Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal-Organic Framework

Zitong Wang; Pierce Yeary; Yingjie Fan; Chenghua Deng; Wenbin Lin

doi:10.1021/acscatal.4c02326

Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO₂ Reduction by A Multifunctional Metal-Organic Framework

Zitong Wang
, Pierce Yeary
, Yingjie Fan
, Chenghua Deng
, Wenbin Lin

The University of Chicago

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

Abstract

We report a multifunctional metal-organic framework (MOF) photocatalyst for the CO₂ reduction reaction (CO₂RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO₂RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO₂RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO₂RR without significant loss of catalytic activity.

Original language	English
Pages (from-to)	9217-9223
Number of pages	7
Journal	ACS Catalysis
Volume	14
Issue number	12
DOIs	https://doi.org/10.1021/acscatal.4c02326
Publication status	Published - 21 Jun 2024
Externally published	Yes

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

Keywords

CO photoreduction
heterogeneous photocatalysis
metal−organic framework
site isolation
synergistic catalysis

Access to Document

10.1021/acscatal.4c02326

Cite this

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title = "Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal-Organic Framework",

abstract = "We report a multifunctional metal-organic framework (MOF) photocatalyst for the CO2 reduction reaction (CO2RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0\%). The short distance (6.6 {\AA}) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO2RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO2RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO2RR without significant loss of catalytic activity.",

keywords = "CO photoreduction, heterogeneous photocatalysis, metal−organic framework, site isolation, synergistic catalysis",

author = "Zitong Wang and Pierce Yeary and Yingjie Fan and Chenghua Deng and Wenbin Lin",

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T1 - Active Site Isolation and Enhanced Electron Transfer Facilitate Photocatalytic CO2 Reduction by A Multifunctional Metal-Organic Framework

AU - Wang, Zitong

AU - Yeary, Pierce

AU - Fan, Yingjie

AU - Deng, Chenghua

AU - Lin, Wenbin

PY - 2024/6/21

Y1 - 2024/6/21

N2 - We report a multifunctional metal-organic framework (MOF) photocatalyst for the CO2 reduction reaction (CO2RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO2RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO2RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO2RR without significant loss of catalytic activity.

AB - We report a multifunctional metal-organic framework (MOF) photocatalyst for the CO2 reduction reaction (CO2RR) under visible light irradiation with high efficiency (turnover number = 2638) and CO selectivity (97.0%). The short distance (6.6 Å) between bipyridine sites in the MOF allows the integration of Ir photosensitizers and Ni catalysts in proximity, thereby enhancing their electron transfer for photocatalytic CO2RR. Isolation of these metal centers by the MOF structure prevents their deactivation, leading to 54 times higher CO2RR activity than the homogeneous system and allowing for easy recovery for use in five consecutive cycles of photocatalytic CO2RR without significant loss of catalytic activity.

KW - CO photoreduction

KW - heterogeneous photocatalysis

KW - metal−organic framework

KW - site isolation

KW - synergistic catalysis

UR - https://www.scopus.com/pages/publications/85195266141

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M3 - Article

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