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Tuning the dual-active sites of ZIF-67 derived porous nanomaterials for boosting oxygen catalysis and rechargeable Zn-air batteries

查看全文 作  者:Zeyi [1]Zhang;Yangyang [1]Tan;Tang [1]Zeng;Liyue [1]Yu;Runzhe [1]Chen;Niancai [1]Cheng;Shichun [2]Mu;Xueliang [3]Sun 高影响力作者 机构地区:[1]College of Materials Science and Engineering,Fuzhou University,Fuzhou 350108,China;[2]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China;[3]Department of Mechanical and Materials Engineering,University of Western Ontario,London,ON N6A 5B9,Canada高影响力机构 出  处:《Nano Research》索引2021年第14卷第7期,共10页高影响力期刊 基  金:The authors acknowledge support from the National Natural Science Foundation of China(No.21875039);Minjiang Professorship(XRC-1677);Fujian province’s high level innovative and entrepreneurial talents(No.50012709);the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-201814),Fuzhou University. 摘  要:The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived nanomaterials.The formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) catalysts.The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in OER.The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability.This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices. 关 键 词:dual-active sites bifunctional oxygen electrocatalysts metal−organic frameworks Zn-air batteries density functional theory(DFT)
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