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Title: Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries

Abstract

The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni2P electrocatalyst supported on N, P co-doped graphene (Ni2P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni2P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li2S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni2P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm–2, the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.

Authors:
 [1];  [1];  [1];  [2];  [3];  [3];  [4];  [1];  [1]
+ Show Author Affiliations
  1. Taiyuan Univ. of Technology (China)
  2. North Univ. of China, Taiyuan (China)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Chinese Academy of Sciences, Taiyuan (China)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NSFC); Natural Science Foundation of Shanxi Province; USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1902349
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Engineering Journal
Additional Journal Information:
Journal Volume: 450; Journal Issue: Part 3; Journal ID: ISSN 1385-8947
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; modified separator; Lithium-sulfur batteries; chemical adsorption; phosphide; redox kinetics

Citation Formats

Zhao, Zhenxin, Duan, Yunrui, Chen, Feng, Tian, Zhen, Pathak, Rajesh, Elam, Jeffrey W., Yi, Zonglin, Wang, Yongzhen, and Wang, Xiaomin. Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries. United States: N. p., 2022. Web. doi:10.1016/j.cej.2022.138310.
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Zhao, Zhenxin, Duan, Yunrui, Chen, Feng, Tian, Zhen, Pathak, Rajesh, Elam, Jeffrey W., Yi, Zonglin, Wang, Yongzhen, & Wang, Xiaomin. Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries. United States. https://doi.org/10.1016/j.cej.2022.138310
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Zhao, Zhenxin, Duan, Yunrui, Chen, Feng, Tian, Zhen, Pathak, Rajesh, Elam, Jeffrey W., Yi, Zonglin, Wang, Yongzhen, and Wang, Xiaomin. Fri . "Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries". United States. https://doi.org/10.1016/j.cej.2022.138310. https://www.osti.gov/servlets/purl/1902349.
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@article{osti_1902349,
title = {Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries},
author = {Zhao, Zhenxin and Duan, Yunrui and Chen, Feng and Tian, Zhen and Pathak, Rajesh and Elam, Jeffrey W. and Yi, Zonglin and Wang, Yongzhen and Wang, Xiaomin},
abstractNote = {The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni2P electrocatalyst supported on N, P co-doped graphene (Ni2P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni2P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li2S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni2P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm–2, the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.},
doi = {10.1016/j.cej.2022.138310},
journal = {Chemical Engineering Journal},
number = Part 3,
volume = 450,
place = {United States},
year = {Fri Jul 29 00:00:00 EDT 2022},
month = {Fri Jul 29 00:00:00 EDT 2022}
}
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https://doi.org/10.1016/j.cej.2022.138310
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Works referenced in this record:

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Lithium-sulfur batteries poised for leap
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Black phosphorus supported Ni2P co-catalyst on graphitic carbon nitride enabling simultaneous boosting charge separation and surface reaction
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Surface-substituted Prussian blue analogue cathode for sustainable potassium-ion batteries
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