Recent progress in electronic modulation of electrocatalysts for high-efficient polysulfide conversion of Li-S batteries

doi:10.1016/S1872-2067(21)63984-0

Abstract

Abstract:

With the merits of high energy density, environmental friendliness, and cost effectiveness, lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation electrochemical storage systems. However, the notorious polysulfide shuttle effect, which results in low active material utilization and serious capacity fading, severely impedes the practical application of Li-S batteries. Utilizing various electrocatalysts to improve the polysulfide redox kinetics has recently emerged as a promising strategy to address the shuttle effect. Specially, the electronic structure of the electrocatalysts plays a decisive role in determining the catalytic activity to facilitate the polysulfide conversion. Therefore, reasonably modulating the electronic structure of electrocatalysts is of paramount significance for improving the electrochemical performance of Li-S batteries. Herein, a comprehensive overview of the fascinating strategies to tailor the electronic structure of electrocatalysts for Li-S batteries is presented, including but not limited to vacancy engineering, heteroatom doping, single atom doping, band regulation, alloying, and heterostructure engineering. The future perspectives and challenges are also proposed for designing high-efficient electrocatalysts to construct high-energy-density and long-lifetime Li-S batteries.

Key words: Lithium-sulfur batteries, Catalytic effect, Electronic modification, Shuttle effect, Redox kinetics

Pan Zeng, Cheng Yuan, Genlin Liu, Jiechang Gao, Yanguang Li, Liang Zhang. Recent progress in electronic modulation of electrocatalysts for high-efficient polysulfide conversion of Li-S batteries[J]. Chinese Journal of Catalysis, 2022, 43(12): 2946-2965.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63984-0

https://www.cjcatal.com/EN/Y2022/V43/I12/2946

Figures/Tables 10

Fig. 1. Schematic illustration of the strategies for regulating the electronic structure of electrocatalysts to address the key challenges of Li-S batteries. Reprinted with permission from Ref. [150]. Copyright 2020, American Chemical Society. Reprinted with permission from Ref. [152]. Copyright 2019, Wiley-VCH. Reprinted with permission from Ref. [179]. Copyright 2021, American Chemical Society. Reprinted with permission from Ref. [171]. Copyright 2020, American Chemical Society. Reprinted with permission from Ref. [207]. Copyright 2019, Wiley-VCH. Reprinted with permission from Ref. [208]. Copyright 2018, Elsevier. Reprinted with permission from Ref. [215]. Copyright 2019, Wiley-VCH. Reprinted with permission from Ref. [211]. Copyright 2020, American Chemical Society. Reprinted with permission from Ref. [218]. Copyright 2021, Elsevier. Reprinted with permission from Ref. [227]. Copyright 2021, Wiley-VCH.

Fig. 2. (a) Schematic configuration of Li-S batteries. (b) Discharge/charge voltage profiles and corresponding reaction mechanism [15]. Reprinted with permission from Ref. [15]. Copyright 2020, Wiley-VCH.

Fig. 3. (a) Ta L3-edge XANES spectra of Ta2O5 related samples; (b) Band diagram of a-Ta2O5?x/MCN; Ta L3-edge XANES spectra (c) and FT-EXAFS (d) of Ta L-edge in a-Ta2O5-x/MCN/S at different discharge/charge states. (a?d) Reprinted with permission from Ref. [141]. Copyright 2020, Elsevier. (e) Crystal structure of Ni3N0.85. (f) Schematic illustration of rational catalyst design by correlating activation barrier with orbital interactions. (g) Partial density of states for Ni 3d orbitals. (h) COOP diagram of the S1-S2 and S3-S4 bonds of Li2S4. (e?h) Reprinted with permission from Ref. [150]. Copyright 2020, American Chemical Society. (i) DOS patterns of Fe3C and Fe3-xC. Reprinted with permission from Ref. [154]. Copyright 2020, Wiley-VCH. (j) Atomic structure model and illustration of polysulfides etching process. (i,j) Reprinted with permission from Ref. [152]. Copyright 2019, Wiley-VCH.

Fig. 4. (a) The reaction pathways from S8 to Li2S for different pyridinic N configurations and pure graphene; Illustrations of the working mechanism of graphene (b), N-doped graphene (c), and N-rich graphene (d). Reprinted with permission from Ref. [169]. Copyright 2020, Wiley-VCH.

Fig. 5. Optimized interaction configurations between polysulfides and the (311) (a) and (440) (b) surfaces of Co9S8 and N-Co9S8 nanoparticles, respectively. (a,b) Reprinted with permission from Ref. [163]. Copyright 2020, Wiley-VCH. DOS (c) and PDOS (d) of CoSe2 and N-CoSe2. (e) PDOS of Co 3d. The vertical view models and charge number of Co for DFT calculation of CoSe2 (f) and N-CoSe2 (g). (h) The bond lengths of CoSe2 and N-CoSe2. (i) The Li-S bond lengths of Li2S on the surfaces of CoSe2 and N-CoSe2 and possible conversion mechanism of sulfur species on the surface of N-CoSe2. (c-g) Reprinted with permission from Ref. [171]. Copyright 2020, American Chemical Society.

Fig. 6. (a) Formation energies of 1T and 2H MoS2 with different Co doping contents. (b) Formation energies of sulfur vacancies in MoS2 and Co-MoS2 with the Co/Mo atomic ratio of 1:5. (c) Schematic illustration of the structure and phase transition of MoS2 after Co doping. (a-c) Reprinted with permission from Ref. [179]. Copyright 2021, American Chemical Society. (d) Mo K-edge FT-EXAFS of Co-MoSe2/MXene, MoSe2/MXene, and Mo foil; TDOS plots (e) and PDOS plots (f,g) of the main orbital contribution for MoSe2 and Co-MoSe2. (d-g) Reprinted with permission from Ref. [183]. Copyright 2021, American Chemical Society. (h) Intercalation process of Sn atoms into MoO3 nanoribbons; (i,j) DOS of MoO3 and Sn-MoO3 slab, respectively; (k,l) DOS of Li2S4 adsorbed on MoO3 and Sn-MoO3 slab, respectively. (d-l) Reprinted with permission from Ref. [184]. Copyright 2019, Wiley-VCH.

Fig. 7. (a) DOS of CN and Fe-N2/CN. (b) PDOS of the Fe atom anchored on Fe-N2/CN. (c) Decomposition energy barriers of Li2S on Fe-N2/CN and CN. (a?c) Reprinted with permission from Ref. [201]. Copyright 2020, American Chemical Society. Simulated deformation charge density of SA-Fe (d) and Fe2N (e). Geometric configurations of Li2S6 on SA-Fe (f) and Fe2N (g). (h) Binding energy of sulfur species adsorbed on NG, SA-Fe, and Fe2N. (i) Energy profiles for the reduction of polysulfides and decomposition of the Li2S on NG, SA-Fe, and Fe2N; Decomposition energy barriers of Li2S on NG (j), SA-Fe (k), and Fe2N (l). (d?l) Reprinted with permission from Ref. [202]. Copyright 2021, Wiley-VCH.

Fig. 8. (a) COOP of Ni2P and Ni2Co4P3. (b) DOS showing the d-bands shift upon Co doping. (c) Activation energy change of Li2S nucleation when using Ni2P and Ni2Co4P3. (a?c) Reprinted with permission from Ref. [207]. Copyright 2019, Wiley-VCH. (d) DOS analysis of the p bands of anions and the d bands of Co in Co-based compounds. (e) Scaling relation between the d band center and Li-S redox potentials for Co-based compounds. (f) Diffusion energy barriers of Li2S on Co-based compounds. (g) Adsorption configurations and energies of Li2S6 and Li2S on rGO and Co-based compounds. (d?g) Reprinted with permission from Ref. [208]. Copyright 2018, Elsevier. (h) DOS of the p- and the d-bands of Fe3C, Fe3O4, and Fe3N; (i) the relationship of ∆ band center (d-p) and reaction voltage of Li2S4. (j) Radial distribution functions of S-S molecules. (h?j) Reprinted with permission from Ref. [210]. Copyright 2021, Wiley-VCH.

Fig. 9. (a) Pt 4f XPS spectra of Pt, Pt-Ni (2 h), and Pt-Ni (4 h). (b) Diagram of the HOMO and LUMO energy levels showing a reactive energy barrier between short-chain polysulfides and catalysis for Pt, Pt-Ni alloy, and Ni. (c) Adsorption energy of various polysulfides on different catalyst surfaces. (a?c) Reprinted with permission from Ref. [215]. Copyright 2019, Wiley-VCH. AIMD simulations of the adsorption of S8 on CoTe2 (d) and Co (e). (d,e) Reprinted with permission from Ref. [218]. Copyright 2021, Elsevier. (f) Catalytic conversion mechanism of Fe-Ni alloys. (f) Reprinted with permission from Ref. [220]. Copyright 2021, American Chemical Society.

Fig. 10. (a) Working schematic illustration of MoS2-MoN heterostructure. Reprinted with permission from Ref. [227]. Copyright 2021, Wiley-VCH. (b) Schematic illustration of the conversion from polysulfides to Li2S on SnO2-Mo2N surface. (c) High-resolution TEM image of SnO2-Mo2N. (a?c) Reprinted with permission from Ref. [237]. Copyright 2021, American Chemical Society. (d) High-resolution TEM image of MoN-VN. (e) Mo L-edge NEXAFS spectra of MoN-VN and MoN. (f) Mo 3d XPS spectra of MoN, MoN-VN, and MoN-VN-polysulfides. (g) DOS of Mo on surface of V-MoN and MoN. (d?g) Reprinted with permission from Ref. [239]. Copyright 2018, Wiley-VCH.

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