期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 114, 期 40, 页码 10560-10565出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1711493114
关键词
heterogeneous catalysis; electrocatalysis; CO2 reduction; copper nanoparticles; in situ structural transformation
资金
- Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, & Biosciences Division, of the US Department of Energy [DE-AC02-05CH11231, FWP CH030201]
- Office of Science, Office of Basic Energy Sciences, of the US Department of Energy [DE-AC02-05CH11231]
- Microanalytical Facility, College of Chemistry, University of California, Berkeley
- Samsung
- Alexander von Humboldt Foundation
Direct conversion of carbon dioxide to multicarbon products remains as a grand challenge in electrochemical CO2 reduction. Various forms of oxidized copper have been demonstrated as electrocatalysts that still require large overpotentials. Here, we show that an ensemble of Cu nanoparticles (NPs) enables selective formation of C-2-C-3 products at low overpotentials. Densely packed Cu NP ensembles underwent structural transformation during electrolysis into electrocatalytically active cube-like particles intermixed with smaller nanoparticles. Ethylene, ethanol, and n-propanol are the major C-2-C-3 products with onset potential at -0.53 V (vs. reversible hydrogen electrode, RHE) and C-2-C-3 faradaic efficiency (FE) reaching 50% at only -0.75 V. Thus, the catalyst exhibits selective generation of C-2-C-3 hydrocarbons and oxygenates at considerably lowered overpotentials in neutral pH aqueous media. In addition, this approach suggests new opportunities in realizing multicarbon product formation from CO2, where the majority of efforts has been to use oxidized copper-based materials. Robust catalytic performance is demonstrated by 10 h of stable operation with C-2-C-3 current density 10 mA/cm(2) (at -0.75 V), rendering it attractive for solar-to-fuel applications. Tafel analysis suggests reductive CO coupling as a rate determining step for C-2 products, while n-propanol (C-3) production seems to have a discrete pathway.
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