Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal–Organic Framework

Huabin Zhang; Jing Wei; Juncai Dong; Guigao Liu; Li Shi; Pengfei An; Guixia Zhao; Jintao Kong; Xiaojun Wang; Xianguang Meng; Jing Zhang; Jinhua Ye

doi:10.1002/anie.201608597

Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal–Organic Framework

Huabin Zhang, Jing Wei, Juncai Dong, Guigao Liu, Li Shi, Pengfei An, Guixia Zhao, Jintao Kong, Xiaojun Wang, Xianguang Meng, Jing Zhang, Jinhua Ye

Research output: Contribution to journal › Article › peer-review

656 Scopus citations

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.

Original language	English (US)
Pages (from-to)	14310-14314
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	55
Issue number	46
DOIs	https://doi.org/10.1002/anie.201608597
State	Published - Nov 7 2016
Externally published	Yes

ASJC Scopus subject areas

General Chemistry
Catalysis

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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.",

author = "Huabin Zhang and Jing Wei and Juncai Dong and Guigao Liu and Li Shi and Pengfei An and Guixia Zhao and Jintao Kong and Xiaojun Wang and Xianguang Meng and Jing Zhang and Jinhua Ye",

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T1 - Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal–Organic Framework

AU - Zhang, Huabin

AU - Wei, Jing

AU - Dong, Juncai

AU - Liu, Guigao

AU - Shi, Li

AU - An, Pengfei

AU - Zhao, Guixia

AU - Kong, Jintao

AU - Wang, Xiaojun

AU - Meng, Xianguang

AU - Zhang, Jing

AU - Ye, Jinhua

N1 - Generated from Scopus record by KAUST IRTS on 2022-09-15

PY - 2016/11/7

Y1 - 2016/11/7

N2 - 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.

AB - 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.

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ER -

Efficient Visible-Light-Driven Carbon Dioxide Reduction by a Single-Atom Implanted Metal–Organic Framework

Abstract

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