Monolayer MoS2 Fabricated by In Situ Construction of Interlayer Electrostatic Repulsion Enables Ultrafast Ion Transport in Lithium-Ion Batteries

Abstract

Highlights In-situ construction of electrostatic repulsion between MoS 2 interlayers is first proposed to successfully prepare Co-doped monolayer MoS 2 under high vapor pressure. The doped Co atoms radically decrease bandgap and lithium ion diffusion energy barrier of monolayer MoS 2 and can be transformed into ultrasmall Co nanoparticles (~2 nm) to induce strong surface-capacitance effect during conversion reaction. The Co doped monolayer MoS 2 shows ultrafast ion transport capability along with ultrahigh capacity and outstanding cycling stability as lithium-ion-battery anodes. Abstract High theoretical capacity and unique layered structures make MoS 2 a promising lithium-ion battery anode material. However, the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS 2 lead to unacceptable ion transport capability. Here, we propose in-situ construction of interlayer electrostatic repulsion caused by Co 2 + substituting Mo 4+ between MoS 2 layers, which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS 2 , thus establishing isotropic ion transport paths. Simultaneously, the doped Co atoms change the electronic structure of monolayer MoS 2 , thus improving its intrinsic conductivity. Importantly, the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport. Hence, the Co-doped monolayer MoS 2 shows ultrafast lithium ion transport capability in half/full cells. This work presents a novel route for the preparation of monolayer MoS 2 and demonstrates its potential for application in fast-charging lithium-ion batteries. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-023-01042-4.

Boosting Charge Transport and Catalytic Performance in MoS2 by Zn2+ Intercalation Engineering for Lithium–Sulfur Batteries

“…In Figure a, it is obvious that as the amount of embedded Zn 2+ increases from 0 to 0.18 mmol, the diffraction peak associated with the MoS 2 (002) plane moves to a lower angle from 14.34° to 13.35°. The shift of the XRD peak further confirms the expansion of the interlayer spacing, which is consistent with the results obtained by HRTEM . The fwhm of the peak near 14° in the XRD spectrum of the sample was fitted.…”

“…The shift of the XRD peak further confirms the expansion of the interlayer spacing, which is consistent with the results obtained by HRTEM. 29 The fwhm of the peak near 14°in the XRD spectrum of the sample was fitted.…”

Hierarchical Spatial Confinement Unlocking the Storage Limit of MoS2 for Flexible High-Energy Supercapacitors

“…The desirable electronic conductivity, low K-ion migration barrier, and high diffusion coefficient of Co-EG/S V -MoS 2 enable its superior rate performance. As shown in Figure l, a radar chart summarizes and compares various parameters, including the interlayer distance, 1T phase content, migration barrier, cycling numbers, and specific capacitance, of the Co-EG/S V -MoS 2 electrode with other reported MoS 2 -based electrodes that have been optimized through strategies such as structural optimization, composite engineering, 1T phase transition, anion vacancy, and cation substitution . Compared with these alternative optimization strategies, the hierarchical confinement design demonstrates greater advantages and potential for enhancing the capacitive performance.…”

“…As shown in Figure 4l, a radar chart summarizes and compares various parameters, including the interlayer distance, 1T phase content, migration barrier, cycling numbers, and specific capacitance, of the Co-EG/S V -MoS 2 electrode with other reported MoS 2 -based electrodes that have been optimized through strategies such as structural optimization, 40 composite engineering, 41 1T phase transition, 42 anion vacancy, 43 and cation substitution. 44 Compared with these alternative optimization strategies, the hierarchical confinement design demonstrates greater advantages and potential for enhancing the capacitive performance. The enhanced electrochemical performance of Co-EG/S V -MoS 2 is attributed to the following factors: (i) Abundant sulfur vacancies are created in Co-EG/S V -MoS 2 due to the reduction of EG molecules during the preparation process.…”

Interfacial engineering of transition metal dichalcogenide/carbon heterostructures for electrochemical energy applications

“…The substrates enhance the reaction kinetics in several ways as follows: (1) by improving the distribution of 2D TMDCs, (2) by enhancing electrical conductivity, and (3) by improving structural stability during repeated cycles. 50–56 This has led to increased use of TMDC/C heterostructures for achieving improved reaction kinetics and electrochemical performance in both EES and EEC devices. 57 In the past few years, several reviews have summarized the progress of TMDC/C heterostructures for the application in EES or EEC devices, with emphasis on the preparation method, nanostructure design, and electrochemical performance improvement.…”