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Atomic Structure Modification of Fe-N-C Catalysts via Morphology Engineering of Graphene for Enhanced Conversion Kinetics of Lithium-Sulfur Batteries

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Title
Atomic Structure Modification of Fe-N-C Catalysts via Morphology Engineering of Graphene for Enhanced Conversion Kinetics of Lithium-Sulfur Batteries
Author(s)
Jiheon Kim; Kim, Seong-Jun; Euiyeon Jung; Mok, Dong Hyeon; Paidi, Vinod K.; Jaewoo Lee; Hyeon Seok Lee; Yunseo Jeoun; Wonjae Ko; Heejong Shin; Byoung-Hoon Lee; Shin-Yeong Kim; Hyunjoong Kim; Ji Hwan Kim; Cho, Sung-Pyo; Lee, Kug-Seung; Back, Seoin; Yu, Seung-Ho; Yung-Eun Sung; Taeghwan Hyeon
Publication Date
2022-05
Journal
ADVANCED FUNCTIONAL MATERIALS, v.32, no.19
Publisher
WILEY-V C H VERLAG GMBH
Abstract
Single-atom M-N-C catalysts have attracted tremendous attention for their application to electrocatalysis. Nitrogen-coordinated mononuclear metal moieties (MNx moities) are bio-inspired active sites that are analogous to various metal-porphyrin cofactors. Given that the functions of metal-porphyrin cofactors are highly dependent on the local coordination environments around the mononuclear active site, engineering MNx active sites in heterogeneous M-N-C catalysts would provide an additional degree of freedom for boosting their electrocatalytic activity. This work presents a local coordination structure modification of FeN4 moieties via morphological engineering of graphene support. Introducing highly wrinkled structure in graphene matrix induces nonplanar distortion of FeN4 moieties, resulting in the modification of electronic structure of mononuclear Fe. Electrochemical analysis combined with first-principles calculations reveal that enhanced electrocatalytic lithium polysulfide conversion, especially the Li2S redox step, is attributed to the local structure modified FeN4 active sites, while increased specific surface area also contributes to improved performance at low C-rates. Owing to the synergistic combination of atomic-level modified FeN4 active sites and morphological advantage of graphene support, Fe-N-C catalysts with wrinkled graphene morphology show superior lithium-sulfur battery performance at both low and high C-rates (particularly 915.9 mAh g(-1) at 5 C) with promising cycling stability.
URI
https://pr.ibs.re.kr/handle/8788114/11957
DOI
10.1002/adfm.202110857
ISSN
1616-301X
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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