A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H<sub>2</sub>O<sub>2</sub> Electrosynthesis

doi:10.1002/anie.202408500

IMR OpenIR

	A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H₂O₂ Electrosynthesis
	Li, Zhenxin 1; Jia, Jingjing 1; Sang, Zhiyuan 1; Liu, Wei 1; Nie, Jiahuan 1; Yin, Lichang 2; Hou, Feng 1; Liu, Jiachen 1; Liang, Ji 1
通讯作者	Sang, Zhiyuan(sangzhiyuan@tju.edu.cn) ; Liang, Ji(liangji@tju.edu.cn)
	2024-10-08
发表期刊	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN	1433-7851
页码	10
摘要	Electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e(-)-ORR) provides an alternative method to the energy-intensive anthraquinone method. Metal macrocycles with precise coordination are widely used for 2e(-)-ORR electrocatalysis, but they have to be commonly loaded on conductive substrates, thus exposing a large number of 2e(-)-ORR-inactive sites that result in poor H2O2 production rate and efficiency. Herein, guided by first-principle predictions, a substrate-free and two-dimensional conductive metal-organic framework (Ni-TCPP(Co)), composed of CoN4 sites in porphine(Co) centers and Ni2O8 nodes, is designed as a multi-site catalyst for H2O2 electrosynthesis. The approperiate distance between the CoN4 and Ni2O8 sites in Ni-TCPP(Co) weakens the electron transfer between them, thus ensuring their inherent activities and creating high-density active sites. Meanwhile, the intrinsic electronic conductivity and porosity of Ni-TCPP(Co) further facilitate rapid reaction kinetics. Therefore, outstanding 2e(-)-ORR electrocatalytic performance has been achieved in both alkaline and neutral electrolytes (>90 %/85 % H2O2 selectivity within 0-0.8 V vs. RHE and >18.2/18.0 mol g(-1) h(-1) H2O2 yield under alkaline/neutral conditions), with confirmed feasibility for water purification and disinfection applications. This strategy thus provides a new avenue for designing catalysts with precise coordination and high-density active sites, promoting high-efficiency electrosynthesis of H2O2 and beyond.
关键词	conductive metal-organic frameworks multi-site catalysts two-electron oxygen reduction reaction hydrogen peroxide
资助者	National Natural Science Foundation of China
DOI	10.1002/anie.202408500
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China ; [22379111] ; [22179093]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001331233400001
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/321006/190588
专题	中国科学院金属研究所
通讯作者	Sang, Zhiyuan; Liang, Ji
作者单位	1.Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ, Tianjin 300072, Peoples R China 2.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	Li, Zhenxin,Jia, Jingjing,Sang, Zhiyuan,et al. A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H₂O₂ Electrosynthesis[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2024:10.
APA	Li, Zhenxin.,Jia, Jingjing.,Sang, Zhiyuan.,Liu, Wei.,Nie, Jiahuan.,...&Liang, Ji.(2024).A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H₂O₂ Electrosynthesis.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,10.
MLA	Li, Zhenxin,et al."A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal-Organic Framework for Efficient H₂O₂ Electrosynthesis".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024):10.