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Adenine Derivative Host with Interlaced 2D Structure and Dual Lithiophilic–Sulfiphilic Sites to Enable High-Loading Li–S Batteries

  • Qingping Wu
    Qingping Wu
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    More by Qingping Wu
  • Xuejun Zhou
    Xuejun Zhou
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    More by Xuejun Zhou
  • Jun Xu*
    Jun Xu
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    *E-mail: [email protected]
    More by Jun Xu
  • Fahai Cao
    Fahai Cao
    State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
    More by Fahai Cao
  • , and 
  • Chilin Li*
    Chilin Li
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 585 He Shuo Road, Shanghai 201899, China
    *E-mail: [email protected]
    More by Chilin Li
Cite this: ACS Nano 2019, 13, 8, 9520–9532
Publication Date (Web):July 29, 2019
https://doi.org/10.1021/acsnano.9b04519
Copyright © 2019 American Chemical Society
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Abstract

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How to simultaneously restrain the loss of active species and facilitate the conversion reaction under high S loading condition is the key to solve the commercialization of Li–S batteries. For this system, the availability of raw materials and simplicity (high efficiency) of synthetic strategies are also important factors. Herein, we propose an interlaced two-dimensional (2D) carbon material as advanced Li–S cathode host characterized by corrugated monolithic morphology and Co/N dopants as dual lithiophilic–sulfiphilic sites. This 2D structure is derived from a cheap biomass precursor, adenine, with bonding interaction with a MgCl2 hydrate template via a facile ionothermal method. It allows a homogeneous spatial distribution of S/Li2S deposits and strong adsorbability and enhanced conversion kinetics for polysulfides. Benefiting from the synergistic effects of corrugated 2D conductive matrix and embedded heteroatom/nanodot catalyst, the resultant sulfur cathode releases a high specific capacity of 1290.4 mA h g–1 at 0.2 C, small capacity fading rate of 0.029% per cycle over 600 cycles at 2 C, superior rate performance up to 20 C, and considerable areal capacity retention of 6.0 mA h cm–2 even under an ultrahigh sulfur loading up to 9.7 mg cm–2.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.9b04519.

  • SEM of Co-CNCs and [email protected], TEM and HAADF-TEM of Co-CNCs, XRD of Co-CNCs and [email protected], Raman spectra of NCs and Co-CNCs, CV of NCs-based symmetric cell, Nyquist plots of NCs- and Co-CNCs-based symmetric cells, current response curve of Li2S nucleation and growth on NCs electrode, specific capacity and CE plots of blank Co-CNCs electrode, Nyquist plots of fresh and cycled [email protected] Li–S cells, SEM images of cycled [email protected] electrode and lithium anode, self-discharge voltage profiles for [email protected] electrode, voltage profiles of [email protected] and [email protected] electrodes at various rates (PDF)

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Cited By


This article is cited by 13 publications.

  1. Qingping Wu, Zhenguo Yao, Xuejun Zhou, Jun Xu, Fahai Cao, Chilin Li. Built-In Catalysis in Confined Nanoreactors for High-Loading Li–S Batteries. ACS Nano 2020, 14 (3) , 3365-3377. https://doi.org/10.1021/acsnano.9b09231
  2. Mengrui Wang, Xunfu Zhou, Xin Cai, Hongqiang Wang, Yueping Fang, Xinhua Zhong. Hierarchically porous, ultrathin N–doped carbon nanosheets embedded with highly dispersed cobalt nanoparticles as efficient sulfur host for stable lithium–sulfur batteries. Journal of Energy Chemistry 2020, 50 , 106-114. https://doi.org/10.1016/j.jechem.2020.03.014
  3. Jianchao Liu, Ruhong Li, Tianrui Chen, Chen Liu, Deying Mu, Shuting Sun, Weihua Wan, Zhen Wang, Junhua Wei, Changsong Dai. From bulk to porous: Structure transformation of nitrogen and phosphorous co-doped carbon material via sodium chloride assistance and its application in lithium-sulfur batteries. Journal of Alloys and Compounds 2020, 830 , 154638. https://doi.org/10.1016/j.jallcom.2020.154638
  4. Bangbei Zheng, Lihong Yu, Narui Li, Jingyu Xi. Efficiently immobilizing and converting polysulfide by a phosphorus doped carbon microtube textile interlayer for high-performance lithium-sulfur batteries. Electrochimica Acta 2020, 345 , 136186. https://doi.org/10.1016/j.electacta.2020.136186
  5. Rongrong Li, Hongjie Peng, Qingping Wu, Xuejun Zhou, Jiang He, Hangjia Shen, Minghui Yang, Chilin Li. Sandwich‐like Catalyst–Carbon–Catalyst Trilayer Structure as a Compact 2D Host for Highly Stable Lithium–Sulfur Batteries. Angewandte Chemie International Edition 2020, 121 https://doi.org/10.1002/anie.202004048
  6. Rongrong Li, Hongjie Peng, Qingping Wu, Xuejun Zhou, Jiang He, Hangjia Shen, Minghui Yang, Chilin Li. Sandwich‐like Catalyst–Carbon–Catalyst Trilayer Structure as a Compact 2D Host for Highly Stable Lithium–Sulfur Batteries. Angewandte Chemie 2020, 121 https://doi.org/10.1002/ange.202004048
  7. Fei Yin, Qi Jin, Hong Gao, XiTian Zhang, ZhiGuo Zhang. A strategy to achieve high loading and high energy density Li-S batteries. Journal of Energy Chemistry 2020, https://doi.org/10.1016/j.jechem.2020.05.014
  8. Milan Jana, Rui Xu, Xin-Bing Cheng, Jeong Seok Yeon, Jae Min Park, Jia-Qi Huang, Qiang Zhang, Ho Seok Park. Rational design of two-dimensional nanomaterials for lithium–sulfur batteries. Energy & Environmental Science 2020, 13 (4) , 1049-1075. https://doi.org/10.1039/C9EE02049G
  9. Zhengqing Ye, Ying Jiang, Tao Feng, Ziheng Wang, Li Li, Feng Wu, Renjie Chen. Curbing polysulfide shuttling by synergistic engineering layer composed of supported Sn4P3 nanodots electrocatalyst in lithium-sulfur batteries. Nano Energy 2020, 70 , 104532. https://doi.org/10.1016/j.nanoen.2020.104532
  10. Jinmeng Sun, Yuhang Liu, Hongfang Du, Song He, Lei Liu, Zhenqian Fu, Linghai Xie, Wei Ai, Wei Huang. Molecularly designed N, S co-doped carbon nanowalls decorated on graphene as a highly efficient sulfur reservoir for Li–S batteries: a supramolecular strategy. Journal of Materials Chemistry A 2020, 8 (11) , 5449-5457. https://doi.org/10.1039/C9TA13999K
  11. Jia Liu, Hong Yuan, Xinyong Tao, Yeru Liang, Seung Jae Yang, Jia‐Qi Huang, Tong‐Qi Yuan, Maria‐Magdalena Titirici, Qiang Zhang. Recent progress on biomass‐derived ecomaterials toward advanced rechargeable lithium batteries. EcoMat 2020, 2 (1) https://doi.org/10.1002/eom2.12019
  12. Yang Wang, Liping Zhou, Jingyun Huang, Xinyang Wang, Xinling Xu, Jianguo Lu, Yang Tian, Zhizhen Ye, Haichao Tang, Shuit‐Tong Lee, Yingying Lu. Highly Stable Lithium−Sulfur Batteries Promised by Siloxene: An Effective Cathode Material to Regulate the Adsorption and Conversion of Polysulfides. Advanced Functional Materials 2020, 30 (12) , 1910331. https://doi.org/10.1002/adfm.201910331
  13. Han Wu, Zhenguo Yao, Qingping Wu, Shengsheng Fan, Congling Yin, Chilin Li. Confinement effect and air tolerance of Li plating by lithiophilic poly(vinyl alcohol) coating for dendrite-free Li metal batteries. Journal of Materials Chemistry A 2019, 7 (39) , 22257-22264. https://doi.org/10.1039/C9TA09146G

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