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

Nature Nanotechnology volume 17, pages 153–158 (2022)Cite this article

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Abstract

Dense, thick, but fast-ion-conductive electrodes are critical yet challenging components of ultrafast electrochemical capacitors with high volumetric power/energy densities1,2,3,4. 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.

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Fig. 1: Schematic of the design and fabrication of 2D 1T-MoS2 QS films.
Fig. 2: Characterizations of 2D 1T-MoS2 QS films.
Fig. 3: Electrochemical performance of the hydrated 2D 1T-MoS2 QS electrodes in 0.5 M H2SO4 electrolyte.
Fig. 4: Comparison of the Cv and Ca of 1T-MoS2 QS electrodes with the benchmark electrodes at scan rates of 1,000 and 2,000 mV s−1 in aqueous electrolytes.

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All the data relevant to the findings of this study have been included in the Supplementary Information.

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No customized code was used in this study.

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Acknowledgements

The work at SJTU was supported by the National Natural Science Foundation of China (grant numbers 52072241, 52071213 and 51772187); the Shanghai Science and Technology Committee (grant number 18JC1410500); and the Natural Science Funds for Colleges and Universities in Jiangsu Province, China (grant number 20KJB430048). The work at LLNL was performed under the auspices of the US Department of Energy under contract number DE-AC52-07NA27344. C.Z. and Y.M.W. acknowledge the support of UCOP Project number LFR-17-477237. T.A.P. was supported as part of the Center for Enhanced Nanofluidic Transport, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences (BES), under award number DESC0019112. B.D. was supported by the Office of Naval Research (grant number N00014-19-1-2113). We thank R. Luo for his help with TEM characterizations and analyses.

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Authors and Affiliations

  1. State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai, China

    Wenshu Chen, Jiajun Gu, Qinglei Liu, Mengzhao Yang, Wang Zhang & Di Zhang

  2. School of Environmental Science and Nanjing Key Laboratory of Advanced Functional Materials, Nanjing Xiaozhuang University, Nanjing, China

    Wenshu Chen & Guangxiang Liu

  3. Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory, Livermore, CA, USA

    Cheng Zhan & Tuan Anh Pham

  4. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Xining Zang

  5. Department of Materials Science and Engineering, University of California, Los Angeles, Los Angeles, CA, USA

    Bruce Dunn & Y. Morris Wang

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Contributions

W.C., J.G., Q.L., D.Z., B.D. and Y.M.W. conceived the idea and designed the experiments. W.C. and M.Y. carried out most of the materials synthesis and electrochemical experiments under the guidance of J.G., Q.L. and D.Z. C.Z. and T.A.P. performed all theoretical calculations. X.Z., G.L. and W.Z. carried out some characterizations and analysis of experiments. W.C., J.G., Q.L. and Y.M.W. wrote the manuscript with contributions from all the co-authors.

Corresponding authors

Correspondence to Jiajun Gu, Qinglei Liu, Di Zhang or Y. Morris Wang.

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Peer review information Nature Nanotechnology thanks Xuebin Zhu and other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–32, Tables 1–4 and references.

Supplementary Video 1

The animation of the diffusion of solvated H3O+ in a −1|e| charged 0.8 nm MoS2 channel from the AIMD trajectory in a top view along the z direction.

Supplementary Video 2

The animation of the diffusion of solvated K+ in a −1|e| charged 0.8 nm MoS2 channel from the AIMD trajectory in a top view along the z direction.

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Chen, W., Gu, J., Liu, Q. et al. Two-dimensional quantum-sheet films with sub-1.2 nm channels for ultrahigh-rate electrochemical capacitance. Nat. Nanotechnol. 17, 153–158 (2022). https://doi.org/10.1038/s41565-021-01020-0

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