Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries

The electrochemical performance of lithium–sulfur batteries (LiSBs) has been hampered by the slow redox kinetics and shuttle effect of lithium polysulfides (LiPSs), which require the rational design and synthesis of highly active electrocatalysts towards this reaction. Herein, worm-like N-doped poro...

Full description

Bibliographic Details
Main Authors: Qi Tan, Hongliang Liu, Guozhu Liang, Kaigui Jiang, Hangxuan Xie, Weijie Si, Jiajv Lin, Xiongwu Kang
Format: Article
Language:English
Published: MDPI AG 2023-07-01
Series:Inorganics
Subjects:
Online Access:https://www.mdpi.com/2304-6740/11/7/305
_version_ 1797588913407131648
author Qi Tan
Hongliang Liu
Guozhu Liang
Kaigui Jiang
Hangxuan Xie
Weijie Si
Jiajv Lin
Xiongwu Kang
author_facet Qi Tan
Hongliang Liu
Guozhu Liang
Kaigui Jiang
Hangxuan Xie
Weijie Si
Jiajv Lin
Xiongwu Kang
author_sort Qi Tan
collection DOAJ
description The electrochemical performance of lithium–sulfur batteries (LiSBs) has been hampered by the slow redox kinetics and shuttle effect of lithium polysulfides (LiPSs), which require the rational design and synthesis of highly active electrocatalysts towards this reaction. Herein, worm-like N-doped porous carbon nanotube-supported low-crystalline Co nanoparticles (a-Co-NC@C) were derived from binary Zn–Co ZIF via a two-step thermal annealing method. Initial thermal annealing 950 °C in Ar + H<sub>2</sub> atmosphere results in the carbonization of binary Zn–Co ZIF and the formation of high crystalline Co nanoparticles. Thermal annealing in ammonia atmosphere at 350 °C not only results in the reduced crystallinity of cobalt nanoparticles; it also promotes the growth of highly graphitized and heavily N-doped intertwined carbon nanotubes. The enlarged porous carbon nanotube structure offers accommodation for sulfur content, while the doped carbon and Co nanoparticles with reduced crystallinity facilitate the redox kinetics of LiPSs, improving the cycling stability, rate performance and capacity of LiSBs batteries. As a result, the a-Co-NC@C cathode displays a specific capacity of 559 mAh g<sup>−1</sup> after 500 cycles at 1 C, and a specific capacity of 572 mAh g<sup>−1</sup> at 3 C. It delivers a specific capacity of 579 mAh g<sup>−1</sup> at high sulfur loading of a 2.55 mg cm<sup>−2</sup> at 1 C after 400 cycles. This work highlights the importance of phase engineering of carbon matrix and transition metal nanoparticles in electrochemical performance of Li-S batteries.
first_indexed 2024-03-11T00:58:47Z
format Article
id doaj.art-81c121e3210743bcbbe317a956f622b7
institution Directory Open Access Journal
issn 2304-6740
language English
last_indexed 2024-03-11T00:58:47Z
publishDate 2023-07-01
publisher MDPI AG
record_format Article
series Inorganics
spelling doaj.art-81c121e3210743bcbbe317a956f622b72023-11-18T19:48:14ZengMDPI AGInorganics2304-67402023-07-0111730510.3390/inorganics11070305Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur BatteriesQi Tan0Hongliang Liu1Guozhu Liang2Kaigui Jiang3Hangxuan Xie4Weijie Si5Jiajv Lin6Xiongwu Kang7Guangdong Electric Power Development Co., Ltd., Guangzhou 510080, ChinaGuangdong Zhuhai Jinwan Power Co., Ltd., Zhuhai 519000, ChinaGuangdong Zhuhai Jinwan Power Co., Ltd., Zhuhai 519000, ChinaGuangdong Zhuhai Jinwan Power Co., Ltd., Zhuhai 519000, ChinaChina Southern Power Grid Technology Co., Ltd., Guangzhou 510080, ChinaNew Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaNew Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaNew Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou 510006, ChinaThe electrochemical performance of lithium–sulfur batteries (LiSBs) has been hampered by the slow redox kinetics and shuttle effect of lithium polysulfides (LiPSs), which require the rational design and synthesis of highly active electrocatalysts towards this reaction. Herein, worm-like N-doped porous carbon nanotube-supported low-crystalline Co nanoparticles (a-Co-NC@C) were derived from binary Zn–Co ZIF via a two-step thermal annealing method. Initial thermal annealing 950 °C in Ar + H<sub>2</sub> atmosphere results in the carbonization of binary Zn–Co ZIF and the formation of high crystalline Co nanoparticles. Thermal annealing in ammonia atmosphere at 350 °C not only results in the reduced crystallinity of cobalt nanoparticles; it also promotes the growth of highly graphitized and heavily N-doped intertwined carbon nanotubes. The enlarged porous carbon nanotube structure offers accommodation for sulfur content, while the doped carbon and Co nanoparticles with reduced crystallinity facilitate the redox kinetics of LiPSs, improving the cycling stability, rate performance and capacity of LiSBs batteries. As a result, the a-Co-NC@C cathode displays a specific capacity of 559 mAh g<sup>−1</sup> after 500 cycles at 1 C, and a specific capacity of 572 mAh g<sup>−1</sup> at 3 C. It delivers a specific capacity of 579 mAh g<sup>−1</sup> at high sulfur loading of a 2.55 mg cm<sup>−2</sup> at 1 C after 400 cycles. This work highlights the importance of phase engineering of carbon matrix and transition metal nanoparticles in electrochemical performance of Li-S batteries.https://www.mdpi.com/2304-6740/11/7/305porous carbon nanotubelow crystallinecobalt nanoparticlespromoted redox kineticsLi–S batteries
spellingShingle Qi Tan
Hongliang Liu
Guozhu Liang
Kaigui Jiang
Hangxuan Xie
Weijie Si
Jiajv Lin
Xiongwu Kang
Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
Inorganics
porous carbon nanotube
low crystalline
cobalt nanoparticles
promoted redox kinetics
Li–S batteries
title Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
title_full Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
title_fullStr Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
title_full_unstemmed Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
title_short Two Birds with One Stone: Ammonium-Induced Carbon Nanotube Structure and Low-Crystalline Cobalt Nanoparticles Enabling High Performance of Lithium-Sulfur Batteries
title_sort two birds with one stone ammonium induced carbon nanotube structure and low crystalline cobalt nanoparticles enabling high performance of lithium sulfur batteries
topic porous carbon nanotube
low crystalline
cobalt nanoparticles
promoted redox kinetics
Li–S batteries
url https://www.mdpi.com/2304-6740/11/7/305
work_keys_str_mv AT qitan twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT hongliangliu twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT guozhuliang twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT kaiguijiang twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT hangxuanxie twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT weijiesi twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT jiajvlin twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries
AT xiongwukang twobirdswithonestoneammoniuminducedcarbonnanotubestructureandlowcrystallinecobaltnanoparticlesenablinghighperformanceoflithiumsulfurbatteries