Regulating the Transfer of Photogenerated Carriers for Photocatalytic Hydrogen Evolution Coupled with Furfural Synthesis.

Liu, Boxin; Li, Yanfang; Guo, Yuchen; Tang, Yuan; Wang, Chunyang; Sun, Yan; Tan, Xin; Hu, Zhuofeng et al. · ACS Nano · 2024

basic_science · Level V

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Abstract

How to simultaneously utilize photogenerated electrons and holes still remains a critical challenge in the field of artificial photosynthesis, especially in the process of photocatalytic hydrogen (H<sub>2</sub>) evolution coupled with biomass oxidation to value-added chemicals. Herein, a series-parallel photocatalyst (Cu NPs/CdS/In<sub>2</sub>O<sub>3</sub>) that can intrinsically regulate the transfer of photogenerated carriers is ingeniously designed for photocatalytic H<sub>2</sub> evolution synergized with furfural alcohol (FFA) selective oxidation to furfural (FF). Accordingly, the desired H<sub>2</sub> and FF evolution rates with near 100% selectivity toward FF are achieved on Cu NPs/CdS/In<sub>2</sub>O<sub>3</sub> in a sealed atmospheric system. Experimental and theoretical analyses confirm that the localized surface plasmon resonance (LSPR) effect induced by Cu NPs accelerates the reduction of protons (H<sup>+</sup>) to H<sub>2</sub> efficiently, while the photogenerated holes from In<sub>2</sub>O<sub>3</sub> preferentially activate the α-C-H bond of FFA adsorbed on Lewis acid sites to generate FF. This work provides a reference for regulating the transfer of photogenerated carriers for H<sub>2</sub> evolution coupled with FF synthesis.