A synergetic cocatalyst for conversion of carbon dioxide, sunlight, and water into methanol

• 成果类型: Article
• 署名作者: Ye, Zhengwei; Yang, Ke R.; Zhang, Bingxing; Navid, Ishtiaque Ahmed; Shen, Yifan; Xiao, Yixin; Pofelski, Alexandre; Botton, Gianluigi A.; Ma, Tao; Mondal, Shubham; Norris, Theodore B.; Batista, Victor S.; Mi, Zetian
• 署名单位: University of Michigan System; University of Michigan; Yale University; Yale University; McMaster University; University of Michigan System; University of Michigan
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-13674
• DOI: 10.1073/pnas.2408183121
• 发表日期: 2024-08-27
• 关键词: containing formate dehydrogenase; initio molecular-dynamics; total-energy calculations; co2 reduction; electrochemical reduction; photocatalytic reduction; electroreduction; oxide; tio2; hydrogenation

摘要

The conversion of CO2 into liquid fuels, using only sunlight and water, offers a promising path to carbon neutrality. An outstanding challenge is to achieve high efficiency and product selectivity. Here, we introduce a wireless photocatalytic architecture for conversion of CO2 and water into methanol and oxygen. The catalytic material consists of semiconducting nanowires decorated with core-shell nanoparticles, with a copper- rhodium core and a chromium oxide shell. The Rh/CrOOH interface provides a unidirectional channel for proton reduction, enabling hydrogen spillover at the core-shell interface. The vectorial transfer of protons, electrons, and hydrogen atoms allows for switching the mechanism of CO2 reduction from a proton- coupled electron transfer pathway in aqueous solution to hydrogenation of CO2 with a solar- to- methanol efficiency of 0.22%. The reported findings demonstrate a highly efficient, stable, and scalable wireless system for synthesis of methanol from CO2 that could provide a viable path toward carbon neutrality and environmental sustainability.