journal article·2020-06-03

Synergy between a Silver–Copper Surface Alloy Composition and Carbon Dioxide Adsorption and Activation

Yifan Ye, Jin Qian, Hao Yang, Hongyang Su, Kyung-Jae Lee, Ane Etxebarria, Tao Cheng, Hai Xiao, Junko Yano, William A. Goddard, Ethan J. Crumlin

ACS Applied Materials & Interfaces· Volume 12· Issue 22
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Abstract

Bimetallic electrocatalysts provide a promising strategy for improving performance, especially in the enhancement of selectivity of CO2 reduction reactions. However, the first step of CO2 activation on bimetallic materials remains obscure. Considering bimetallic silver–copper (AgCu) as an example, we coupled ambient pressure X-ray photoelectron spectroscopy (APXPS) and quantum mechanics (QM) to examine CO2 adsorption and activation on AgCu exposed to CO2 with and without H2O at 298 K. The interplay between adsorbed species and the surface alloy composition of Cu and Ag is studied in atomic details. The APXPS experiment and density functional theory (DFT) calculations indicate that the clean sample has a Ag-rich surface layer. Upon adsorption of CO2 and surface O, we found that it is thermodynamically more favorable to induce subsurface Cu atoms substitution for some surface Ag atoms, modifying the stability and activation of CO2-related chemisorbed species. We further characterized this substitution effect by correlating the new adsorption species with the observed binding energy (BE) shift and intensity change in APXPS.
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Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Catalytic Processes in Materials Science · nanoparticles nucleation surface interactions

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Joint Center for Artificial Photosynthesis, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Materials and Process Simulation Center, California Institute of Technology, Pasadena, California 91125, United States

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, Jiangsu 215123, China

Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China

Department of Physics and Photon Science, Gwangju Institute of Science and Technology (GIST), Gwangju 500-712, South Korea

Centre for Cooperative Research on Alternative Energies (CIC energiGUNE), Basque Research and Technology Alliance (BRTA), Alava Technology Park, Albert Einstein 48, Vitoria-Gasteiz 01510, Spain

Department of Condensed Matter Physics, Faculty of Science and Technology, University of the Basque Country, UPV/EHU, Apdo 644, Bilbao 48080, Spain

Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, California 91125, United States

Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Funding

Collaborative Innovation Center of Suzhou Nano Science and Technology · Soochow University · Basic Energy Sciences · China Postdoctoral Science Foundation · Government of Jiangsu Province · China Scholarship Council · National Natural Science Foundation of China · Priority Academic Program Development of Jiangsu Higher Education Institutions · Natural Science Foundation of Jiangsu Higher Education Institutions · Basque Government

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