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

被引:24
作者
Wang, Zitong [1 ]
Yeary, Pierce [1 ]
Fan, Yingjie [1 ]
Deng, Chenghua [1 ]
Lin, Wenbin [1 ]
机构
[1] Univ Chicago, Dept Chem, Chicago, IL 60637 USA
关键词
metal-organic framework; heterogeneous photocatalysis; CO2; photoreduction; site isolation; synergistic catalysis; CONVERSION; CATALYSIS; CARBON; COMPLEXES; NODES;
D O I
10.1021/acscatal.4c02326
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 & Aring;) 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.
引用
收藏
页码:9217 / 9223
页数:7
相关论文
共 65 条
[31]   Metal-Organic Layers as Multifunctional Two-Dimensional Nanomaterials for Enhanced Photoredox Catalysis [J].
Lan, Guangxu ;
Quan, Yangjian ;
Wang, Maolin ;
Nash, Geoffrey T. ;
You, Eric ;
Song, Yang ;
Veroneau, Samuel S. ;
Jiang, Xiaomin ;
Lin, Wenbin .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2019, 141 (40) :15767-15772
[32]   Function-Integrated Ru Catalyst for Photochemical CO2 Reduction [J].
Lee, Sze Koon ;
Kondo, Mio ;
Okamura, Masaya ;
Enomoto, Takafumi ;
Nakamura, Go ;
Masaoka, Shigeyuki .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (49) :16899-16903
[33]   Metal-Organic-Framework-Based Catalysts for Photoreduction of CO2 [J].
Li, Rui ;
Zhang, Wang ;
Zhou, Kun .
ADVANCED MATERIALS, 2018, 30 (35)
[34]   Engineering Porphyrin Metal-Organic Framework Composites as Multifunctional Platforms for CO2 Adsorption and Activation [J].
Liu, Jiewei ;
Fan, Yan-Zhong ;
Zhang, Kun ;
Zhang, Li ;
Su, Cheng-Yong .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (34) :14548-14556
[35]   Applications of metal-organic frameworks in heterogeneous supramolecular catalysis [J].
Liu, Jiewei ;
Chen, Lianfen ;
Cui, Hao ;
Zhang, Jianyong ;
Zhang, Li ;
Su, Cheng-Yong .
CHEMICAL SOCIETY REVIEWS, 2014, 43 (16) :6011-6061
[36]   Single-layer electroluminescent devices and photoinduced hydrogen production from an ionic iridium(III) complex [J].
Lowry, MS ;
Goldsmith, JI ;
Slinker, JD ;
Rohl, R ;
Pascal, RA ;
Malliaras, GG ;
Bernhard, S .
CHEMISTRY OF MATERIALS, 2005, 17 (23) :5712-5719
[37]  
Mateo D, 2021, ADV FUNCT MATER, V31, DOI [10.1002/adfm.202170053, 10.1002/adfm.202008244]
[38]   Engineering Single-Atom Sites into Pore-Confined Nanospaces of Porphyrinic Metal-Organic Frameworks for the Highly Efficient Photocatalytic Hydrogen Evolution Reaction [J].
Mo, Qijie ;
Zhang, Li ;
Li, Sihong ;
Song, Haili ;
Fan, Yanan ;
Su, Cheng-Yong .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (49) :22747-22758
[39]   Anthropogenic Chemical Carbon Cycle for a Sustainable Future [J].
Olah, George A. ;
Prakash, G. K. Surya ;
Goeppert, Alain .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (33) :12881-12898
[40]   Isolated Fe Sites in Metal Organic Frameworks Catalyze the Direct Conversion of Methane to Methanol [J].
Osadchii, Dmitrii Y. ;
Olivos-Suarez, Alma I. ;
Szecsenyi, Agnes ;
Li, Guanna ;
Nasalevich, Maxim A. ;
Dugulan, Julian A. ;
Crespo, Pablo Serra ;
Hensen, Emiel J. M. ;
Veber, Sergey L. ;
Fedin, Matvey V. ;
Sankar, Gopinathan ;
Pidko, Evgeny A. ;
Gascon, Jorge .
ACS CATALYSIS, 2018, 8 (06) :5542-+