Wang Chao, Li Xiyi, Ren Yifei, Jiao Haimiao, Wang Feng Ryan, Tang Junwang
Department of Chemical Engineering, University College London, London WC1E 7JE, U.K.
Industrial Catalysis Center, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
ACS Catal. 2023 Mar 2;13(6):3768-3774. doi: 10.1021/acscatal.2c06093. eCollection 2023 Mar 17.
Oxidation of methane into valuable chemicals, such as C molecules, has been long sought after but the dilemma between high yield and high selectivity of desired products remains. Herein, methane is upgraded through the photocatalytic oxidative coupling of methane (OCM) over a ternary Ag-AgBr/TiO catalyst in a pressurized flow reactor. The ethane yield of 35.4 μmol/h with a high C selectivity of 79% has been obtained under 6 bar pressure. These are much better than most of the previous benchmark performance in photocatalytic OCM processes. These results are attributed to the synergy between Ag and AgBr, where Ag serves as an electron acceptor and promotes the charge transfer and AgBr forms a heterostructure with TiO not only to facilitate charge separation but also to avoid the overoxidation process. This work thus demonstrates an efficient strategy for photocatalytic methane conversion by both the rational design of the catalyst for the high selectivity and reactor engineering for the high conversion.
将甲烷氧化为有价值的化学品,如碳分子,长期以来一直是人们所追求的,但所需产物的高收率和高选择性之间的两难问题仍然存在。在此,在加压流动反应器中,通过三元Ag-AgBr/TiO催化剂上的甲烷光催化氧化偶联(OCM)对甲烷进行升级。在6巴压力下,乙烷产率达到35.4 μmol/h,对碳的选择性高达79%。这些都比光催化OCM过程中以前的大多数基准性能要好得多。这些结果归因于Ag和AgBr之间的协同作用,其中Ag作为电子受体促进电荷转移,AgBr与TiO形成异质结构,不仅有助于电荷分离,还能避免过度氧化过程。因此,这项工作通过合理设计高选择性催化剂和高转化率的反应器工程,展示了一种光催化甲烷转化的有效策略。