Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis

Abstract Multiphase sulfur redox reactions with advanced homogeneous and heterogeneous electrochemical processes in lithium–sulfur (Li–S) batteries possess sluggish kinetics. The slow kinetics leads to significant capacity decay during charge/discharge processes. Therefore, electrocatalysts with ade...

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Main Authors: Menghao Cheng, Zhenyu Xing, Rui Yan, Zhenyang Zhao, Tian Ma, Mi Zhou, Xikui Liu, Shuang Li, Chong Cheng
Format: Article
Language:English
Published: Wiley 2023-04-01
Series:InfoMat
Subjects:
Online Access:https://doi.org/10.1002/inf2.12387
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author Menghao Cheng
Zhenyu Xing
Rui Yan
Zhenyang Zhao
Tian Ma
Mi Zhou
Xikui Liu
Shuang Li
Chong Cheng
author_facet Menghao Cheng
Zhenyu Xing
Rui Yan
Zhenyang Zhao
Tian Ma
Mi Zhou
Xikui Liu
Shuang Li
Chong Cheng
author_sort Menghao Cheng
collection DOAJ
description Abstract Multiphase sulfur redox reactions with advanced homogeneous and heterogeneous electrochemical processes in lithium–sulfur (Li–S) batteries possess sluggish kinetics. The slow kinetics leads to significant capacity decay during charge/discharge processes. Therefore, electrocatalysts with adequate sulfur‐redox properties are required to accelerate reversible polysulfide conversion in cathodes. In this study, we have fabricated an oxygen‐modulated metal nitride cluster (C‐MoNx‐O) that has a moderate binding ability to the insoluble Li2Sx for reversible polysulfide electrocatalysis. A Li–S battery equipped with C‐MoNx‐O electrocatalyst displayed a high discharge capacity of 875 mAh g−1 at 0.5 C. The capacity decay rate of each cycle was only 0.10% after 280 cycles, which is much lower than the control groups (C‐MoOx: 0.16%; C‐MoNx: 0.21%). Kinetic studies and theoretical calculations suggest that C‐MoNx‐O electrocatalyst presents a moderate binding ability to the insoluble Li2S2 and Li2S when compared to the C‐MoOx and C‐MoNx surfaces. Thus, the C‐MoNx‐O can effectively immobilize and reversibly catalyze the solid–solid conversion of Li2S2–Li2S during charge–discharge cycling, thus promoting reaction kinetics and eliminating the shuttle effect. This study to design oxygen‐doped metal nitrides provides innovative structures and reversible solid–solid conversions to overcome the sluggish redox chemistry of polysulfides.
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spelling doaj.art-a7ac1960b41e440b8e048c8ff7931bf32023-04-27T11:44:19ZengWileyInfoMat2567-31652023-04-0154n/an/a10.1002/inf2.12387Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysisMenghao Cheng0Zhenyu Xing1Rui Yan2Zhenyang Zhao3Tian Ma4Mi Zhou5Xikui Liu6Shuang Li7Chong Cheng8College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Biomass Science and Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu the People's Republic of ChinaAbstract Multiphase sulfur redox reactions with advanced homogeneous and heterogeneous electrochemical processes in lithium–sulfur (Li–S) batteries possess sluggish kinetics. The slow kinetics leads to significant capacity decay during charge/discharge processes. Therefore, electrocatalysts with adequate sulfur‐redox properties are required to accelerate reversible polysulfide conversion in cathodes. In this study, we have fabricated an oxygen‐modulated metal nitride cluster (C‐MoNx‐O) that has a moderate binding ability to the insoluble Li2Sx for reversible polysulfide electrocatalysis. A Li–S battery equipped with C‐MoNx‐O electrocatalyst displayed a high discharge capacity of 875 mAh g−1 at 0.5 C. The capacity decay rate of each cycle was only 0.10% after 280 cycles, which is much lower than the control groups (C‐MoOx: 0.16%; C‐MoNx: 0.21%). Kinetic studies and theoretical calculations suggest that C‐MoNx‐O electrocatalyst presents a moderate binding ability to the insoluble Li2S2 and Li2S when compared to the C‐MoOx and C‐MoNx surfaces. Thus, the C‐MoNx‐O can effectively immobilize and reversibly catalyze the solid–solid conversion of Li2S2–Li2S during charge–discharge cycling, thus promoting reaction kinetics and eliminating the shuttle effect. This study to design oxygen‐doped metal nitrides provides innovative structures and reversible solid–solid conversions to overcome the sluggish redox chemistry of polysulfides.https://doi.org/10.1002/inf2.12387electrocatalystslithium–sulfur batteriesmetal nitridereversible polysulfide catalysisshuttle effects
spellingShingle Menghao Cheng
Zhenyu Xing
Rui Yan
Zhenyang Zhao
Tian Ma
Mi Zhou
Xikui Liu
Shuang Li
Chong Cheng
Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
InfoMat
electrocatalysts
lithium–sulfur batteries
metal nitride
reversible polysulfide catalysis
shuttle effects
title Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
title_full Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
title_fullStr Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
title_full_unstemmed Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
title_short Oxygen‐modulated metal nitride clusters with moderate binding ability to insoluble Li2Sx for reversible polysulfide electrocatalysis
title_sort oxygen modulated metal nitride clusters with moderate binding ability to insoluble li2sx for reversible polysulfide electrocatalysis
topic electrocatalysts
lithium–sulfur batteries
metal nitride
reversible polysulfide catalysis
shuttle effects
url https://doi.org/10.1002/inf2.12387
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