期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 48, 页码 26437-26447出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c07553
关键词
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资金
- Joint Center for Artificial Photosynthesis (JCAP), a DOE Energy Innovation Hub - the Office of Science of the U.S. Department of Energy [DESC0004993]
- Liquid Sunlight Alliance (LiSA)
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub [DESC0021266]
- Office of Science of the U.S. Department of Energy [DE-AC0205CH11231]
- Knut and Alice Wallenberg Foundation [2019.0586]
- JCAP funding
The study investigates the competitive coupling mechanisms leading to C-3 products on Cu(100) and Cu(511) using density functional theory (DFT). It suggests that there are multiple possible pathways towards forming C-3 intermediates on different surfaces, with local field stabilization playing a pivotal role in certain coupling steps.
Challenges in improving catalysts for electrochemical CO2 reduction require a clear understanding of the reaction mechanisms that lead to products of higher value. In this work, we use density functional theory (DFT) to determine the most competitive coupling mechanisms leading to C-3 products on Cu(100) and Cu(511). We exhaustively consider surface coupling pathways between CO* and different C-2 intermediates. On Cu(100), CO* coupling with acetaldehyde was identified as a notable step for C-3 product formation. On Cu(511), local field stabilizations enable an additional coupling step between HCCH* and CO*. This suggests that there is more than one possible pathway toward forming C-3 intermediates. Our simulations show that much like C-2 formation, C-3 formation prefers stepped surfaces with (100)-like sites and that local field stabilization can play a pivotal role in certain coupling steps.
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