Aligning Metal Coordination Sites in Metal-Organic Framework- Enabled Metallaphotoredox Catalysis

被引：3
作者：
Liu, Tianjiao [1 ,2 ]
Deng, Chaoyuan [1 ,2 ]
Meng, Di [2 ,3 ]
Zhang, Yufan [1 ,2 ]
Duan, Ran [1 ,2 ]
Ji, Hongwei [1 ,2 ]
Sheng, Hua [1 ,2 ]
Li, Jikun [2 ,3 ]
Chen, Chuncheng [1 ,2 ]
Zhao, Jincai [1 ,2 ]
Song, Wenjing [1 ,2 ]
机构：
[1] Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Key Lab Photochem, Beijing 100190, Peoples R China
[2] Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Inst Chem, CAS Res Educ Ctr Excellence Mol Sci, Key Lab Photochem, Beijing 100190, Peoples R China
来源：
ACS APPLIED MATERIALS & INTERFACES | 2023年 / 15卷 / 04期
基金：
中国国家自然科学基金;
关键词：
metal-organic frameworks; metallophotoredox catalysis; coordination environment; cross-coupling; artificial photosynthesis; CO2; REDUCTION;
D O I：
10.1021/acsami.2c18378
中图分类号：
TB3 [工程材料学];
学科分类号：
0805 ; 080502 ;
摘要：
Construction of catalytic metal centers, the key modules in artificial photosynthetic systems, lies at the heart to explore unpaved reactivity patterns powered by light. Here, we disclose that the amino (-NH2) and carboxylic (-COO) functionalities, aligned in various visible-light-harvesting metal- organic frameworks (MOFs) (NH2-UiO-66, (NH2)2-UiO-67, and NH2-MIL-125), provide N/O-ligated Ni featuring different configurations and valence states. Of note, these Ni centers, in situ formed or preimplanted, demonstrated coordination units' spatial arrangement-dependent activity in cross-coupling of aryl halides and various nucleophiles. Our work provides a novel approach to construct and to regulate metal center(s) by MOFs' skeleton defined coordination environments, highlighting exclusive potential in exploring the reactivity pattern of the hosted metals.
引用
收藏
页码：5139 / 5147
页数：9
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