Tailoring surface chemistry of MXenes to boost initial coulombic efficiency for lithium storage

• Published in: Applied surface science Vol. 612; p. 155875
• Main Authors: Guan, Yunfeng, Zhao, Rong, Li, Ke, Chen, Kai, Zhu, Hui, Li, Xuanke, Zhang, Qin, Yang, Nianjun, Dong, Zhijun, Yuan, Guanming, Li, Yanjun, Cong, Ye
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.03.2023
• Subjects: Heteroatoms doping; Initial coulombic efficiency; Lithium storage; MXene; Surface chemistry; Initial coulombic efficiency; MXene; Surface chemistry; Lithium storage; Heteroatoms doping
• ISSN: 0169-4332; 1873-5584
• DOI: 10.1016/j.apsusc.2022.155875

A facile d-band center regulation strategy via doping engineering is proposed to tailor the surface chemistry of MXenes, where the higher chemical affinity and absorbability for oxygen-containing functional groups and lithium ions effectively improve the lithium storage performance, particularly the initial coulombic efficiency. [Display omitted] •Heteroatoms doping induces intrinsic charge redistribution, thereby modulating the d-band center.•Favorable surface chemistry of MXene is tailored due to the shift of d-band center towards the Fermi level.•V1.8Cr0.2C MXene delivers a superior reversible capacity and initial coulombic efficiency.•The d-band center regulation strategy via doping engineering is applicable to various MXenes. MXenes are expected to exhibit excellent lithium-ion storage performance due to its good electron conductivity, tunable functional groups, and unique accordion-like structure. However, they suffer from low initial coulombic efficiency (ICE) caused by the trapping and the irreversible reaction between MXene nanosheets and lithium ions. In this work, we propose a facile d-band center regulation strategy via doping engineering to achieve tailorable surface chemistry of MXene, revealing the intrinsic effects of heteroatoms doping on surface chemistry and ICE. This strategy can be applied to various MXenes, which is verified in the case of V2-yCryC as well as TiNbC, and TiVC MXenes. Typically, the V1.8Cr0.2C MXene delivers a double lithium storage capacity in comparison to V2C MXene. Its ICE is improved from 60% to 86%, surpassing most state-of-the-art MXenes. Theoretical calculations reveal that the shift of the d-band center towards the Fermi level is induced by the introduction of Cr and responsible for the improved electrochemical performance. It increases its chemical affinity and absorbability for oxygen-containing functional groups and lithium ions, providing a favorable surface chemistry for efficient lithium storage. This work provides a new strategy to tailor the fine structures of MXenes for their further energy storage applications.