Elucidating the mechanism of photocatalytic reduction of bicarbonate (aqueous CO2) into formate and other organics

Van Can Nguyen, Dipak B. Nimbalkar, Vu Hoang Huong, Yuh Lang Lee, Hsisheng Teng

研究成果: Article同行評審

3 引文 斯高帕斯(Scopus)

摘要

The photocatalytic reduction of CO2 under solar irradiation is an ideal approach to mitigating global warming, and reducing aqueous forms of CO2 that interact strongly with a catalyst (e.g., HCO3) is a promising strategy to expedite such reductions. This study uses Pt-deposited graphene oxide dots as a model photocatalyst to elucidate the mechanism of HCO3 reduction. The photocatalyst steadily catalyzes the reduction of an HCO3 solution (at pH = 9) containing an electron donor under 1-sun illumination over a period of 60 h to produce H2 and organic compounds (formate, methanol, and acetate). H2 is derived from solution-contained H2O, which undergoes photocatalytic cleavage to produce •H atoms. Isotopic analysis reveals that all of the organics formed via interactions between HCO3 and •H. This study proposes mechanistic steps, which are governed by the reacting behavior of the •H, to correlate the electron transfer steps and product formation of this photocatalysis. This photocatalysis achieves overall apparent quantum efficiency of 27% in the formation of reaction products under monochromatic irradiation at 420 nm. This study demonstrates the effectiveness of aqueous-phase photocatalysis in converting aqueous CO2 into valuable chemicals and the importance of H2O-derived •H in governing the product selectivity and formation kinetics.

原文English
頁(從 - 到)918-928
頁數11
期刊Journal of Colloid And Interface Science
649
DOIs
出版狀態Published - 2023 11月

All Science Journal Classification (ASJC) codes

  • 電子、光磁材料
  • 生物材料
  • 表面、塗料和薄膜
  • 膠體和表面化學

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