Bidirectional Tandem Electrocatalysis Manipulated Sulfur Speciation Pathway for High-Capacity and Stable Na-S Battery

Hong Zhang; Bin Song; Weiwei Zhang; Bowen An; Lin Fu; Songtao Lu; Yingwen Cheng; Qianwang Chen; Ke Lu

doi:10.1002/anie.202217009

Bidirectional Tandem Electrocatalysis Manipulated Sulfur Speciation Pathway for High-Capacity and Stable Na-S Battery

Angew Chem Int Ed Engl. 2023 Feb 1;62(6):e202217009. doi: 10.1002/anie.202217009. Epub 2023 Jan 4.

Authors

Hong Zhang^{1

2}, Bin Song³, Weiwei Zhang^{1

4

5}, Bowen An⁶, Lin Fu⁷, Songtao Lu⁵, Yingwen Cheng⁶, Qianwang Chen^{1

2}, Ke Lu^{1

2}

Affiliations

¹ Institutes of Physical Science and Information Technology, School of Materials Science and Engineering, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, Anhui 230601, China.
² Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
³ Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou, Jiangsu 215123, China.
⁴ School of Chemistry and Chemical Engineering, Qufu Normal University, Qufu, Shandong 273165, China.
⁵ School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150001, China.
⁶ Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, IL 60115, USA.
⁷ School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou 550025, China.

PMID: 36494321
DOI: 10.1002/anie.202217009

Abstract

The sluggish polysulfide redox kinetics and the uncontrollable sulfur speciation pathway, leading to serious shuttling effect and high activation barrier associated with sulfur cathode. We describe here the use of core-shell structured composite matrixes containing abundant catalytic sites for nearly fully reversible cycling of sulfur cathodes for Na-S batteries. The bidirectional tandem electrocatalysis provide successive reversible conversion of both long- and short-chain polysulfides, whereas Fe₂ O₃ accelerates Na₂ S₈ /Na₂ S₆ to Na₂ S₄ conversion and the redox-active Fe(CN)₆ ^4- -doped polypyrrole shell catalyzes Na₂ S₄ reduction to Na₂ S. The electrochemically reactive Na₂ S can be readily charged back to sulfur with minimal overpotential. Simultaneously, stable cycling of Na-S pouch cell with a high reversible capacity of 696 mAh g^-1 is also demonstrated. The bidirectional confined tandem catalysis renders the manipulation of sulfur redox electrochemistry for practical Na-S cells.

Keywords: Bidirectional Catalysts; Confined Catalysis; Na-S Battery; Polysulfide Manipulation.

Abstract

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