Liu Boxin, Li Yanfang, Guo Yuchen, Tang Yuan, Wang Chunyang, Sun Yan, Tan Xin, Hu Zhuofeng, Yu Tao
School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, P. R. China.
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, P. R. China.
ACS Nano. 2024 Jul 9;18(27):17939-17949. doi: 10.1021/acsnano.4c04562. Epub 2024 Jun 25.
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) evolution coupled with biomass oxidation to value-added chemicals. Herein, a series-parallel photocatalyst (Cu NPs/CdS/InO) that can intrinsically regulate the transfer of photogenerated carriers is ingeniously designed for photocatalytic H evolution synergized with furfural alcohol (FFA) selective oxidation to furfural (FF). Accordingly, the desired H and FF evolution rates with near 100% selectivity toward FF are achieved on Cu NPs/CdS/InO 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) to H efficiently, while the photogenerated holes from InO 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 evolution coupled with FF synthesis.
如何同时利用光生电子和空穴在人工光合作用领域仍然是一个关键挑战，特别是在光催化析氢（H）与生物质氧化耦合生产增值化学品的过程中。在此，一种能够内在调节光生载流子转移的串并联光催化剂（Cu NPs/CdS/InO）被巧妙设计用于光催化析氢，并与糠醇（FFA）选择性氧化为糠醛（FF）协同作用。相应地，在密封大气系统中，在Cu NPs/CdS/InO上实现了所需的析氢和FF生成速率，对FF的选择性接近100%。实验和理论分析证实，Cu NPs诱导的局域表面等离子体共振（LSPR）效应有效地加速了质子（H）还原为H，而InO产生的光生空穴优先激活吸附在路易斯酸位点上的FFA的α-C-H键以生成FF。这项工作为调节光生载流子转移以实现析氢与FF合成的耦合提供了参考。
