Constructing Bipolar Dual-Active Sites through High-Entropy-Induced Electric Dipole Transition for Decoupling Oxygen Redox

doi:10.1002/adma.202401018

IMR OpenIR

	Constructing Bipolar Dual-Active Sites through High-Entropy-Induced Electric Dipole Transition for Decoupling Oxygen Redox
	Zhang, Qi 1,2; Zheng, Zhiyang 1,2; Gao, Runhua 1,2; Xiao, Xiao 1,2; Jiao, Miaolun 1,2; Wang, Boran 1,2; Zhou, Guangmin 1,2; Cheng, Hui-Ming 3,4,5
通讯作者	Zhou, Guangmin(guangminzhou@sz.tsinghua.edu.cn) ; Cheng, Hui-Ming(hm.cheng@siat.ac.cn)
	2024-04-19
发表期刊	ADVANCED MATERIALS
ISSN	0935-9648
页码	11
摘要	It remains a significant challenge to construct active sites to break the trade-off between oxidation and reduction processes occurring in battery cathodes with conversion mechanism, especially for the oxygen reduction and evolution reactions (ORR/OER) involved in the zinc-air batteries (ZABs). Here, using a high-entropy-driven electric dipole transition strategy to activate and stabilize the tetrahedral sites is proposed, while enhancing the activity of octahedral sites through orbital hybridization in a FeCoNiMnCrO spinel oxide, thus constructing bipolar dual-active sites with high-low valence states, which can effectively decouple ORR/OER. The FeCoNiMnCrO high-entropy spinel oxide with severe lattice distortion, exhibits a strong 1s -> 4s electric dipole transition and intense t2g(Co)/eg(Ni)-2p(OL) orbital hybridization that regulates the electronic descriptors, eg and t2g, which leads to the formation of low-valence Co tetrahedral sites (Coth) and high-valence Ni octahedral sites (Nioh), resulting in a higher half-wave potential of 0.87 V on Coth sites and a lower overpotential of 0.26 V at 10 mA cm-2 on Nioh sites as well as a superior performance of ZABs compared to low/mild entropy spinel oxides. Therefore, entropy engineering presents a distinctive approach for designing catalytic sites by inducing novel electromagnetic properties in materials across various electrocatalytic reactions, particularly for decoupling systems. High-entropy FeCoNiMnCrO exhibits a higher half-wave potential of 0.87 V on Coth sites and a lower overpotential of 0.26 V at 10 mA cm-2 on Nioh sites compared to low/mild entropy spinel oxides, which is resulted from the low-valence Co tetrahedral sites and high-valence Ni octahedral sites generated by the severe lattice distortion. image
关键词	bifunctional electrocatalyst decoupling high-entropy lattice distortion
资助者	National Natural Science Foundation of China
DOI	10.1002/adma.202401018
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001205060500001
出版者	WILEY-V C H VERLAG GMBH
引用统计	被引频次：17[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/185619
专题	中国科学院金属研究所
通讯作者	Zhou, Guangmin; Cheng, Hui-Ming
作者单位	1.Tsinghua Univ, Shenzhen Geim Graphene Ctr, Tsinghua Berkeley Shenzhen Inst, Shenzhen 518055, Peoples R China 2.Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China 3.Shenzhen Inst Adv Technol, Fac Mat Sci & Energy Engn, Shenzhen 518055, Peoples R China 4.Chinese Acad Sci, Shenzhen Inst Adv Technol, Inst Technol Carbon Neutral, Shenzhen 518055, Peoples R China 5.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	Zhang, Qi,Zheng, Zhiyang,Gao, Runhua,et al. Constructing Bipolar Dual-Active Sites through High-Entropy-Induced Electric Dipole Transition for Decoupling Oxygen Redox[J]. ADVANCED MATERIALS,2024:11.
APA	Zhang, Qi.,Zheng, Zhiyang.,Gao, Runhua.,Xiao, Xiao.,Jiao, Miaolun.,...&Cheng, Hui-Ming.(2024).Constructing Bipolar Dual-Active Sites through High-Entropy-Induced Electric Dipole Transition for Decoupling Oxygen Redox.ADVANCED MATERIALS,11.
MLA	Zhang, Qi,et al."Constructing Bipolar Dual-Active Sites through High-Entropy-Induced Electric Dipole Transition for Decoupling Oxygen Redox".ADVANCED MATERIALS (2024):11.