首页|Polysulfide regulation by defect-modulated Ta3N5-x electrocatalyst toward superior room-temperature sodium-sulfur batteries

Polysulfide regulation by defect-modulated Ta3N5-x electrocatalyst toward superior room-temperature sodium-sulfur batteries

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Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metal-sulfur batteries.Motivated by a theoretical prediction,herein,we strategically propose nitrogen-vacancy tantalum nitride(Ta3N5-x)impregnated inside the interconnected nanopores of nitrogen-decorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in room-temperature sodium-sulfur batteries.Through a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of Ta3N5-x.The defect manipulation on the local envi-ronment enables well-regulated Ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of Ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide conversion.Moreover,the interconnected continuous Ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle behav-ior.Due to these attributes,the as-developed Ta3N5-x-based electrode achieves superior rate capability of 730 mAh g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mAh cm-2 under high sulfur loading of 6.2 mg cm-2.This work not only presents a new sulfur electro-catalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.

Tantalum nitrideNitrogen defectsSodium-sulfur batteriesElectrocatalystsPolysulfide conversion

Zhen Zhang、Dan Luo、Jun Chen、Chuyin Ma、Matthew Li、Haoze Zhang、Renfei Feng、Rui Gao、Haozhen Dou、Aiping Yu、Xin Wang、Zhongwei Chen

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Department of Chemical Engineering,Waterloo Institute for Nanotechnology,University of Waterloo,Waterloo N2L 3G1,Canada

Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China

South China Academy of Advanced Optoelectronics & International Academy of Optoelectronics at Zhaoqing,South China Normal University,Guangzhou 510006,China

Chemical Sciences and Engineering Division,Argonne National Laboratory,Lemont 60439,USA

Canadian Light Source,Saskatoon S7N 2V3,Canada

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University of Waterloo,Waterloo Institute for Nanotechnology,and Natural Sciences and Engineering Research Council of Canada(NSEOutstanding Youth Project of Guangdong Natural Science FoundationDepartment of Science and Technology of Guangdong ProvinceDepartment of Science and Technology of Guangdong ProvinceNatural Science Foundation of NingxiaFoundation of State Key Laboratory of High Efficiency Utilization of Coal and Green Chemical Engineering

2021B15150200512019JC01L2032020B09090300042023AAC010032022-K79

2024

10.1016/j.scib.2023.11.035

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(2)
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