Zhang Dayu School of Chemistry, Dalian University of Technology, Dalian 116024, Liaoning, P. R. China.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning P. R. China.
J Am Chem Soc. 2021 May 5;143(17):6533-6541. doi: 10.1021/jacs.1c00830. Epub 2021 Apr 27.
Photocatalytic biomass conversion represents an ideal way of generating syngas because of the sustainable use of biomass carbon and solar energy. However, the lack of efficient electron-proton transfer limits its efficiency. We here report an unprecedented method to simultaneously increase both the electron and proton transfer by creating surface sulfate ions on the CdS catalyst ([SO]/CdS). Surface sulfate ion [SO] is bifunctional, serving as the proton acceptor to promote proton transfer, and increasing the oxidation potential of the valence band to enhance electron transfer. [SO]/CdS produces a syngas mixture from glycerol without CO. Compared with pristine CdS, [SO]/CdS exhibits 9-fold higher CO generation rate (0.31 mmol g h) and 4-fold higher H generation (0.05 mmol g h). A wide range of sugars, such as glucose, fructose, maltose, sucrose, xylose, lactose, insulin, and starch, were facilely converted into syngas. This study reports the pivotal effect of surface sulfate ion on electron-proton transfer in photocatalysis and provides a facile method for increasing photocatalytic efficiency.
光催化生物质转化是一种生成合成气的理想方法,因为它可以可持续地利用生物质碳和太阳能。然而,电子-质子转移效率低限制了其应用。我们在此报告了一种前所未有的方法,即在 CdS 催化剂上通过创造表面硫酸根离子([SO])来同时增加电子和质子转移。表面硫酸根离子[SO]具有双重功能,既能作为质子受体促进质子转移,又能提高价带的氧化电位以增强电子转移。[SO]/CdS 可以从甘油中产生合成气混合物而无需 CO。与原始 CdS 相比,[SO]/CdS 的 CO 生成速率提高了 9 倍(0.31mmol g h),H 生成速率提高了 4 倍(0.05mmol g h)。葡萄糖、果糖、麦芽糖、蔗糖、木糖、乳糖、胰岛素和淀粉等多种糖都可以很容易地转化为合成气。本研究报告了表面硫酸根离子对光催化中电子-质子转移的关键作用,并提供了一种提高光催化效率的简便方法。