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Inducing fe 3d electron delocalization and Spin‑State Transition of feN_(4) Species Boosts Oxygen Reduction Reaction for Wearable Zinc–Air Battery

引用

Nano-Micro Letters 2023年第4期15卷 23-39页

作者： Shengmei Chen Xiongyi Liang Sixia Hu Xinliang Li Guobin Zhang Shuyun Wang Longtao Ma Chi‑Man Lawrence Wu Chunyi Zhi Juan Antonio Zapien department of Materials Science and Engineering City University of Hong KongHong Kong 999077People’s Republic of China Sustech Core Research Facilities Southern University of Science and Technology1088 Xueyuan BlvdShenzhenGuangdong 518055People’s Republic of China Frontiers Science Center for Flexible electronics Institute of Flexible ElectronicsNorthwestern Polytechnical UniversityXi’an 710072People’s Republic of China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhenGuangdong518055People’s Republic of China

Transition metal-nitrogen-carbon materials(M-N-Cs),particularly fe-N-Cs,have been found to be electroactive for accelerating oxygen reduction reaction(ORR)*** substantial efforts have been devoted to design fe-N-Cs with increased active species content,surface area,and electronic conductivity,their performance is still far from ***,there is limited research about regulation on the electronic spin states of fe centers for fe-N-Cs electrocatalysts to improve their catalytic ***,we introduce Ti_(3)C_(2) MXene with sulfur terminals to regulate the electronic configuration of feN_(4) species and dramatically enhance catalytic activity toward *** MXene with sulfur terminals induce the spin-state transition of feN_(4) species and fe 3d electron delocalization with d band center upshift,enabling the fe(II)ions to bind oxygen in the end-on adsorption mode favorable to initiate the reduction of oxygen and boosting oxygen-containing groups adsorption on feN_(4) species and ORR *** resulting feN_(4)-Ti_(3)C_(2)Sx exhibits comparable catalytic performance to those of commercial *** developed wearable ZABs using feN_(4)-Ti_(3)C_(2)Sx also exhibit fast kinetics and excellent *** study confirms that regulation of the electronic structure of active species via coupling with their support can be a major contributor to enhance their catalytic activity.

关键词： fe 3d electron delocalization Spin-state transition Oxygen reduction reaction Wearable zinc-air batteries

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