Soontornchaiyakul Wasusate, Yoshino Shunya, Kanazawa Tomoki, Haruki Rie, Fan Dongxiao, Nozawa Shunsuke, Yamaguchi Yuichi, Kudo Akihiko
Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo 162-8601, Japan.
Institute of Materials Structure Science, High Energy Accelerator Research Organization, Tsukuba, Ibaraki 305-0801, Japan.
J Am Chem Soc. 2023 Sep 20;145(37):20485-20491. doi: 10.1021/jacs.3c06413. Epub 2023 Aug 21.
CO reduction as an artificial photosynthetic system is a promising technology to produce green energies and chemicals because it uses light energy to convert HO and CO into valuable products such as CO, HCOOH, CHOH, CH, and preferably higher hydrocarbons. In photocatalytic reduction, water should be used as hydrogen and electron sources for CO reduction. Moreover, CH formation is an attractive and challenging topic because of the eight-electron-reducing product of CO. Herein, we report the development of a new Rh-Ru cocatalyst decorated on an alkaline earth-doped NaTaO surface for the photocatalytic CO reduction to form CH using water as an electron donor. CH was obtained by a photocatalytic "uphill" reaction of CO reduction using Rh-Ru cocatalyst-loaded NaTaO:Sr, water, and CO in an aqueous suspension system. About 10% of a selectivity (electronic efficiency) was obtained for CH formation under ambient conditions accompanied with O evolution of the oxidation product of HO.
作为一种人工光合系统，一氧化碳还原是一种很有前景的生产绿色能源和化学品的技术，因为它利用光能将水和一氧化碳转化为有价值的产品，如一氧化碳、甲酸、甲醇、甲烷，更理想的是转化为高级烃类。在光催化还原中，水应用作一氧化碳还原的氢和电子源。此外，由于一氧化碳的八电子还原产物，甲烷的形成是一个有吸引力且具有挑战性的课题。在此，我们报道了一种新的负载在碱土掺杂的钽酸钠表面的铑-钌助催化剂的开发，用于以水作为电子供体的光催化一氧化碳还原以形成甲烷。在水悬浮体系中，使用负载铑-钌助催化剂的钽酸钠锶、水和一氧化碳，通过光催化“上坡”一氧化碳还原反应获得了甲烷。在环境条件下，伴随着水氧化产物氧气的析出，甲烷形成的选择性（电子效率）约为10%。
