journal article·2019-06-05Open access

Sulfur in Mesoporous Tungsten Nitride Foam Blocks: A Rational Lithium Polysulfide Confinement Experimental Design Strategy Augmented by Theoretical Predictions

Zhen-Dong Huang, Yanwu Fang, Mingtong Yang, Jike Yang, Yizhou Wang, Zhen Wu, Qingchuan Du, Titus Masese, Ruiqing Liu, Xusheng Yang, Chenhui Qian, Shaowei Jin, Yanwen Ma

ACS Applied Materials & Interfaces· Volume 11· Issue 22

Abstract

To enhance the utilization of sulfur in lithium–sulfur batteries, three-dimensional tungsten nitride (WN) mesoporous foam blocks are designed to spatially localize the soluble Li2S6 and Li2S4 within the pore spaces. Meanwhile, the chemisorption behaviors of polysulfides and the capability of WN as an effective confiner are systematically investigated through density functional theory calculations and experimental studies. The theoretical calculations reveal a decrease in chemisorption strength between WN and the soluble polysulfides (Li2S8 > Li2S6 > Li2S4), while the interactions between WN and the insoluble Li2S2/Li2S show a high chemisorption strength of ca. 3 eV. Validating theoretical insights through electrochemical measurements further manifest that the assembled battery configurations with sulfur cathode confined in the thickest WN blocks exhibit the best rate capabilities (1090 and 510 mAh g–1 at 0.5C and 5C, respectively) with the highest initial Coulombic efficiency of 90.5%. Moreover, a reversible capacity of 358 mAh g–1 is maintained with a high Coulombic efficiency approaching to 100%, even after 500 cycles at 2C. As guided by in silico design, this work not only provides an effective strategy to improve the retentivity of polysulfides but also underpins that properly architectured WN can be effective retainers of polysulfides.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · MXene and MAX Phase Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Key Laboratory for Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing University of Posts and Telecommunications, 9 Wenyuan Road, Nanjing 210023, P. R. China

Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an 710049, P. R. China

Research Institute of Electrochemical Energy, National Institute of Advanced Industrial Science and Technology (AIST), Ikeda, Osaka 563-8577, Japan

Department of Industrial and Systems Engineering, Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, P. R. China

Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen 518057, P. R. China

National Supercomputing Center in Shenzhen, Shenzhen 518055, P. R. China

Funding

Natural Science Foundation of Jiangsu Province · Nanjing University of Posts and Telecommunications · Hong Kong Polytechnic University · National Natural Science Foundation of China · Natural Science Foundation of Shaanxi Province · Jiangsu National Synergistic Innovation Center for Advanced Materials · Natural Science Foundation of the Higher Education Institutions of Jiangsu Province · Priority Academic Program Development of Jiangsu Higher Education Institutions

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