Magnetic-atom strategy enables unilamellar MoS2-C interoverlapped superstructure with ultrahigh capacity and ultrafast ion transfer capability in Li/Na/K-ion batteries

Han，Meisheng1,2,3; Chen，Jiaxin1,2,3; Cai，Yuanyuan1,2,3; Wei，Lei1,2,3; Zhao，Tianshou1,2,3

2023-02-15

10.1016/j.cej.2022.140137

CHEMICAL ENGINEERING JOURNAL   Impact Factor & Quartile

1385-8947

1873-3212

Constructing a unilamellar MoS-C interoverlapped superstructure (UIS) is the most promising way to improve electrical conductivity and alleviate volume expansion of MoS electrodes during Li/Na/K storage due to the maximized atomic interface contact. However, the interlayer distance of ∼ 0.48 nm between MoS and C (lower than 0.62 nm of pristine MoS), the unconspicuous enhancement of intrinsic conductivity of MoS, and the inevitable decrease in capacity due to the introduced low-capacity C undoubtedly hamper ion transport and storage, thus resulting in limited enhancement of capacity and fast-charging performances of UIS. Herein, we propose a magnetic-atom strategy for UIS via a one-step high-pressure vapor-phase synthesis method, during which the interlayer electrostatic repulsion is in-situ constructed by magnetic-atom Fe and/or Co doping to adjust the interlayer distance from 0.48 to 0.64 nm. In addition, the doped magnetic atom can regulate the electronic structure of UIS to obtain the bandgap of 0 eV to enhance electron transfer. Importantly, the doped magnetic atom can be reduced to superparamagnetic metallic nanoparticles during conversion reactions, which can store abundant spin-polarized electrons to induce strong surface-capacitance effects, thus boosting ion transport and storage. Consequently, the magnetic-atom strategy endows the UIS with ultrahigh reversible capacities of 1572.1/738.5/542.3 mAh/g at 0.1C, 971.2/383.5/209.8 mAh/g at 5C after 3000 cycles, and 761.5/340.8/204.5 mAh/g at 20C as Li/Na/K-ion-battery anodes, respectively. This work verifies the efficiency of magnetic-atom strategy and paves a way for the design of other transition metal dichalcogenides for electrochemical energy storage.

Interlayer electrostatic repulsion Li/Na/K-ion batteries Magnetic-atom strategy Surface-capacitance effect Unilamellar MoS2-C interoverlapped superstructure

SCI

English

First ; Corresponding

[202204013000060] ; [R6005-20]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000895300800002

ELSEVIER SCIENCE SA

ENGINEERING

2-s2.0-85141983858

Scopus

1.Shenzhen Key Laboratory of Advanced Energy Storage,Southern University of Science and Technology,Shenzhen,518055,China
2.SUSTech Energy Institute for Carbon Neutrality,Southern University of Science and Technology,Shenzhen,518055,China
3.Department of Mechanical and Energy Engineering,Southern University of Science and Technology,Shenzhen,518055,China

Han，Meisheng,Chen，Jiaxin,Cai，Yuanyuan,et al. Magnetic-atom strategy enables unilamellar MoS2-C interoverlapped superstructure with ultrahigh capacity and ultrafast ion transfer capability in Li/Na/K-ion batteries[J]. CHEMICAL ENGINEERING JOURNAL,2023,454.

Han，Meisheng,Chen，Jiaxin,Cai，Yuanyuan,Wei，Lei,&Zhao，Tianshou.(2023).Magnetic-atom strategy enables unilamellar MoS2-C interoverlapped superstructure with ultrahigh capacity and ultrafast ion transfer capability in Li/Na/K-ion batteries.CHEMICAL ENGINEERING JOURNAL,454.

Han，Meisheng,et al."Magnetic-atom strategy enables unilamellar MoS2-C interoverlapped superstructure with ultrahigh capacity and ultrafast ion transfer capability in Li/Na/K-ion batteries".CHEMICAL ENGINEERING JOURNAL 454(2023).