Highly Reversible Sodium-ion Storage in A Bifunctional Nanoreactor Based on Single-atom Mn Supported on N-doped Carbon over MoS(2) Nanosheets

Affiliations
  • 1School of Materials Science and Engineering, Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin, 300350, P. R. China E-mails.
  • 2Tianjin Key Laboratory of Materials Laminating Fabrication and Interface Control Technology, School of Materials Science and Engineering, Hebei University of Technology, Tianjin, 300401, People’s Republic of China.
  • 3National Industry-Education Platform of Energy Storage, Tianjin University, 135 Yaguan Road, Tianjin, 300350, People’s Republic of China.
  • 4Xi’an Key Laboratory of Functional Organic Porous Materials, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an, 710129, P. R. China.
  • 5Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, P. R. China.
  • 6Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, P. R. China.

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Abstract

Conversion-type electrode materials have gained massive research attention in sodium-ion batteries (SIBs), but their limited reversibility hampers practical use. Herein, we report a bifunctional nanoreactor to boost highly reversible sodium-ion storage, wherein a record-high reversible degree of 85.65 % is achieved for MoS anodes. Composed of nitrogen-doped carbon-supported single atom Mn (NC-SAMn), this bifunctional nanoreactor concurrently confines active materials spatially and catalyzes reaction kinetics. In situ/ex situ characterizations including spectroscopy, microscopy, and electrochemistry, combined with theoretical simulations containing density functional theory and molecular dynamics, confirm that the NC-SAMn nanoreactors facilitate the electron/ion transfer, promote the distribution and interconnection of discharging products (NaS/Mo), and reduce the NaS decomposition barrier. As a result, the nanoreactor-promoted MoS anodes exhibit ultra-stable cycling with a capacity retention of 99.86 % after 200 cycles in the full cell. This work demonstrates the superiority of bifunctional nanoreactors with two-dimensional confined and catalytic effects, providing a feasible approach to improve the reversibility for a wide range of conversion-type electrode materials, thereby enhancing the application potential for long-cycled SIBs.