4.8 Article

Photoelectrochemical CO2 Reduction toward Multicarbon Products with Silicon Nanowire Photocathodes Interfaced with Copper Nanoparticles

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 18, Pages 8002-8006

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c03702

Keywords

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Funding

  1. Liquid Sunlight Alliance
  2. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub [DE-SC0021266]
  3. NIH [S10OD024998]
  4. Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
  5. Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
  6. Microanalytical Facility, College of Chemistry, University of California, Berkeley

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The integration of silicon nanowire photocathodes with copper nanoparticle ensemble enables efficient photoelectrochemical CO2 conversion to multicarbon products. This system achieves CO2-to-C2H4 conversion with high selectivity and stability.
The development of photoelectrochemical systems for converting CO2 into chemical feedstocks offers an attractive strategy for clean energy storage by directly utilizing solar energy, but selectivity and stability for these systems have thus been limited. Here, we interface silicon nanowire (SiNW) photocathodes with a copper nanoparticle (CuNP) ensemble to drive efficient photoelectrochemical CO2 conversion to multicarbon products. This integrated system enables CO2-to-C2H4 conversion with faradaic efficiency approaching 25% and partial current densities above 2.5 mA/cm(2) at -0.50 V vs RHE, while the nanowire photocathodes deliver 350 mV of photovoltage under 1 sun illumination. Under 50 h of continual bias and illumination, CuNP/SiNW can sustain stable photoelectrochemical CO2 reduction. These results demonstrate the nanowire/catalyst system as a powerful modular platform to achieve stable photoelectrochemical CO2 reduction and the feasibility to facilitate complex reactions toward multicarbons using generated photocarriers.

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