N, S-Coordinated Co Single Atomic Catalyst Boosting Adsorption and Conversion of Lithium Polysulfides for Lithium-Sulfur Batteries

Liu, Kun1,2,3; Wang, Xinyang1,2,3; Gu, Shuai1,2,3; Yuan, Huimin1,2,3; Jiang, Feng1,2,3; Li, Yingzhi1,2,3; Tan, Wen1,2,3; Long, Qiurong1,2,3; Chen, Jingjing1,2,3; Xu, Zhenghe1,2,3; Lu, Zhouguang1,2,3

2022-10-01

10.1002/smll.202204707

Small   Impact Factor & Quartile

1613-6810

1613-6829

Boosting reversible solid-liquid phase transformation from lithium polysulfides to Li2S and suppressing the shuttling of lithium polysulfides from the cathode to the lithium anode are critical challenges in lithium-sulfur batteries. Here, sulfiphilic single atomic cobalt implanted in lithiophilic heteroatoms-dopped carbon (SACo@HC) matrix with a CoN3S structure for high-performance lithium-sulfur batteries is reported. Density functional theory calculation and in situ experiments demonstrate that the optimal CoN3S structure in SACo@HC can effectively improve the adsorption and redox conversion efficiency of lithium polysulfides. Consequently, the S-SACo@HC composite with sulfur loading of 80 wt% delivers a high capacity of 1425.1 mAh g(-1) at 0.05 C and outstanding rate performance with 745.9 mAh g(-1) at 4 C. Furthermore, a capacity of 680.8 mAh g(-1) at 0.5 C with a low electrolyte/sulfur ratio (6 mu L mg(-1)) can be achieved even after 300 cycles. With the harsh conditions of lean electrolyte (E/S = 4 mu L mg(-1)) and high sulfur loading (5.4 mg cm(-2)), a superior area capacity of 5.8 mAh cm(-2) can be obtained. This work contributes to building a profound understanding of the adsorption and interface engineering of lithium polysulfides and provides ideas to tackle the long-standing polysulfide shuttle problem of lithium-sulfur batteries.

CoN S-3 active moiety heteroatoms-doped carbon lithium polysulfides conversion lithium-sulfur batteries single-atom catalysts

SCI

English

First ; Corresponding

Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[JCYJ20200925154236004] ; Leading Talents of Guangdong Province Program[2016LJ06C536] ; Guangdong-Hong Kong-Macau Joint Laboratory[2019B121205001] ; Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies[EEST2021-1] ; National Natural Science Foundation of China["51974162","21938003","22008105"]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000863678500001

WILEY-V C H VERLAG GMBH

Web of Science

1.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Interfacial Sci & Engn Mat, Shenzhen 518055, Peoples R China
2.Guangdong Southern Univ Sci & Technol, Key Univ Lab Highly Efficient Utilizat Solar Ener, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Guangdong Hong Kong Macau Joint Lab Photon Therma, Shenzhen 518055, Peoples R China

Liu, Kun,Wang, Xinyang,Gu, Shuai,et al. N, S-Coordinated Co Single Atomic Catalyst Boosting Adsorption and Conversion of Lithium Polysulfides for Lithium-Sulfur Batteries[J]. Small,2022.

Liu, Kun.,Wang, Xinyang.,Gu, Shuai.,Yuan, Huimin.,Jiang, Feng.,...&Lu, Zhouguang.(2022).N, S-Coordinated Co Single Atomic Catalyst Boosting Adsorption and Conversion of Lithium Polysulfides for Lithium-Sulfur Batteries.Small.

Liu, Kun,et al."N, S-Coordinated Co Single Atomic Catalyst Boosting Adsorption and Conversion of Lithium Polysulfides for Lithium-Sulfur Batteries".Small (2022).