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Engineering Fe‑N_(4)Electronic Structure with Adjacent Co‑N_(2)C_(2)and Co Nanoclusters on Carbon Nanotubes for Efficient Oxygen Electrocatalysis

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纳微快报:英文版 2023年第12期15卷 283-297页

作者： Mingjie Wu Xiaohua Yang Xun Cui Ning Chen Lei Du Mohamed Cherif Fu‑Kuo Chiang Yuren Wen amir hassanpour Francois Vidal Sasha Omanovic Yingkui Yang Shuhui Sun Gaixia Zhang State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhan 430200People’s Republic of China Institut National de la Recherche Scientifique(INRS) Center Energie Materiaux TelecommunicationsVarennesQC J3X 1P7Canada Department of Chemical Engineering McGill University3610 University StreetMontrealQC H3A 0C5Canada Department of Electrical Engineering Ecole de Technologie Superieure(ETS)MontrealQC H3C 1K3Canada Canadian Light Source(CLS) 44 Innovation BoulevardSaskatoonSK S7N 2V3Canada National Institute of Low-Carbon-and-Clean-Energy Beijing 102211People’s Republic of China School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China

Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement.Unlike the previously reported singleatom or dual-atom configurations,we designed a new type of binary-atom catalyst,through engineering Fe-N_(4)electronic structure with adjacent Co-N_(2)C_(2)and nitrogen-coordinated Co nanoclusters,as oxygen electrocatalysts.The resultant optimized electronic structure of the Fe-N_(4)active center favors the binding capability of intermediates and enhances oxygen reduction reaction(ORR)activity in both alkaline and acid conditions.In addition,anchoring M-N-C atomic sites on highly graphitized carbon supports guarantees of efficient charge-and mass-transports,and escorts the high bifunctional catalytic activity of the entire catalyst.Further,through the combination of electrochemical studies and in-situ X-ray absorption spectroscopy analyses,the ORR degradation mechanisms under highly oxidative conditions during oxygen evolution reaction processes were revealed.This work developed a new binary-atom catalyst and systematically investigates the effect of highly oxidative environments on ORR electrochemical behavior.It demonstrates the strategy for facilitating oxygen electrocatalytic activity and stability of the atomically dispersed M-N-C catalysts.

关键词： Atomically dispersed Fe-N-C catalysts ORR/OER Rechargeable zinc-air battery Fuel cells

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Biomass-derived nonprecious metal catalysts for oxygen reduction reaction: The demand-oriented engineering of active sites and structures

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Carbon Energy 2020年第4期2卷 561-581页

作者： Lei Du Gaixia Zhang Xianhu Liu amir hassanpour Marc Dubois Ana CTavares Shuhui Sun Center of Energy Materials and Telecommunications Institut National de la Recherche ScientifiqueVarennesQuebecCanada School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbinChina Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhouChina CNRS SIGMA ClermontInstitut de Chimie de Clermont-FerrandUniversitéClermont AuvergneClermont-FerrandFrance

Oxygen reduction reaction(ORR)is an important electrochemical process for renewable energy conversion and storage applications such as fuel cells and metal-air batteries.ORR is sluggish in kinetics and requires a large amount of platinum group metal(PGM)-based catalysts to facilitate its slow reaction rate.Application of precious metals raises the cost and decreases the competitivity of these devices in the market.To address this challenge,PGM-free ORR catalysts have been intensively investigated as an alternative to replace the PGM-based catalysts and to promote the deployment of ORR-related applications.In particular,the biomass holds promising potential to be used as the precursor material for PGM-free ORR catalysts.This pathway has gained more and more attention in recent years.In this review,recent advances regarding biomass-derived ORR catalysts are summarized with a focus on the rational design of both active sites and porous structures which are the two key factors in determining ORR performance of catalysts.At the end,the perspectives of development of biomass-derived catalysts is discussed.

关键词： active sites biomass oxygen reduction reaction porous structures

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