调控电催化剂电子结构促进锂硫电池多硫化物催化转化的研究进展

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

催化学报 ›› 2022, Vol. 43 ›› Issue (12): 2946-2965.DOI: 10.1016/S1872-2067(21)63984-0

调控电催化剂电子结构促进锂硫电池多硫化物催化转化的研究进展

曾攀, 袁程, 刘根林, 郜杰昌, 李彦光(), 张亮()

苏州大学功能纳米与软物质研究院, 江苏省碳基功能材料与器件重点实验室, 江苏苏州215123

收稿日期:2022-03-30 接受日期:2022-04-23 出版日期:2022-12-18 发布日期:2022-10-18
通讯作者: 李彦光,张亮
基金资助:
江苏省自然科学基金(BK20190814);国家自然科学基金(11905154);江苏省高校自然科学基金(19KJA550004);苏州纳米科技协同创新中心;江苏省高校优势学科建设工程项目,111计划

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

Pan Zeng, Cheng Yuan, Genlin Liu, Jiechang Gao, Yanguang Li(), Liang Zhang()

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, Jiangsu, China

Received:2022-03-30 Accepted:2022-04-23 Online:2022-12-18 Published:2022-10-18
Contact: Yanguang Li, Liang Zhang
Supported by:
Natural Science Foundation of Jiangsu Province(BK20190814);National Natural Science Foundation of China(11905154);Natural Science Foundation of the Jiangsu Higher Education Institutions of China(19KJA550004);Collaborative Innovation Center of Suzhou Nano Science and Technology;Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD), the 111 Project

摘要/Abstract

摘要：

锂硫电池具有高的理论能量密度(2600 Wh kg^‒1), 是传统金属氧化物正极和石墨负极组装的锂离子电池能量密度的3‒5倍. 同时, 锂硫电池以单质硫作为活性物质, 具有环境友好及价格低廉的优势, 因此被认为是最具发展前景的电化学储能系统之一. 然而, 锂硫电池的商业化应用仍面临诸多挑战和障碍, 比如单质硫和放电产物硫化锂的绝缘特性, 活性物质充放电过程中的体积变化以及多硫化物穿梭导致的活性物质不可逆损失、低的库伦效率及差的循环稳定性等. 对于单质硫及放电产物的绝缘特性, 可通过构建高导电的网络结构或者减小硫颗粒尺寸来克服. 对于充放电过程中活性物质的体积变化问题, 可通过制备柔性电极或者设计具有分级多孔的三维网络结构材料来克服. 唯独对多硫化物的穿梭问题, 还没有找到一种方案来有效解决. 锂硫电池前期的研究工作主要通过调控载体材料的物理结构实现对多硫化物的物理及化学吸附, 从而在一定程度上抑制了多硫化物的穿梭. 然而多硫化物穿梭的产生不仅仅与多硫化物的迁移扩散有关, 更与载体材料界面处多硫化物迟缓的氧化还原转化有关. 当载体材料界面处多硫化物无法实现快速转化时就会导致界面处多硫化物的富集, 进而导致严重的穿梭效应. 因此, 引入各类电催化材料来加速多硫化物的氧化还原转化被认为是更有效抑制穿梭效应的策略之一. 目前已报道的锂硫电池综述大多侧重从催化材料本身的物理及化学结构特性出发进行归纳总结, 但是对于催化材料本身的电子结构与催化活性间的关系鲜有探讨. 实际上, 电催化剂的电子结构在改善催化剂的催化活性进而加速多硫化物氧化还原转化方面起着决定性作用, 因此合理调控电催化剂的电子结构对于抑制穿梭效应, 进而提高锂硫电池的电化学性能具有至关重要的意义.

本文全面概述了锂硫电池中电催化剂电子结构的调控策略, 包括但不限于空位工程、杂原子掺杂、单原子掺杂、能带调节、合金化及异质结构工程等. 此外, 分析了设计高效电催化剂, 构建高能量密度和长寿命锂硫电池的未来发展前景和面临的挑战.

关键词: 锂硫电池, 催化效应, 电子改性, 穿梭效应, 氧化还原动力学

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

曾攀, 袁程, 刘根林, 郜杰昌, 李彦光, 张亮. 调控电催化剂电子结构促进锂硫电池多硫化物催化转化的研究进展[J]. 催化学报, 2022, 43(12): 2946-2965.

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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图/表 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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调控电催化剂电子结构促进锂硫电池多硫化物催化转化的研究进展

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

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