4.8 Article

Perovskite Photocatalytic CO2 Reduction or Photoredox Organic Transformation?

期刊

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202205572

关键词

CO Surrogate; CO2 Reduction; Perovskite; Photocatalytic Organic Reactions; Photoredox

资金

  1. NSF CAREER award
  2. Office of Science, Office of Basic Energy Sciences within the US Department of Energy
  3. DOE [DE-AC36-08GO28308]

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It has been found that metal-halide perovskites used as photocatalysts for CO2 reduction in organic solvents may face issues due to photoredox organic transformations involving the solvent, resulting in CO production rather than CO2 reduction products. The rate of CO generation in organic solvents can be orders of magnitude higher than typical CO2 reduction pathways.
Metal-halide perovskites have been explored as photocatalysts for CO2 reduction. We report that perovskite photocatalytic CO2 reduction in organic solvents is likely problematic. Instead, the detected products (i.e., CO) likely result from a photoredox organic transformation involving the solvent. Our observations have been validated using isotopic labeling experiments, band energy analysis, and new control experiments. We designed a typical perovskite photocatalytic setup in organic solvents that led to CO production of up to approximate to 1000 mu mol g(-1) h(-1). CO2 reduction in organic solvents must be studied with extra care because photoredox organic transformations can produce orders of magnitude higher rate of CO or CH4 than is typical for CO2 reduction routes. Though CO2 reduction is not likely to occur, in situ CO generation is extremely fast. Hence a suitable system can be established for challenging organic reactions that use CO as a feedstock but exploit the solvent as a CO surrogate.

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