Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 27, Pages 10099-10107Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c02139
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Funding
- Basic Science Research Program through the NRF of Korea - Ministry of Education [2020R1I1A1A01069108]
- Korea Institute of Energy Technology Evaluation and Planning (KETEP) of the Republic of Korea [20172010106300]
- Ministry of Trade, Industry, and Energy (MOTIE) of the Republic of Korea [20172010106300]
- National Research Foundation of Korea (NRF) - Korea government (MSIT) [2019R1A2C1091158]
- Blue Sky program in the College of Engineering
- Korea Evaluation Institute of Industrial Technology (KEIT) [20172010106300] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2019R1A2C1091158, 2020R1I1A1A01069108] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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This study presents a unique photocathode for converting H2S-containing CO2 mixture gas to formic acid, where H2S impurity can enhance the performance of the PEC CO2 reduction reaction by facilitating the transformation of Cu to CuS NPs, resulting in improved faradaic efficiency of formic acid generation.
Hybrid materials consisting of semiconductors and cocatalysts have been widely used for photoelectrochemical (PEC) conversion of CO2 gas to value-added chemicals such as formic acid (HCOOH). To date, however, the rational design of catalytic architecture enabling the reduction of real CO2 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 H2S-containing CO2 mixture gas to HCOOH. It was discovered that H2S impurity in the modeled industrial CO2 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(2) at -1.0 V-RHE under AM1.5G 1 sun illumination. To our knowledge, this is the first demonstration that impurity mixed in the CO2 gas can enhance, rather than degrade, the performance of the PEC CO2 reduction reaction.
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