title: Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal-Organic Framework.
abstract: Modular optimization of metal-organic frameworks (MOFs) was realized by incorporation of coordinatively unsaturated single atoms in a MOF matrix. The newly developed MOF can selectively capture and photoreduce CO2with high efficiency under visible-light irradiation. Mechanistic investigation reveals that the presence of single Co atoms in the MOF can greatly boost the electron-hole separation efficiency in porphyrin units. Directional migration of photogenerated excitons from porphyrin to catalytic Co centers was witnessed, thereby achieving supply of long-lived electrons for the reduction of CO2molecules adsorbed on Co centers. As a direct result, porphyrin MOF comprising atomically dispersed catalytic centers exhibits significantly enhanced photocatalytic conversion of CO2, which is equivalent to a 3.13-fold improvement in CO evolution rate (200.6 μmol g-1h-1) and a 5.93-fold enhancement in CH4generation rate (36.67 μmol g-1h-1) compared to the parent MOF.
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Huabin
authors.initials: H
authors.lastname: Zhang
authors.affiliation: Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, P.R. China.
authors.forename: Jing
authors.initials: J
authors.lastname: Wei
authors.affiliation: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, P.R. China.
authors.forename: Juncai
authors.initials: J
authors.lastname: Dong
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Guigao
authors.initials: G
authors.lastname: Liu
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Li
authors.initials: L
authors.lastname: Shi
authors.affiliation: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, P.R. China.
authors.forename: Pengfei
authors.initials: P
authors.lastname: An
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Guixia
authors.initials: G
authors.lastname: Zhao
authors.affiliation: Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, P.R. China.
authors.forename: Jintao
authors.initials: J
authors.lastname: Kong
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Xiaojun
authors.initials: X
authors.lastname: Wang
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
authors.forename: Xianguang
authors.initials: X
authors.lastname: Meng
authors.affiliation: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, P.R. China.
authors.forename: Jing
authors.initials: J
authors.lastname: Zhang
authors.affiliation: International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan. Jinhua.YE@nims.go.jp.|TU-NIMS Joint Research Center, School of Material Science and Engineering, Tianjin University, Tianjin, 300072, P.R. China. Jinhua.YE@nims.go.jp.|Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, P.R. China. Jinhua.YE@nims.go.jp.
authors.forename: Jinhua
authors.initials: J
authors.lastname: Ye
keywords: CO2 reduction; active sites; heterogeneous catalysis; photocatalysis; solar-energy conversion