Bie Chuanbiao, Zhu Bicheng, Wang Linxi, Yu Huogen, Jiang Chenhui, Chen Tao, Yu Jiaguo
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, 430074, Wuhan, P. R. China.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, 430070, Wuhan, P. R. China.
Angew Chem Int Ed Engl. 2022 Nov 2;61(44):e202212045. doi: 10.1002/anie.202212045. Epub 2022 Oct 5.
The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst is constructed based on CdS/MoO /MoS hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS and MoO are simultaneously obtained from the conversion of CdMoO in one step. In a photocatalytic process, the MoS and MoO function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two-step single-electron route for PA production is proposed, initiated by the cleavage of the α-C(sp )-H bond in the LA. The conversion of LA and the selectivity of PA can reach ca. 29 % and 95 % after a five-hour reaction, respectively.
光生电子和空穴的最佳利用对于提高光催化活性至关重要。在此，基于CdS/MoO₃/MoS₂空心球构建了一种双功能双助催化剂修饰的光催化剂，用于析氢以及从乳酸（LA）氧化中选择性生产丙酮酸（PA）。MoS₂和MoO₃通过一步法将CdMoO₄转化同时获得。在光催化过程中，MoS₂和MoO₃分别作为还原和氧化中心，光生电子和空穴在其上积累并分别用于析氢反应（HER）和PA合成。通过监测中间体，提出了一条由LA中α-C(sp³)-H键裂解引发的PA生成的两步单电子途径。反应五小时后，LA的转化率和PA的选择性分别可达约29%和95%。
