Catalytic Current Collector Design to Accelerate LiNO₃ Decomposition for High-Performing Lithium Metal Batteries

Zhang, Qicheng1,2; Xu, Lei3; Yue, Xinyang1; Liu, Jijiang1; Wang, Xin4; He, Xiaoya1; Shi, Zidan1; Niu, Shuzhang4; Gao, Wei2; Cheng, Chun3; Liang, Zheng1

2023-10-01

10.1002/aenm.202302620

ADVANCED ENERGY MATERIALS   Impact Factor & Quartile

1614-6832

1614-6840

Lithium nitrate is an attractive lithium additive in the construction of high-performance lithium metal anodes with a Li3N-rich solid electrolyte interphase (SEI) layer. However, the eight-electron transfer process induces high energy barriers between LiNO3 and Li3N. Herein, the inner Helmholtz plane is tuned on a Li deposition host to attain sluggish/rapid LiNO3 decomposition kinetics, resulting in different intermediate content distributions of Li species in the SEI. Notably, lithium oxynitride (LiNO) is identified as the decomposition intermediate, and experimental and simulation results confirm its role in obstructing LiNO3 decomposition. Moreover, the results reveal that the dipole-dipole interaction between LiNO and the polar V equivalent to N bond can change the ionic/covalent character of the NO bonds, considerably facilitating the energy transfer process of the NO cleavage, and promoting a LiNO3 reduction to achieve a Li3N-rich SEI. Consequently, when the electrolyte contains 0.37 m LiNO3, dendrite, and dead Li formation are suppressed effectively with the VN system, and an average Coulombic efficiency of 99.7% over 1000 cycles (1 mA cm(-2), 1 mAh cm(-2)) can be attained. These results can promote the nitride oxidation break process and pave the way for fabricating high-performance Li3N-rich lithium metal batteries.

electrolyte decomposition lithium dendrite lithium metal batteries lithium nitride solid electrolyte interphases

SCI

English

Corresponding

This work was supported by the National Natural Science Foundation of China (NSFC) under Grant No. 52102282 and 51972161, the Young Elite Scientists Sponsorship Program by CAST (2020QNRC001), and start-up funds from Shanghai Jiao Tong University.["52102282","51972161"] ; National Natural Science Foundation of China (NSFC)[2020QNRC001]

Chemistry ; Energy & Fuels ; Materials Science ; Physics

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001076303300001

WILEY-V C H VERLAG GMBH

Web of Science

1.Shanghai Jiao Tong Univ, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China
2.Univ Auckland, Fac Engn, Dept Chem & Mat Engn, Auckland 1010, New Zealand
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Shenzhen Technol Univ, Coll New Mat & New Energies, Shenzhen 518118, Peoples R China

Zhang, Qicheng,Xu, Lei,Yue, Xinyang,et al. Catalytic Current Collector Design to Accelerate LiNO₃ Decomposition for High-Performing Lithium Metal Batteries[J]. ADVANCED ENERGY MATERIALS,2023.

Zhang, Qicheng.,Xu, Lei.,Yue, Xinyang.,Liu, Jijiang.,Wang, Xin.,...&Liang, Zheng.(2023).Catalytic Current Collector Design to Accelerate LiNO₃ Decomposition for High-Performing Lithium Metal Batteries.ADVANCED ENERGY MATERIALS.

Zhang, Qicheng,et al."Catalytic Current Collector Design to Accelerate LiNO₃ Decomposition for High-Performing Lithium Metal Batteries".ADVANCED ENERGY MATERIALS (2023).