Controlling the Polarity of Metal-Organic Frameworks to Promote Electrochemical CO<sub>2</sub> Reduction

doi:10.1002/anie.202416367

IMR OpenIR

	Controlling the Polarity of Metal-Organic Frameworks to Promote Electrochemical CO₂ Reduction
	Chen, Junnan 1,2; Wang, Guangming 1,2; Dong, Yingjun 1,2; Ji, Jiapeng 1,2; Li, Linbo 1,2; Xue, Ming 3; Zhang, Xiaolong 1,2; Cheng, Hui-Ming 1,2,4
通讯作者	Zhang, Xiaolong(hm.cheng@siat.ac.cn) ; Cheng, Hui-Ming()
	2024-11-11
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	8
摘要	The addition of polar functional groups to porous structures is an effective strategy for increasing the ability of metal-organic frameworks (MOFs) to capture CO2 by enhancing interactions between the dipoles of the polar functional groups and the quadrupoles of CO2. However, the potential of MOFs with polar functional groups to activate CO2 has not been investigated in the context of CO2 electrolysis. In this study, we report a mixed-ligand strategy to incorporate various functional groups in the MOFs. We found that substituents with strong polarity led to increased catalytic performance of electrochemical CO2 reduction for these polarized MOFs. Both experimental and theoretical evidence indicates that the presence of polar functional groups induces a charge redistribution in the micropores of MOFs. We have shown that higher electron densities of sp(2)-carbon atoms in benzimidazolate ligands reduces the energy barrier to generate *COOH, which is simultaneously controlled by the mass transfer of CO2. Our research offers an effective method of disrupting local electron neutrality in the pores of electrocatalysts/supports to activate CO2 under electrochemical conditions.
关键词	electrochemical CO2 reduction metal-organic frameworks mixed-ligand engineering polar functional groups CO2 activation
资助者	National Natural Science Foundation of China ; Shenzhen Science and Technology Innovation Bureau ; Talent Introduction Project of Chinese Academy of Sciences ; Cross Institute Joint Research Youth Team Project of SIAT
DOI	10.1002/anie.202416367
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; Shenzhen Science and Technology Innovation Bureau[KQTD2022110109364705] ; Shenzhen Science and Technology Innovation Bureau[ZDSYS20210706144000003] ; Talent Introduction Project of Chinese Academy of Sciences[E344011] ; Talent Introduction Project of Chinese Academy of Sciences[E2Z1521] ; Cross Institute Joint Research Youth Team Project of SIAT[E25427] ; [52201237]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001355149800001
出版者	WILEY-V C H VERLAG GMBH
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/191506
专题	中国科学院金属研究所
通讯作者	Zhang, Xiaolong; Cheng, Hui-Ming
作者单位	1.Chinese Acad Sci, Shenzhen Inst Adv Technol, Shenzhen Key Lab Energy Mat Carbon Neutral, Shenzhen 518055, Peoples R China 2.Shenzhen Univ Adv Technol, Fac Mat Sci & Energy Engn, Shenzhen 518055, Peoples R China 3.Sun Yat Sen Univ, Sch Chem Engn & Technol, Zhuhai 519082, Peoples R China 4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
推荐引用方式 GB/T 7714	Chen, Junnan,Wang, Guangming,Dong, Yingjun,et al. Controlling the Polarity of Metal-Organic Frameworks to Promote Electrochemical CO₂ Reduction[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024:8.
APA	Chen, Junnan.,Wang, Guangming.,Dong, Yingjun.,Ji, Jiapeng.,Li, Linbo.,...&Cheng, Hui-Ming.(2024).Controlling the Polarity of Metal-Organic Frameworks to Promote Electrochemical CO₂ Reduction.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,8.
MLA	Chen, Junnan,et al."Controlling the Polarity of Metal-Organic Frameworks to Promote Electrochemical CO₂ Reduction".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024):8.