Volume 20, Issue 31 2311750
Research Article

Regulating Electron Filling and Orbital Occupancy of Anti-Bonding States of Transition Metal Nitride Heterojunction for High Areal Capacity Lithium–Sulfur Full Batteries

Jintao Liu

Jintao Liu

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

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Lianghao Yu

Lianghao Yu

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

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Qiwen Ran

Qiwen Ran

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 610054 P. R. China

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Xi'an Chen

Corresponding Author

Xi'an Chen

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Xueyu Wang

Xueyu Wang

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

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Xuedong He

Xuedong He

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

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Huile Jin

Huile Jin

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

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Tao Chen

Tao Chen

CAS Key Laboratory of Materials for Energy Conversion, Department of Materials Science and Engineering, University of Science and Technology of China, No. 96 Jinzhai Road, Hefei, 230026 P. R. China

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Jun Song Chen

Corresponding Author

Jun Song Chen

School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 610054 P. R. China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Daying Guo

Corresponding Author

Daying Guo

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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Shun Wang

Corresponding Author

Shun Wang

Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, 325035 P. R. China

E-mail: [email protected]; [email protected]; [email protected]; [email protected]

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First published: 08 March 2024
Citations: 18

Abstract

The commercialization of lithium–sulfur (Li–S) battery is seriously hindered by the shuttle behavior of lithium (Li) polysulfide, slow conversion kinetics, and Li dendrite growth. Herein, a novel hierarchical p-type iron nitride and n-type vanadium nitride (p-Fe2N/n-VN) heterostructure with optimal electronic structure, confined in vesicle-like N-doped nanofibers (p-Fe2N/n-VN⊂PNCF), is meticulously constructed to work as “one stone two birds” dual-functional hosts for both the sulfur cathode and Li anode. As demonstrated, the d-band center of high-spin Fe atom captures more electrons from V atom to realize more π* and moderate σ* bond electron filling and orbital occupation; thus, allowing moderate adsorption intensity for polysulfides and more effective d–p orbital hybridization to improve reaction kinetics. Meanwhile, this unique structure can dynamically balance the deposition and transport of Li on the anode; thereby, more effectively inhibiting Li dendrite growth and promoting the formation of a uniform solid electrolyte interface. The as-assembled Li–S full batteries exhibit the conspicuous capacities and ultralong cycling lifespan over 2000 cycles at 5.0 C. Even at a higher S loading (20 mg cm−2) and lean electrolyte (2.5 µL mg−1), the full cells can still achieve an ultrahigh areal capacity of 16.1 mAh cm−2 after 500 cycles at 0.1 C.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

Research data are not shared.

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