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Optimizing the electronic spin state and delocalized electron of NiCo2(OH)(x)/MXene composite by interface engineering and plasma boosting oxygen evolution reaction

文献类型：期刊论文

作者Xu, Jingyao4; Zhong, Xia2,3; Wu, Xiaofeng4; Wang, Ying1; Feng, Shouhua4
刊名JOURNAL OF ENERGY CHEMISTRY
出版日期2022-08-01
卷号71页码:129-140
ISSN号2095-4956
关键词Transition metal compounds

Electronic state control of surface/interface

 Electron spin state Delocalized electron Electrocatalytic material
DOI10.1016/j.jechem.2022.03.025
通讯作者Wu, Xiaofeng(wuxf@jlu.edu.cn) ; Wang, Ying(ywang_2012@ciac.ac.cn) ; Feng, Shouhua(shfeng@jlu.edu.cn)
英文摘要The electrocatalytic activity of transition-metal-based compounds is closely related to the electronic configuration. However, optimizing the surface electron spin state of catalysts remains a challenge. Here, we developed a spin-state and delocalized electron regulation method to optimize oxygen evolution reaction (OER) performance by in-situ growth of NiCo2(OH)(x) using Oswald ripening and coordinating etching process on MXene and plasma treatment. X-ray absorption spectroscopy, magnetic tests and electron paramagnetic resonance reveal that the coupling of NiCo2(OH)(x) and MXene can induce remarkable spin-state transition of Co3+ and transition metal ions electron delocalization, plasma treatment further optimizes the 3d orbital structure and delocalized electron density. The unique Jahn-Teller phenomenon can be brought by the intermediate spin state (t(2g)(5)e(g)(1)) of Co3+, which benefits from the partial electron occupied eg orbitals. This distinct electron configuration (t(2g)(5)e(g)(1)) with unpaired electrons leads to orbital degeneracy, that the adsorption free energy of intermediate species and conductivity were further optimized. The optimized electrocatalyst exhibits excellent OER activity with an overpotential of 268 mV at 10 mA cm(-2). DFT calculations show that plasma treatment can effectively regulate the d-band center of TMs to optimize the adsorption and improve the OER activity. This approach could guide the rational design and discovery of electrocatalysts with ideal electron configurations in the future. (C)& nbsp;2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
资助项目National Natural Science Foundation of China[21801090] ; National Natural Science Foundation of China[21831003] ; National Natural Science Foundation of China[21621001] ; Jilin Scientific and Technological Development Program[20200802003GH] ; Scientific Research Project in the Education Department of Jilin Province[JJKH20211044KJ] ; Project on Experimental Technique of Jilin University[409020720202] ; Users with the Excellence Program of Hefei Science Center CAS[2020HSC-UE002]
WOS研究方向Chemistry ; Energy & Fuels ; Engineering
语种英语
出版者ELSEVIER
WOS记录号WOS:000793730300013
资助机构National Natural Science Foundation of China ; Jilin Scientific and Technological Development Program ; Scientific Research Project in the Education Department of Jilin Province ; Project on Experimental Technique of Jilin University ; Users with the Excellence Program of Hefei Science Center CAS
源URL[http://ir.imr.ac.cn/handle/321006/174122]  
专题金属研究所_中国科学院金属研究所
通讯作者Wu, Xiaofeng; Wang, Ying; Feng, Shouhua
作者单位1.Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Jilin, Peoples R China
2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Liaoning, Peoples R China
3.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
4.Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Jilin, Peoples R China
推荐引用方式
GB/T 7714		 Xu, Jingyao,Zhong, Xia,Wu, Xiaofeng,et al.

Optimizing the electronic spin state and delocalized electron of NiCo2(OH)(x)/MXene composite by interface engineering and plasma boosting oxygen evolution reaction

[J]. JOURNAL OF ENERGY CHEMISTRY,2022,71:129-140.
APA Xu, Jingyao,Zhong, Xia,Wu, Xiaofeng,Wang, Ying,&Feng, Shouhua.(2022).

Optimizing the electronic spin state and delocalized electron of NiCo2(OH)(x)/MXene composite by interface engineering and plasma boosting oxygen evolution reaction

.JOURNAL OF ENERGY CHEMISTRY,71,129-140.
MLA Xu, Jingyao,et al."

Optimizing the electronic spin state and delocalized electron of NiCo2(OH)(x)/MXene composite by interface engineering and plasma boosting oxygen evolution reaction

".JOURNAL OF ENERGY CHEMISTRY 71(2022):129-140.

入库方式： OAI收割

来源：金属研究所

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