Enabling Efficient Anchoring-Conversion Interface by Fabricating Double-Layer Functionalized Separator for Suppressing Shuttle Effect
Junan Feng
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
These authors equally contributed to this work.
Contribution: Formal analysis (equal), Investigation (equal), Methodology (equal), Project administration (equal)
Search for more papers by this authorChaoyue Zhang
College of Mechanical and Electrical Engineering, Qingdao University, Qingdao, 266071 P. R. China
These authors equally contributed to this work.
Contribution: Conceptualization (equal), Investigation (equal), Methodology (equal), Writing - original draft (equal)
Search for more papers by this authorWendong Liu
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Search for more papers by this authorShunxian Yu
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Contribution: Methodology (supporting), Software (supporting), Validation (supporting)
Search for more papers by this authorLei Wang
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Department of Chemical Engineering, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorProf. Tianyi Wang
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002 P. R. China
Search for more papers by this authorProf. Chuan Shi
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Xiaoxian Zhao
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding, 071001 P. R. China
Contribution: Resources (equal), Supervision (equal)
Search for more papers by this authorCorresponding Author
Prof. Shuangqiang Chen
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Department of Chemical Engineering, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444 P. R. China
Contribution: Project administration (equal), Resources (equal), Software (equal), Writing - review & editing (equal)
Search for more papers by this authorCorresponding Author
Prof. Shulei Chou
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Jianjun Song
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Contribution: Project administration (equal), Resources (equal), Supervision (equal), Visualization (equal), Writing - review & editing (equal)
Search for more papers by this authorJunan Feng
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
These authors equally contributed to this work.
Contribution: Formal analysis (equal), Investigation (equal), Methodology (equal), Project administration (equal)
Search for more papers by this authorChaoyue Zhang
College of Mechanical and Electrical Engineering, Qingdao University, Qingdao, 266071 P. R. China
These authors equally contributed to this work.
Contribution: Conceptualization (equal), Investigation (equal), Methodology (equal), Writing - original draft (equal)
Search for more papers by this authorWendong Liu
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Search for more papers by this authorShunxian Yu
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Contribution: Methodology (supporting), Software (supporting), Validation (supporting)
Search for more papers by this authorLei Wang
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Department of Chemical Engineering, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorProf. Tianyi Wang
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002 P. R. China
Search for more papers by this authorProf. Chuan Shi
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Xiaoxian Zhao
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding, 071001 P. R. China
Contribution: Resources (equal), Supervision (equal)
Search for more papers by this authorCorresponding Author
Prof. Shuangqiang Chen
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Department of Chemical Engineering, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444 P. R. China
Contribution: Project administration (equal), Resources (equal), Software (equal), Writing - review & editing (equal)
Search for more papers by this authorCorresponding Author
Prof. Shulei Chou
Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China
Search for more papers by this authorCorresponding Author
Prof. Jianjun Song
College of Physics, Qingdao University, Qingdao, 266071 P. R. China
Contribution: Project administration (equal), Resources (equal), Supervision (equal), Visualization (equal), Writing - review & editing (equal)
Search for more papers by this authorGraphical Abstract
A novel double-layer strategy to functionalize separators is proposed, where Co/CoN4 layer serves as adsorption-catalytic centers for high-order and low-order LiPSs, combined with 2D MXene layer that acts as the second barrier for additional leaked LiPSs, and thus a circulation interface of adsorption-conversion-reactivation of S species has been realized, effectively alleviating the shuttle effect in lithium-sulfur/selenium batteries.
Abstract
Lithium-sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature of ordinary separators to LiPSs. To tackle these, a novel double-layer strategy to functionalize separators is proposed, which consists of Co with atomically dispersed CoN4 decorated on Ketjen black (Co/CoN4@KB) layer and an ultrathin 2D Ti3C2Tx MXene layer. The theoretical calculations and experimental results jointly demonstrate metallic Co sites provide efficient adsorption and catalytic capability for long-chain LiPSs, while CoN4 active sites facilitate the absorption of short-chain LiPSs and promote the conversion to Li2S. The stacking MXene layer serves as a microscopic barrier to further physically block and chemically anchor the leaked LiPSs from the pores and gaps of the Co/CoN4@KB layer, thus preserving LiPSs within efficient anchoring-conversion reaction interfaces to balance the accumulation of “dead S” and Li2S. Consequently, with an ultralight loading of Co/CoN4@KB-MXene, the LiSBs exhibit amazing electrochemical performance even under high sulfur loading and lean electrolyte, and the outperforming performance for lithium-selenium batteries (LiSeBs) can also be achieved. This work exploits a universal and effective strategy of a double-layer functionalized separator to regulate the equilibrium adsorption-catalytic interface, enabling high-energy and long-cycle LiSBs/LiSeBs.
Conflict of Interests
All authors declared that there are no conflicts of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
Supporting Information
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| anie202407042-sup-0001-misc_information.pdf2.8 MB | Supporting Information |
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