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Title: Manipulation of Edge‐Site Fe–N 2 Moiety on Holey Fe, N Codoped Graphene to Promote the Cycle Stability and Rate Capacity of Li–S Batteries

Journal Article · · Advanced Functional Materials
 [1];  [2];  [2];  [1];  [1];  [2];  [2]; ORCiD logo [1]
  1. Beijing Key Laboratory for Magnetoelectric Materials and Devices (BKL‐MEMD) Beijing Innovation Center for Engineering Science and Advanced Technology (BIC‐ESAT) Department of Materials Science and Engineering College of Engineering Peking University Beijing 100871 China
  2. Centre for Clean Environmental and Energy and School of Environment and Science Griffith University Gold Coast Queensland 4222 Australia

Abstract Graphene‐based materials have been widely studied to overcome the hurdles of Li–S batteries, but suffer from low adsorptivity to polar polysulfide species, slow mass transport of Li + ions, and severe irreversible agglomeration. Herein, via a one‐step scalable calcination process, a holey Fe, N codoped graphene (HFeNG) is successfully synthesized to address these problems. Diverging by the holey structures, the Fe atoms are anchored by four N atoms (Fe–N 4 moiety) or two N atoms (Fe–N 2 moiety) localized on the graphene sheets and edge of holes, respectively, which is confirmed by X‐ray absorption spectroscopy and density functional theory calculations. The unique holey structures not only promote the mass transport of lithium ions, but also prohibit the transportation of polysulfides across these additional channels via strong adsorption forces of Fe–N 2 moiety at the edges. The as‐obtained HFeNG delivers a high rate capacity of 810 mAh g −1 at 5 C and a stable cycling performance with the capacity decay of 0.083% per cycle at 0.5 C. The concept of holey structure and introduction of polar moieties could be extended to other carbon and 2D nanostructures for energy storage and conversion devices such as supercapacitors, alkali‐ion batteries, metal–air batteries, and metal–halogen batteries.

Sponsoring Organization:
USDOE
Grant/Contract Number:
DE‐AC02‐76SF00515
OSTI ID:
1485167
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Vol. 29 Journal Issue: 5; ISSN 1616-301X
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

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