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CO2 Electroreduction with Enhanced Ethylene and Ethanol Selectivity by Nanostructuring Polycrystalline Copper

Journal Article · · ChemElectroChem
 [1];  [2];  [2];  [2];  [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
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There are a number of recent reports on the use of oxidation/reduction cycling of Cu surfaces to improve their selectivity for ethylene formation in the aqueous CO2 reduction reaction. Here, the oxidation/reduction process is examined in detail. It is found that the faradaic efficiencies for both ethylene and ethanol are enhanced after oxidation/reduction cycling in the presence of halide anions. Specifically, cycling of the electrode in the presence of chloride, bromide, or fluoride anions allows for an ethylene faradaic efficiency of approximately 15.2 %, a factor of 1.5 higher than that for polycrystalline copper (at -1.0 V vs. RHE). The faradaic efficiency for ethanol is also enha nced from 2.65 to approximately 7.6 %. The effects of electrochemical oxidation/reduction with the chloride anion were investigated by using in situ Raman spectroscopy, and the changes in the surface morphology of copper were monitored by using SEM. Consistent with prior reports, it is observed that during the oxidation part of the cycle, anodic corrosion forms a Cu2O layer, which consists of cubical crystals of about 150 nm. During the reduction sweep, it is converted to metallic copper, which forms irregular Cu nanoparticles of around 20 nm in diameter. The enhancement in ethylene formation is presumably attributed to the formation of grain boundaries, which may serve as active sites.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
DOE Contract Number:
AC02-05CH11231
OSTI ID:
1393048
Journal Information:
ChemElectroChem, Journal Name: ChemElectroChem Journal Issue: 6 Vol. 3; ISSN 2196-0216
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English

References (14)

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Sustainable hydrocarbon fuels by recycling CO 2 and H 2 O with renewable or nuclear energy journal January 2011

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY