title: Oxide Defect Engineering Enables to Couple Solar Energy into Oxygen Activation.
abstract: Modern development of chemical manufacturing requires a substantial reduction in energy consumption and catalyst cost. Sunlight-driven chemical transformation by metal oxides holds great promise for this goal; however, it remains a grand challenge to efficiently couple solar energy into many catalytic reactions. Here we report that defect engineering on oxide catalyst can serve as a versatile approach to bridge light harvesting with surface reactions by ensuring species chemisorption. The chemisorption not only spatially enables the transfer of photoexcited electrons to reaction species, but also alters the form of active species to lower the photon energy requirement for reactions. In a proof of concept, oxygen molecules are activated into superoxide radicals on defect-rich tungsten oxide through visible-near-infrared illumination to trigger organic aerobic couplings of amines to corresponding imines. The excellent efficiency and durability for such a highly important process in chemical transformation can otherwise be virtually impossible to attain by counterpart materials.
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Ning
authors.initials: N
authors.lastname: Zhang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Xiyu
authors.initials: X
authors.lastname: Li
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Huacheng
authors.initials: H
authors.lastname: Ye
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Shuangming
authors.initials: S
authors.lastname: Chen
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Huanxin
authors.initials: H
authors.lastname: Ju
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Daobin
authors.initials: D
authors.lastname: Liu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Yue
authors.initials: Y
authors.lastname: Lin
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Wei
authors.initials: W
authors.lastname: Ye
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Chengming
authors.initials: C
authors.lastname: Wang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Qian
authors.initials: Q
authors.lastname: Xu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Junfa
authors.initials: J
authors.lastname: Zhu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Li
authors.initials: L
authors.lastname: Song
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Jun
authors.initials: J
authors.lastname: Jiang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), School of Chemistry and Materials Science, Hefei Science Center (CAS), and National Synchrotron Radiation Laboratory, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
authors.forename: Yujie
authors.initials: Y
authors.lastname: Xiong