Two-dimensional quantum-sheet films with sub-1.2 nm channels for ultrahigh-rate electrochemical capacitance

Wenshu Chen; Jiajun Gu; Qinglei Liu; Mengzhao Yang; Cheng Zhan; Xining Zang; Tuan Anh Pham; Guangxiang Liu; Wang Zhang; Di Zhang; Bruce Dunn; Y Morris Wang

doi:10.1038/s41565-021-01020-0

Two-dimensional quantum-sheet films with sub-1.2 nm channels for ultrahigh-rate electrochemical capacitance

Nat Nanotechnol. 2022 Feb;17(2):153-158. doi: 10.1038/s41565-021-01020-0. Epub 2021 Nov 18.

Authors

Wenshu Chen^{1

2}, Jiajun Gu³, Qinglei Liu⁴, Mengzhao Yang¹, Cheng Zhan⁵, Xining Zang⁶, Tuan Anh Pham⁵, Guangxiang Liu², Wang Zhang¹, Di Zhang⁷, Bruce Dunn⁸, Y Morris Wang⁹

Affiliations

¹ State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, China.
² School of Environmental Science and Nanjing Key Laboratory of Advanced Functional Materials, Nanjing Xiaozhuang University, Nanjing, China.
³ State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, China. gujiajun@sjtu.edu.cn.
⁴ State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, China. liuqinglei@sjtu.edu.cn.
⁵ Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, USA.
⁶ Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA.
⁷ State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, China. zhangdi@sjtu.edu.cn.
⁸ Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, CA, USA.
⁹ Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, CA, USA. ymwang@ucla.edu.

PMID: 34795438
DOI: 10.1038/s41565-021-01020-0

Abstract

Dense, thick, but fast-ion-conductive electrodes are critical yet challenging components of ultrafast electrochemical capacitors with high volumetric power/energy densities^1-4. Here we report an exfoliation-fragmentation-restacking strategy towards thickness-adjustable (1.5‒24.0 μm) dense electrode films of restacked two-dimensional 1T-MoS₂ quantum sheets. These films bear the unique architecture of an exceptionally high density of narrow (sub-1.2 nm) and ultrashort (~6.1 nm) hydrophobic nanochannels for confinement ion transport. Among them, 14-μm-thick films tested at 2,000 mV s^-1 can deliver not only a high areal capacitance of 0.63 F cm^-2 but also a volumetric capacitance of 437 F cm^-3 that is one order of magnitude higher than that of other electrodes. Density functional theory and ab initio molecular dynamics simulations suggest that both hydration and nanoscale channels play crucial roles in enabling ultrafast ion transport and enhanced charge storage. This work provides a versatile strategy for generating rapid ion transport channels in thick but dense films for energy storage and filtration applications.

Grants and funding

N00014-19-1-2113/United States Department of Defense | United States Navy | Office of Naval Research (ONR)