文献类型：期刊文献

英文题名：Site-defined Cu-O ensembles enable hydrogen-conserving light-driven ethane upgrading

作者：Zhang, Qingqing[1,2,3];Liu, Cong[1,2];Xu, Chang[1,2,3];Huang, Dingnan[1,2,3];Xie, Cheng[4,5];Wang, Zhandong[4,5];Cao, Xiao-Ming[1,2,6];Zhang, Jinlong[1,3];Lei, Juying[3];Ye, Ziwei[1,2,3];Wang, Lingzhi[1,2,3]

机构：[1]East China Univ Sci & Technol, Inst Fine Chem,State Key Lab Green Chem Engn & Ind, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Inst Fine Chem,Joint Int Res Lab Precis Chem & Mol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn,State Key Lab Green Chem Engn, Shanghai, Peoples R China;[3]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Shanghai, Peoples R China;[4]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei, Peoples R China;[5]Univ Sci & Technol China, State Key Lab Fire Sci, Hefei, Peoples R China;[6]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Synergist Chem Bio Synth, Shanghai, Peoples R China

年份：2026

卷号：17

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001746723500003)】；

基金：This work was supported by National Key R&D Program of China (2023YFA1507601 to X.-M.C.), National Natural Science Foundation of China (22472056 to L.W. and 22461142136 to J.Z.), the Science and Technology Commission of Shanghai Municipality (24ZR1491000 to L.W.), and the Fundamental Research Funds for the Central Universities (222201717003 to J.Z.). The authors thank Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

摘要：Upgrading light alkanes to value-added olefins is a long-standing challenge, owing to the high stability of C-H bonds and the tendency for overoxidation at elevated temperatures. Here, we introduce a light-driven strategy for ethane dehydrogenation using Cu-doped TiO2, in which atomically dispersed Cu coordinated to bridging oxygen (Obr-Cu) creates well-defined [Cu-O] ensembles that orchestrate site-specific, stepwise C-H activation. Photogenerated holes localize at Obr-Cu sites to initiate the first C-H cleavage, while adjacent Cu centers mediate beta-H elimination and H2 evolution. In contrast, minor beta-H activation at Obr-Ti sites generates *H species that cannot desorb due to a prohibitive coupling barrier with *H on Obr-Cu, leading to Cu reduction and progressive deactivation. Co-feeding CO2 restores the active Cu coordination environment and suppresses this deactivation process without perturbing the primary reaction pathway. This cooperative design achieves a C2H4 production rate of 21.1 mmol g-1 h-1 with nearly stoichiometric H2 evolution and an apparent quantum efficiency of 6.1% under 365 nm irradiation. These findings establish a site-defined, hydrogen-conserving route for photocatalytic alkane upgrading, offering a general blueprint for selective C-H bond transformations with long-term stability.