Suppressing gas swelling in self-assembled Li4Ti5O12 (400) for high-performance rechargeable batteries

Qiwei Wang; Yang Li; Weichan Si; Wenyu Tan; Gao Cheng; Lin Yu; Wei Ran; Jianfang Chen; Yi-Ming Zhao; Chaoling Wu; Wei Liu; Lei Shen; Qiang Wang

doi:10.1016/j.jcis.2023.08.021

Suppressing gas swelling in self-assembled Li₄Ti₅O₁₂ (400) for high-performance rechargeable batteries

J Colloid Interface Sci. 2023 Dec:651:785-793. doi: 10.1016/j.jcis.2023.08.021. Epub 2023 Aug 6.

Authors

Qiwei Wang¹, Yang Li¹, Weichan Si¹, Wenyu Tan¹, Gao Cheng², Lin Yu², Wei Ran¹, Jianfang Chen¹, Yi-Ming Zhao³, Chaoling Wu⁴, Wei Liu⁴, Lei Shen⁵, Qiang Wang⁶

Affiliations

¹ School of Materials and Energy, Southwest University, Chongqing 400715, PR China.
² Key Laboratory of Clean Chemistry Technology of Guangdong Regular Higher Education Institutions, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, PR China.
³ Department of Mechanical Engineering, National University of Singapore, Singapore 117575, Singapore.
⁴ Institute of New-Energy and Low-Carbon Technology, Engineering Research Center of Alternative Energy Materials & Devices, Ministry of Education, Sichuan University, Chengdu 610065, PR China.
⁵ Department of Mechanical Engineering, National University of Singapore, Singapore 117575, Singapore. Electronic address: shenlei@nus.edu.sg.
⁶ School of Materials and Energy, Southwest University, Chongqing 400715, PR China. Electronic address: wysnu@swu.edu.cn.

PMID: 37572614
DOI: 10.1016/j.jcis.2023.08.021

Abstract

Lithium titanate is a promising anode material for lithium-ion batteries due to its high-rate capability and long-cycle duration. However, gas swelling during electrochemical reactions has hindered its industrial application. Here, we synthesize self-assembled (400)-orientation lithium titanate (SA-LTONF) with ultrafine nanoparticles using a feasible thermal method. The SA-LTONF with an organic carbon coating exhibited superior electrochemical performance. To understand such high-rate capability, we perform density functional theory (DFT) calculations which elucidate the orientation-dependent electrochemical mechanism of hydrogen evolution and the atomically dynamic mechanism of lithium-ion migration in Li₄Ti₅O₁₂ and Li₇Ti₅O₁₂. Our findings provide a unique insight into the gas generation and ultrafast lithium-ion transportation in lithium titanate and offer guidance for nanoarchitecture construction and materials design of lithium titanate for commercial applications.

Keywords: High-rate capability; Lithium-ion transportation; Orientation-dependent; Self-assembled lithium titanate; Suppression of gaseous generation.