Hybrid materials consisting of semiconductors and cocatalysts have been widely used for photoelectrochemical (PEC) conversion of CO gas to value-added chemicals such as formic acid (HCOOH). To date, however, the rational design of catalytic architecture enabling the reduction of CO gas to chemical has remained a grand challenge. Here, we report a unique photocathode consisting of CuS-decorated GaN nanowires (NWs) integrated on planar silicon (Si) for the conversion of HS-containing CO mixture gas to HCOOH. It was discovered that HS impurity in the modeled industrial CO gas could lead to the spontaneous transformation of Cu to CuS NPs, which resulted in significantly increased faradaic efficiency of HCOOH generation. The CuS/GaN/Si photocathode exhibited superior faradaic efficiency of HCOOH = 70.2% and partial current density = 7.07 mA/cm at -1.0 V under AM1.5G 1 sun illumination. To our knowledge, this is the first demonstration that impurity mixed in the CO gas can enhance, rather than degrade, the performance of the PEC CO reduction reaction.
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http://dx.doi.org/10.1021/jacs.1c02139 | DOI Listing |
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