhang, Bingxing; Zhang, Jianling; Hua, Manli Journal of the American Chemical Society, Vol. 142, Issue 31 https://doi.org/10.1021/jacs.0c06420	journal	July 2020
Quantum mechanical embedding theory based on a unique embedding potential Huang, Chen; Pavone, Michele; Carter, Emily A. The Journal of Chemical Physics, Vol. 134, Issue 15 https://doi.org/10.1063/1.3577516	journal	April 2011
Advances in Correlated Electronic Structure Methods for Solids, Surfaces, and Nanostructures Huang, Patrick; Carter, Emily A. Annual Review of Physical Chemistry, Vol. 59, Issue 1 https://doi.org/10.1146/annurev.physchem.59.032607.093528	journal	May 2008
Multiconfigurational perturbation theory with level shift — the Cr2 potential revisited Roos, Björn O.; Andersson, Kerstin Chemical Physics Letters, Vol. 245, Issue 2-3 https://doi.org/10.1016/0009-2614(95)01010-7	journal	October 1995
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
Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution Monteiro, Mariana C. O.; Dattila, Federico; Hagedoorn, Bellenod Nature Catalysis, Vol. 4, Issue 8 https://doi.org/10.1038/s41929-021-00655-5	journal	July 2021
Electrochemical CO₂ Reduction on Metal Electrodes Hori, Y.; Vayenas, Constantinos G.; White, Ralph E. Modern Aspects of Electrochemistry, p. 89-189 https://doi.org/10.1007/978-0-387-49489-0_3	book	January 2008
The complete active space SCF method in a fock-matrix-based super-CI formulation Roos, Björn O. International Journal of Quantum Chemistry, Vol. 18, Issue S14 https://doi.org/10.1002/qua.560180822	journal	March 1980
Molpro: a general-purpose quantum chemistry program package: Molpro Werner, Hans-Joachim; Knowles, Peter J.; Knizia, Gerald Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 2, Issue 2 https://doi.org/10.1002/wcms.82	journal	July 2011
Theoretical Insights into Heterogeneous (Photo)electrochemical CO 2 Reduction Xu, Shenzhen; Carter, Emily A. Chemical Reviews, Vol. 119, Issue 11 https://doi.org/10.1021/acs.chemrev.8b00481	journal	October 2018
Density and Potential Functional Embedding: Theory and Practice Yu, Kuang; Krauter, Caroline M.; Dieterich, Johannes M. Fragmentation: Toward Accurate Calculations on Complex Molecular Systems https://doi.org/10.1002/9781119129271.ch2	book	January 2017
Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal electrodes in aqueous media Hori, Yoshio; Wakebe, Hidetoshi; Tsukamoto, Toshio Electrochimica Acta, Vol. 39, Issue 11-12, p. 1833-1839 https://doi.org/10.1016/0013-4686(94)85172-7	journal	August 1994
Atomistic Insight into Cation Effects on Binding Energies in Cu-Catalyzed Carbon Dioxide Reduction Ludwig, Thomas; Gauthier, Joseph A.; Dickens, Colin F. The Journal of Physical Chemistry C, Vol. 124, Issue 45 https://doi.org/10.1021/acs.jpcc.0c07004	journal	November 2020
Norm-conserving and ultrasoft pseudopotentials for first-row and transition elements Kresse, G.; Hafner, J. Journal of Physics: Condensed Matter, Vol. 6, Issue 40 https://doi.org/10.1088/0953-8984/6/40/015	journal	October 1994
A grid-based Bader analysis algorithm without lattice bias Tang, W.; Sanville, E.; Henkelman, G. Journal of Physics: Condensed Matter, Vol. 21, Issue 8 https://doi.org/10.1088/0953-8984/21/8/084204	journal	January 2009
Stable Surfaces That Bind Too Tightly: Can Range-Separated Hybrids or DFT+U Improve Paradoxical Descriptions of Surface Chemistry? Zhao, Qing; Kulik, Heather J. The Journal of Physical Chemistry Letters, Vol. 10, Issue 17 https://doi.org/10.1021/acs.jpclett.9b01650	journal	August 2019
Ab initio effective core potentials for molecular calculations. Potentials for K to Au including the outermost core orbitals Hay, P. Jeffrey; Wadt, Willard R. The Journal of Chemical Physics, Vol. 82, Issue 1, p. 299-310 https://doi.org/10.1063/1.448975	journal	January 1985
The influence of pH on the reduction of CO and ${CO}_{2}$ to hydrocarbons on copper electrodes Schouten, Klaas Jan P.; Pérez Gallent, Elena; Koper, Marc T. M. Journal of Electroanalytical Chemistry, Vol. 716 https://doi.org/10.1016/j.jelechem.2013.08.033	journal	March 2014
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
Origin of the Energy Barrier to Chemical Reactions of $O_{2}$ on Al(111): Evidence for Charge Transfer, Not Spin Selection Libisch, Florian; Huang, Chen; Liao, Peilin Physical Review Letters, Vol. 109, Issue 19 https://doi.org/10.1103/PhysRevLett.109.198303	journal	November 2012
Identification of Cu(100)/Cu(111) Interfaces as Superior Active Sites for CO Dimerization During CO ₂ Electroreduction Wu, Zhi-Zheng; Zhang, Xiao-Long; Niu, Zhuang-Zhuang Journal of the American Chemical Society, Vol. 144, Issue 1 https://doi.org/10.1021/jacs.1c09508	journal	December 2021
Periodic boundary conditions in ab initio calculations Makov, G.; Payne, M. C. Physical Review B, Vol. 51, Issue 7 https://doi.org/10.1103/PhysRevB.51.4014	journal	February 1995
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen Dunning, Thom H. The Journal of Chemical Physics, Vol. 90, Issue 2 https://doi.org/10.1063/1.456153	journal	January 1989
Improved CO Adsorption Energies, Site Preferences, and Surface Formation Energies from a Meta-Generalized Gradient Approximation Exchange–Correlation Functional, M06-L Luo, Sijie; Zhao, Yan; Truhlar, Donald G. The Journal of Physical Chemistry Letters, Vol. 3, Issue 20 https://doi.org/10.1021/jz301182a	journal	September 2012
The Role of Cation Acidity on the Competition between Hydrogen Evolution and CO ₂ Reduction on Gold Electrodes Monteiro, Mariana C. O.; Dattila, Federico; López, Núria Journal of the American Chemical Society, Vol. 144, Issue 4 https://doi.org/10.1021/jacs.1c10171	journal	December 2021
A benchmark database for adsorption bond energies to transition metal surfaces and comparison to selected DFT functionals Wellendorff, Jess; Silbaugh, Trent L.; Garcia-Pintos, Delfina Surface Science, Vol. 640 https://doi.org/10.1016/j.susc.2015.03.023	journal	October 2015
Embedded Configuration Interaction Description of CO on Cu(111): Resolution of the Site Preference Conundrum Sharifzadeh, Sahar; Huang, Patrick; Carter, Emily The Journal of Physical Chemistry C, Vol. 112, Issue 12 https://doi.org/10.1021/jp710890a	journal	March 2008
Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K Cheng, Tao; Xiao, Hai; Goddard, William A. Proceedings of the National Academy of Sciences, Vol. 114, Issue 8 https://doi.org/10.1073/pnas.1612106114	journal	February 2017
Understanding cation effects in electrochemical CO ₂ reduction Ringe, Stefan; Clark, Ezra L.; Resasco, Joaquin Energy & Environmental Science, Vol. 12, Issue 10 https://doi.org/10.1039/C9EE01341E	journal	January 2019
Engineering Catalyst–Electrolyte Microenvironments to Optimize the Activity and Selectivity for the Electrochemical Reduction of CO ₂ on Cu and Ag Bui, Justin C.; Kim, Chanyeon; King, Alex J. Accounts of Chemical Research, Vol. 55, Issue 4 https://doi.org/10.1021/acs.accounts.1c00650	journal	February 2022
PRODUCTION OF CO AND CH ₄ IN ELECTROCHEMICAL REDUCTION OF CO ₂ AT METAL ELECTRODES IN AQUEOUS HYDROGENCARBONATE SOLUTION Hori, Yoshio; Kikuchi, Katsuhei; Suzuki, Shin Chemistry Letters, Vol. 14, Issue 11 https://doi.org/10.1246/cl.1985.1695	journal	November 1985
Implicit self-consistent electrolyte model in plane-wave density-functional theory Mathew, Kiran; Kolluru, V. S. Chaitanya; Mula, Srinidhi The Journal of Chemical Physics, Vol. 151, Issue 23 https://doi.org/10.1063/1.5132354	journal	December 2019
A modified definition of the zeroth-order Hamiltonian in multiconfigurational perturbation theory (CASPT2) Ghigo, Giovanni; Roos, Björn O.; Malmqvist, Per-Åke Chemical Physics Letters, Vol. 396, Issue 1-3 https://doi.org/10.1016/j.cplett.2004.08.032	journal	September 2004
Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation Wellendorff, Jess; Lundgaard, Keld T.; Møgelhøj, Andreas Physical Review B, Vol. 85, Issue 23 https://doi.org/10.1103/PhysRevB.85.235149	journal	June 2012
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
High-precision sampling for Brillouin-zone integration in metals Methfessel, M.; Paxton, A. T. Physical Review B, Vol. 40, Issue 6 https://doi.org/10.1103/PhysRevB.40.3616	journal	August 1989
Acetaldehyde as an Intermediate in the Electroreduction of Carbon Monoxide to Ethanol on Oxide-Derived Copper Bertheussen, Erlend; Verdaguer-Casadevall, Arnau; Ravasio, Davide Angewandte Chemie International Edition, Vol. 55, Issue 4 https://doi.org/10.1002/anie.201508851	journal	December 2015
CO adsorption on the Cu(111) surface: A density functional study Neef, M.; Doll, K. Surface Science, Vol. 600, Issue 5 https://doi.org/10.1016/j.susc.2005.12.036	journal	March 2006
The complete active space SCF (CASSCF) method in a Newton–Raphson formulation with application to the HNO molecule Siegbahn, Per E. M.; Almlöf, Jan; Heiberg, Anders The Journal of Chemical Physics, Vol. 74, Issue 4 https://doi.org/10.1063/1.441359	journal	February 1981
Electrochemical CO ₂ Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design Kibria, Md Golam; Edwards, Jonathan P.; Gabardo, Christine M. Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201807166	journal	December 2018
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Theoretical Insights into a CO Dimerization Mechanism in CO ₂ Electroreduction Montoya, Joseph H.; Shi, Chuan; Chan, Karen The Journal of Physical Chemistry Letters, Vol. 6, Issue 11 https://doi.org/10.1021/acs.jpclett.5b00722	journal	May 2015
Insights into Current Limitations of Density Functional Theory Cohen, A. J.; Mori-Sanchez, P.; Yang, W. Science, Vol. 321, Issue 5890 https://doi.org/10.1126/science.1158722	journal	August 2008
How pH affects electrochemical processes Govindarajan, Nitish; Xu, Aoni; Chan, Karen Science, Vol. 375, Issue 6579 https://doi.org/10.1126/science.abj2421	journal	January 2022
Determination of Site Specific Adsorption Energies of CO on Copper Vollmer, Stefan; Witte, Gregor; Wöll, Christof Catalysis Letters, Vol. 77, Issue 1/3, p. 97-101 https://doi.org/10.1023/A:1012755616064	journal	January 2001
Progress and Perspectives of Electrochemical CO ₂ Reduction on Copper in Aqueous Electrolyte Nitopi, Stephanie; Bertheussen, Erlend; Scott, Soren B. Chemical Reviews, Vol. 119, Issue 12 https://doi.org/10.1021/acs.chemrev.8b00705	journal	April 2019
Revisiting Competing Paths in Electrochemical CO ₂ Reduction on Copper via Embedded Correlated Wavefunction Theory Zhao, Qing; Carter, Emily A. Journal of Chemical Theory and Computation, Vol. 16, Issue 10 https://doi.org/10.1021/acs.jctc.0c00583	journal	August 2020
Screening Surface Structure–Electrochemical Activity Relationships of Copper Electrodes under CO₂ Electroreduction Conditions Wahab, Oluwasegun J.; Kang, Minkyung; Daviddi, Enrico ACS Catalysis, Vol. 12, Issue 11 https://doi.org/10.1021/acscatal.2c01650	journal	May 2022
Benchmarking an Embedded Adaptive Sampling Configuration Interaction Method for Surface Reactions: H ₂ Desorption from and CH ₄ Dissociation on Cu(111) Zhao, Qing; Zhang, Xing; Martirez, John Mark P. Journal of Chemical Theory and Computation, Vol. 16, Issue 11 https://doi.org/10.1021/acs.jctc.0c00341	journal	October 2020
Effect of the damping function in dispersion corrected density functional theory Grimme, Stefan; Ehrlich, Stephan; Goerigk, Lars Journal of Computational Chemistry, Vol. 32, Issue 7 https://doi.org/10.1002/jcc.21759	journal	March 2011
Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways Mathew, Kiran; Sundararaman, Ravishankar; Letchworth-Weaver, Kendra The Journal of Chemical Physics, Vol. 140, Issue 8 https://doi.org/10.1063/1.4865107	journal	February 2014
Mechanism of CO ₂ Reduction at Copper Surfaces: Pathways to C ₂ Products Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin ACS Catalysis, Vol. 8, Issue 2 https://doi.org/10.1021/acscatal.7b03477	journal	January 2018
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
Two Pathways for the Formation of Ethylene in CO Reduction on Single-Crystal Copper Electrodes Schouten, Klaas Jan P.; Qin, Zisheng; Pérez Gallent, Elena Journal of the American Chemical Society, Vol. 134, Issue 24 https://doi.org/10.1021/ja302668n	journal	June 2012
CO adsorption studies on pure and Ni-covered Cu(111) surfaces Kirstein, W.; Krüger, B.; Thieme, F. Surface Science, Vol. 176, Issue 3 https://doi.org/10.1016/0039-6028(86)90052-X	journal	November 1986
Embedded Correlated Wavefunction Schemes: Theory and Applications Libisch, Florian; Huang, Chen; Carter, Emily A. Accounts of Chemical Research, Vol. 47, Issue 9 https://doi.org/10.1021/ar500086h	journal	May 2014
Multireference perturbation theory for large restricted and selected active space reference wave functions Celani, Paolo; Werner, Hans-Joachim The Journal of Chemical Physics, Vol. 112, Issue 13 https://doi.org/10.1063/1.481132	journal	April 2000
Towards constant potential modeling of CO-CO coupling at liquid water-Cu(1 0 0) interfaces Kristoffersen, Henrik H.; Chan, Karen Journal of Catalysis, Vol. 396 https://doi.org/10.1016/j.jcat.2021.02.023	journal	April 2021
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Electric Field Effects in Electrochemical CO ₂ Reduction Chen, Leanne D.; Urushihara, Makoto; Chan, Karen ACS Catalysis, Vol. 6, Issue 10 https://doi.org/10.1021/acscatal.6b02299	journal	September 2016
Structure- and Potential-Dependent Cation Effects on CO Reduction at Copper Single-Crystal Electrodes Pérez-Gallent, Elena; Marcandalli, Giulia; Figueiredo, Marta Costa Journal of the American Chemical Society, Vol. 139, Issue 45 https://doi.org/10.1021/jacs.7b10142	journal	November 2017
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
A density-functional model of the dispersion interaction Becke, Axel D.; Johnson, Erin R. The Journal of Chemical Physics, Vol. 123, Issue 15 https://doi.org/10.1063/1.2065267	journal	October 2005
The evolution of CO adsorption on Cu(111) as studied with bare and CO-functionalized scanning tunneling tips Bartels, L.; Meyer, G.; Rieder, K. -H. Surface Science, Vol. 432, Issue 3 https://doi.org/10.1016/S0039-6028(99)00640-8	journal	July 1999
Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals Hammer, B.; Hansen, L. B.; Nørskov, J. K. Physical Review B, Vol. 59, Issue 11 https://doi.org/10.1103/PhysRevB.59.7413	journal	March 1999
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels Birdja, Yuvraj Y.; Pérez-Gallent, Elena; Figueiredo, Marta C. Nature Energy, Vol. 4, Issue 9 https://doi.org/10.1038/s41560-019-0450-y	journal	September 2019
A few basic concepts in electrochemical carbon dioxide reduction Chan, Karen Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19369-6	journal	November 2020
A direct optimization method for calculating density functionals and exchange–correlation potentials from electron densities Wu, Qin; Yang, Weitao The Journal of Chemical Physics, Vol. 118, Issue 6 https://doi.org/10.1063/1.1535422	journal	January 2003
Second-order perturbation theory with a CASSCF reference function Andersson, Kerstin.; Malmqvist, Per Aake.; Roos, Bjoern O. The Journal of Physical Chemistry, Vol. 94, Issue 14 https://doi.org/10.1021/j100377a012	journal	July 1990
Revisiting Understanding of Electrochemical CO₂ Reduction on Cu(111): Competing Proton-Coupled Electron Transfer Reaction Mechanisms Revealed by Embedded Correlated Wavefunction Theory Zhao, Qing; Martirez, John Mark P.; Carter, Emily A. Journal of the American Chemical Society, Vol. 143, Issue 16 https://doi.org/10.1021/jacs.1c00880	journal	April 2021
Dopant-induced electron localization drives CO2 reduction to C2 hydrocarbons Zhou, Yansong; Che, Fanglin; Liu, Min Nature Chemistry, Vol. 10, Issue 9 https://doi.org/10.1038/s41557-018-0092-x	journal	July 2018
Interactions of CO molecules adsorbed on Cu(111) Hollins, P.; Pritchard, J. Surface Science, Vol. 89, Issue 1-3 https://doi.org/10.1016/0039-6028(79)90633-2	journal	January 1979
Mechanistic Explanation of the pH Dependence and Onset Potentials for Hydrocarbon Products from Electrochemical Reduction of CO on Cu (111) Xiao, Hai; Cheng, Tao; Goddard, William A. Journal of the American Chemical Society, Vol. 138, Issue 2 https://doi.org/10.1021/jacs.5b11390	journal	January 2016
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces Kuhl, Kendra P.; Cave, Etosha R.; Abram, David N. Energy & Environmental Science, Vol. 5, Issue 5 https://doi.org/10.1039/c2ee21234j	journal	January 2012
A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes Schouten, K. J. P.; Kwon, Y.; van der Ham, C. J. M. Chemical Science, Vol. 2, Issue 10 https://doi.org/10.1039/c1sc00277e	journal	January 2011
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
Implementation of density functional embedding theory within the projector-augmented-wave method and applications to semiconductor defect states Yu, Kuang; Libisch, Florian; Carter, Emily A. The Journal of Chemical Physics, Vol. 143, Issue 10 https://doi.org/10.1063/1.4922260	journal	September 2015
Spectroscopic Observation of a Hydrogenated CO Dimer Intermediate During CO Reduction on Cu(100) Electrodes Pérez-Gallent, Elena; Figueiredo, Marta C.; Calle-Vallejo, Federico Angewandte Chemie International Edition, Vol. 56, Issue 13 https://doi.org/10.1002/anie.201700580	journal	February 2017
Catalysts and Reaction Pathways for the Electrochemical Reduction of Carbon Dioxide Kortlever, Ruud; Shen, Jing; Schouten, Klaas Jan P. The Journal of Physical Chemistry Letters, Vol. 6, Issue 20 https://doi.org/10.1021/acs.jpclett.5b01559	journal	September 2015
SBH10: A Benchmark Database of Barrier Heights on Transition Metal Surfaces Mallikarjun Sharada, Shaama; Bligaard, Thomas; Luntz, Alan C. The Journal of Physical Chemistry C, Vol. 121, Issue 36 https://doi.org/10.1021/acs.jpcc.7b05677	journal	September 2017
pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper Liu, Xinyan; Schlexer, Philomena; Xiao, Jianping Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07970-9	journal	January 2019

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30 DIRECT ENERGY CONVERSION
36 MATERIALS SCIENCE
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Title: Charting C–C coupling pathways in electrochemical CO 2 reduction on Cu(111) using embedded correlated wavefunction theory

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Title: Charting C–C coupling pathways in electrochemical CO ₂ reduction on Cu(111) using embedded correlated wavefunction theory