Polyethyleneimine coated AgInS2 quantum dots for efficient CO2 photoreduction to C2H6

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Abstract

Quantum dots exhibit great potential in photocatalytic CO2 conversion into value-added fuels to achieve a carbon-neutral society, owing to their unique optical properties and tunable surface chemistry. However, the generation of multi-carbon hydrocarbon products remains a grand challenge. Herein, polyethyleneimine (PEI) coated AgInS2 quantum dots (AgInS2@PEI QDs) are designed for the photo-catalytic conversion of CO2 to C2 products. It is found that the yield and selectivity of C2H6 can be significantly enhanced by regulating the content of Ag and PEI in AgInS2@PEI QDs. Under the optimal conditions, C2H6 yield reaches 63 μmol g-1, and the electron selectivity is 30.3 %. A mechanistic study reveals that PEI effectively promotes the accumulation of photogenerated electrons, and the CO-enriched local environment caused by Ag boosts CC coupling on asymmetric bimetallic sites. This work offers new insight on the design of efficient quantum dot photocatalysts for CO2 conversion to C2 products.

Abstract Image

聚乙烯亚胺涂层 AgInS2 量子点用于高效 CO2 光还原为 C2H6
量子点因其独特的光学特性和可调表面化学性质,在光催化二氧化碳转化为高附加值燃料以实现碳中和社会方面展现出巨大潜力。然而,生成多碳碳氢化合物产品仍然是一个巨大的挑战。本文设计了聚乙烯亚胺(PEI)包覆的 AgInS2 量子点(AgInS2@PEI QDs),用于光催化将 CO2 转化为 C2 产物。研究发现,通过调节 AgInS2@PEI QDs 中 Ag 和 PEI 的含量,可以显著提高 C2H6 的产率和选择性。在最佳条件下,C2H6 产率达到 63 μmol g-1,电子选择性为 30.3%。机理研究表明,PEI 能有效地促进光生电子的积累,而 Ag 带来的富含 CO 的局部环境则促进了不对称双金属位点上的 CC 耦合。这项研究为设计将 CO2 转化为 C2 产物的高效量子点光催化剂提供了新的思路。
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