近日，广西民族大学黄克靖教授团队等人在Advanced Energy Materials上发表综述文章，论文题为“Recent Advances of Transition Metal Sulfides/Selenides Cathodes for Aqueous Zinc-Ion Batteries”。可充电锌离子电池因其安全性高、环保、成本低、兼容性好而在储能系统中引起了极大的关注。过渡金属硫化物和硒化物由于其独特的层状结构和可调的层间距而被认为是有希望的含水锌基化合物正极,用于加速水合锌的扩散和可逆嵌入。然而,它们的些缺陷严重阻碍了它们的实际应用，如较差的电子导电性、较大的离子扩散能垒和较差的循环稳定性。本文对改善过渡金属硫化物和硒化物正极材料电化学性能的各种改性策略,包括相工程、缺陷工程、层间插层、原位电化学氧化、杂化、掺杂效应和表面改性进行了分类和重点介绍，并针对具体的改性策略进行了讨论和总结。最后，作者提出了机理探索技术、电解质策略、协同工程、高容量转换型、高电压正极材料和摇椅型电池等几个重点突破方向，进一步推动水性ZIBs的发展，指导高性能水性ZIBs正极材料的设计。

Figure 1. Schematic illustration of the composition of rechargeable aqueous ZIBs. Reproduced with permission.I Copyright 2020, RSC. b) The ratio percentage of various cathode materials for aqueous ZIBs. Reproduced with permission.(3) Copyright 2019, Wiley-VCH. c) The brief development history of cathodes for aqueous ZIBs. d) Schematic diagram of the two-step Zn2* insertion/extraction process in VSe, cathode. Reproduced with permission.

Figure 2.   a) Schematic illustration of strategies developed to enhance Zn2+ diffusion kinetics. Reproduced with permission.IS0I Copyright 2019, American Chemical Society. b) HRTEM image of the MoS2/PANI-150 hybrid. c) The charge density. d) Band structures. Reproduced with permission.162) Copyright 2021, Elsevier. e) Schematic fabrication process and f) HRTEM image of h-MoS@CF. g) Schematic illustrations of hydrated Zn2+ inserts into dehydrated MoSz (left) and hydrated MoSz (right). h) Long-term cycling stability of h-Mosz@CF. Reproduced with permission.163) Copyright 2021, Elsevier.

Figure 3.  a) Illustration of the rechargeable Zn/MoS2 battery system. b) HRTEM image of MoSz cathode. c) Calculated diffusion pathway of Zn from one octahedral site to a neighboring octahedral site via an adjacent tetrahedral site (left 2H phase and right IT phase MoS2). d) Calculated energy profiles of Zn diffusion in 2H phase and IT phase MoSz with different interlayer distances. e) Cycle properties of MoSz cathodes. Reproduced with permission.P Copyright 2020, Elsevier. f) Schematic illustration of the preparation process of MoS2. g) HRTEM image of 200- MoSz. h) HRTEM images of the in-plane 1T-MoSz. i) Cycle properties of MoSz cathodes at different temperatures. Reproduced with permission.

Figure 4.  a) Atomic resolution ADF images of various intrinsic point defects present in monolayer CVD MoSz, including Vs, Vs2, Mos2, VMoS3, VMo56n and S2Mo- Reproduced with permission.P6 Copyright 2013, American Chemical Society. b) HAADF STEM image (SAED inset) and c) high-magnification HAADF STEM image of defect-free MoSz nanosheets. d) Long-term cyclic properties of defect-rich MoSz electrode. Reproduced with permission.[52) Copyright 2019, Elsevier. e) Illustration of the preparation process and the crystal structure of D-MoSz-O. f) HAADF-TEM image of D-MoS2-O. g) Zn-ion migration behaviors along the ab plane in MoSz with S-vacancy. h) Diagram of the flexible quasi-solid-state Zn-ion battery. i) Optical image of an LED array powered by five wearable series batteries. Reproduced with permission.

Figure 5. a) TEM images with SAED patterns, and b) HRTEM image of N-doped IT MoSz. c) EPR spectra of MoSz materials. Cycle stability at d) 1A g' and e) 3 A g-'. Reproduced with permission.191l Copyright 2021, American Chemical Society. f) Illustration of the synthetic process of C-MoSz-NC.g) Schematic illustration for the diffusion path of a Zn atom in the MoSz-NC model. h) The curves of diffusion energy barriers in the models of MoS2NC, MoS2-C, and MoS2. i) In situ synchrotron XRD patterns (2 = 0.6888 nm), the 2D contour map of peaks around 20 of 9.2°. j) Cycle performance of C-MoSy-NC cathode. k) Digital photographs of six wearable series batteries in real state, powering the LED array. Reproduced with permission.

Figure 6. a) Schematic synthesis of the MoS/graphene nanocomposites. b) Crystal structures of bulk MoS, and MoS/graphene. c) Zn-ion migration pathways in MoSz/graphene. d) The migration energy barriers of the bulk MoS, and MoSy-to-graphene distance. e) Long-term cycling stability of MoSz/graphene at 1 A g'. f) Schematic diagram of the flexible quasi-solid-state Zn-ion battery. g) Typical voltage curves under the various bending states of the quasi-solid-state MoS/graphene//Zn battery. Reproduced with permission.20 Copyright 2021, Wiley-VCH. h) The optimized diffusion paths of Zn2t in MoSz. i) The calculated energy profiles of Zn2* along the diffusion path in MoSz with different interlayer spacing.

Figure 7. a) Schematic illustration of the preparation processes for the binder-free hierarchical VS2@SS electrode. b) SEM image of the VS@SS electrode. c) Long-term cycling performance of the VS2@SS electrode at 1 and 2 A g-'. d) Long-term cycling performances at 500 and 50 mA g-1 (inset) with a mass loading of 11 mg cm-2. e) Cycling performance of the solid-state battery at 0.5 A g"'. Reproduced with permission.[125) Copyright 2019, RSC.f) Schematic illustration of the synthesis ofVS2@VOOH microflowers. g,h) HRTEM images ofVS2@VOOH-18 h. i) Schematic illustration for the charge/ discharge process of the VS2@VOOH-18 h and the working mechanism of VOOH coating. Reproduced with permission.

Figure 8. a) Illustration of fabrication procedure of hierarchical rGO-VS2 composites. b) FESEM image and c) HRTEM image of rGO-VS2 composites.d) Rate capability and e) cycling performance of rGO-VS2 and VS electrodes. Reproduced with permission.135) Copyright 2020, Elsevier B.V. f) Illustration of synthesis procedure of VS2@N-C hybrid. g) TEM image of the VS2@N-C hybrid. c) Cycling properties of VS2@N-C hybrid. Reproduced with permission.

Figure 9. a) SEM image and b.c) images of VS2/VO, d) Long-term cycle performance and e) rate capability of VS2/VO2 and VSz electrodes. Reproduced with permission.142) Copyright 2021, Wiley-VCH. f) Schematic illustration of the synthesis of interlayer-expanded flower-like VS2-NHs hollow spheres.g) HRTEM image of VS2-NH3. h) The electrochemical oxidation of VS2-NH3 process and the subsequent Zn2+ storage mechanism. Reproduced with permission.

Figure 10. a) HRTEM image of 1T phase WS2-200. b) CV curves of commercial WS2 and WS2-200 at 0.4 mV s-'. c) Cycling performances at 200 mA g-.Reproduced with permission.1147) Copyright 2022, Elsevier B.V. d) HRTEM image and e) the crystallographic structure of TiSz. f) The calculations of the migration energy of Zn2+ ions. g) The long-term cycling properties of Nao.14TiS2 electrode. h) Structural illustrations and i) cycling performance of aqueous Nao.14TiS2//ZnMnO, Zn-ion full battery. Reproduced with permission.

Figure 11. a) Schematic illustration of the Zn storage in VSe. b) HRTEM image of VSey c) Cycling performance of VSe, at a high current density of 2000 mA g". Reproduced with permission.a Copyright 2020, RSC. d) TEM image of VSe, nanosheets with SAED pattern inserted. e) Long-term cycle test of the Zn//VSez battery. f) Schematic illustration of the two-step Zn2" intercalation/de-intercalation process in VSe; cathode. g) Top view of the optimal diffusion pathway of zinc ion. Reproduced with permission.

Figure 12. a) Schematic of the preparation process of the VSez-x-SS. b) SEM image and c,d) HRTEM images of VSe2-y-SS. e) XPS Se 3d spectra and f) EPR spectra of VSe2-x-SS and VSez-SS. g) Long cycling performance. Reproduced with permission.I53] Copyright 2021, American Chemical Society.h) Schematic representation for the synthesis of rGO-VSez nanohybrid. b) Schematic illustration of Zn storage in rGO-VSez nanohybrid. c) TEM images of rGO-VSez nanohybrid. Reproduced with permission.

Figure 13. a) Schematic illustration of preparation WSe, nano-flower. b) HRTEM image of WSe, material. c) Charge-discharge curves of WSe. Reproduced with permission.18) Copyright 2022, Springer-Verlag. d) The structure and storage mechanism of Tisez. e) Proposed diffusion path of site A to site A and site B to site B. The structure and storage mechanism of f) Tisez//VO: ZIB and g) TiSez//AC ZHSC. h) The migration energy of zinc ions at (e). Reproduced with permission.

Figure 14. a) Lateral (left) and vertical (right) views of the crystalline structure of VS,, b) DFT-calculated relative formation energies for different amounts of Zn2* ion occupation in Zn,VSs cells. c) b values of the different redox peaks. d) Galvanostatic charge and discharge curves of the VS4-Zn battery at different current densities. e) Cycle stability of the VSa-Zn battery. Reproduced with permission. 8) Copyright 2020, RSC. f) Low-mag TEM image of VSs@rGO. g) Cycling performance of VS@rGO at 10 A g-'. Reproduced with permission.

Figure 15. a) Schematic of the fabrication procedure of VsSg. b) Schematic of the fabrication procedure of VsSg. c) The diffusion energy barrier profiles in VsSs. Reproduced with permission.192) Copyright 2021, Elsevier B.V. d) Schematic illustration of the formation of the MnS/RGO composites.Reproduced with permission.193] Copyright 2021, Elsevier Inc. e) Advantages of CoSn.S2 compared with CoSnS and Co,Sn.S2. f) The calculated chemical diffusion coefficients for Zn2+ of Co,Sn2-S2- g) Cycling performance at 1 A g'. h) Long-cycle performance of the Zn//Co,SngS battery at -10 °C. Reproduced with permission.

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