Research progress on the interface interaction between alloys and electrolytes in potassium-ion batteries
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摘要: 近年来，钾离子电池（KIBs）因钾元素丰度高、氧化还原电位低等优势受到越来越多的关注。负极是电池的重要组成部分之一，直接影响着电池的安全性、稳定性和能量密度。其中，合金负极基于多电子反应机制能够提供较高的理论比容量，有望提升全电池的能量密度。此外，其储钾电位远离了金属钾的沉积/析出电位，保证了电池的安全性。然而，（去）合金化过程中剧烈的体积波动会引起电极材料的破裂和粉化，进而导致容量快速衰减。优化电解液构筑稳定的电极–电解液界面是一种切实有效稳定合金负极结构的方法，主要包括：调控固体电解质膜的组分、调节钾离子的溶剂化结构、利用溶剂对电极的化学吸附作用等。它具备工艺简单、成本低廉等优点。本文综述了近年来钾离子电池合金负极与电解液界面作用的相关研究进展，总结了电解液的优化策略，分析了合金负极的储钾机制和电化学性能，重点阐述了合金负极与电解液的界面作用机制，并对未来钾离子电池电解液的发展提供了新的见解与思路。Abstract: Developing new energy, reducing fossil energy consumption, and building a green and low-carbon energy system are important strategies to achieve carbon neutrality. To realize the grid connection of new energy generation, rechargeable potassium-ion batteries (KIBs) are expected to be used in large-scale energy storage, considering sufficient potassium resources and potential high-energy density. Anode, an essential battery component, directly determines the battery safety, cycle life, and energy density. Among various anodes, alloys can provide high theoretical specific capacity based on the multi-electron reaction mechanism, which is promising in terms of improving the energy density of a full battery. Their K-storage voltages also stay away from the deposition/stripping potentials of metallic K, thereby enhancing battery safety. However, the dramatic volume variation upon alloying and dealloying leads to electrode pulverization and capacity fading in traditional carbonate-based electrolytes. An effective method for stabilizing an alloy-based anode structure is the construction of a stable electrode–electrolyte interface by electrolyte optimization, which has the advantages of a simple process and low cost. Accordingly, the utilization of interfacial engineering to achieve stable alloy anodes has been frequently reported in the past few years. This topic includes the following: (1) regulation of the components of solid electrolyte interphase (SEI) layers to improve mechanical strength and ionic conductivity, buffer volume fluctuation, and reduce electrode corrosion; (2) adjustment of the solvated structure of K+ to enhance the diffusion rate and inhibit the electrolyte decomposition; and (3) utilization of solvent molecular chemisorption on the electrode to induce its microstructure change, improve the electrolyte wetting ability, and relieve volume change. The SEI is a passivation film generated on the electrode surface at the initial battery operation stage. Research on its structure, component, and formation mechanism is still basic due to its instability and complexity and limited research methods. Whether the solvated structure of cation and electrolyte adsorption affect the SEI structure and composition remains unclear. How the solvated structure and the electrolyte adsorption improve the electrode stability must also be further studied. This review covers recent research progress on the interfacial interaction between alloy anodes and electrolytes in KIBs, summarizes the electrolyte optimization strategies, analyzes the potassium storage mechanisms and electrochemical performance of alloy anodes, and highlights the interfacial interaction mechanisms. More importantly, this paper provides new insights for the future development of KIB electrolytes.
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Key words:
- potassium-ion batteries /
- alloy anodes /
- electrolytes /
- interfacial interaction /
- K-storage mechanisms
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图 3 (a) K+–溶剂和钾盐–溶剂的溶剂化能；(b)K+–溶剂和钾盐–溶剂的HOMO与LUMO能级；(c)1.0 mol·L−1 KFSI/EC+DEC和(d)1.0 mol·L−1 KFSI /DME电解液中RP/C循环10周后的SEM图[71]
Figure 3. (a) Solvation energies of the K+–solvent and K salt–solvent complexes; (b) HOMO and LUMO energy levels of the K+–solvent and K salt–solvent complexes; SEM images of RP/C after 10 cycles in (c) 1.0 mol·L−1 KFSI/EC+DEC and (d) 1.0 mol·L−1 KFSI /DME[71]
图 4 （a）BP/G电极在NCE、HCE和LHCE等电解液中的循环性能；（b）BP/G电极在HCE和LHCE中的离子扩散系数；（c）不同电解液中P和S元素的原子百分比;BP/G电极在LHCE中循环300周后的（d）TEM图以及相应的（e）EDS图谱[74]
Figure 4. (a) Cyclic performance of the BP/G electrodes in the NCE, HCE, and LHCE; (b) diffusion coefficients of K+ in the HCE and LHCE; (c) atomic percentage of the P and S elements in different electrolytes; (d) TEM image of the BP/G electrodes after 300 cycles in the LHCE and corresponding (e) EDS spectra[74]
图 5 （a）Sn4P3在KIBs中循环50周的TEM图像[83]；（b）Sn4P3在KIBs中循环50周后的C1s XPS图谱[83]；（c）K+在Sn、Li2Sn5和LiSn3晶体中的扩散能垒，Li+在Sn晶体中的扩散能垒[85]；（d）含20%–100% Li原子的钾基全电池电解液的EIS图[85]
Figure 5. (a) TEM image of Sn4P3 after 50 cycles in the KIBs[83]; (b) C1s XPS spectrum of Sn4P3 in the KIBs after 50 cycles[83]; (c) diffusion energy barriers of K+ in Sn, Li2Sn5, LiSn3, and Li+ in the Sn crystals[85]; (d) EIS plots of the potassium-based full batteries electrolyte containing 20%–100% Li atoms[85]
图 6 （a）原始Sb电极的SEM图；（b）Sb负极在4.0 mol·L−1 KFSI/DME中循环30周后的SEM图；（c）Sb负极在1.0 mol·L−1 KFSI/EC+EMC中循环30周后的SEM图；（d）Sb电极在不同电解液中循环时的阻抗对比图；（e）K+–溶剂–阴离子络合物的HOMO'–LUMO能级差(ΔE)((1)—K+–DME–FSI–；(2)—K+–2DME–FSI–；(3)—K+–EC–FSI–；(4)—K+–DME–TFSI–)；(f)KFSI和不同电解液的拉曼光谱，以及K+、FSI–与溶剂分子之间相互作用的示意图[61]
Figure 6. (a) SEM image of the pristine Sb electrode; (b) SEM image of Sb anode after 30 cycles in 4.0 mol·L−1 KFSI DME; (c) SEM image of Sb anode after 30 cycles in 1.0 mol·L−1 KFSI EC+EMC; (d) impedance values of Sb electrodes when cycled in different electrolytes; (e) HOMO′–LUMO energy level differences (ΔE) of the K+–solvent–anion complexes ((1)—K+–DME–FSI−; (2)—K+–2DME–FSI−; (3)—K+–EC–FSI−; (4)—K+–DME–TFSI−); (f) Raman spectra of the KFSI and different electrolytes and corresponding illustrations of the interaction among K+, FSI−, and solvents[61]
图 7 （a0原始、（b）1周、（c）10周和（d）70周循环次数下的SEM图及DME分子在Bi表面上的三种吸附模型及吸附能. （e）桥位；（f）顶位；（g）穴位[62]
Figure 7. SEM images of the Bi electrodes after (a) pristine; (b) 1st; (c) 10th; (d) 70th different cycles and three adsorption models of the DME molecules on the Bi surface and corresponding adsorption energies: (e) bridge; (f) top; (g) hollow[62]
图 8 （a）合金负极表面SEI膜的形成示意图[63]；（b）Bi/rGO负极在KPF6电解液中循环10周后的TEM图[100]；（c）Bi/rGO电极在KFSI电解液中循环10周后的TEM图(插图是放大后的TEM图)[100]
Figure 8. (a) Illustration of the SEI film formation on the alloy anode surface[63]; (b) TEM image of Bi/rGO in the KPF6-based electrolyte after 10 cycles[100]; (c) TEM image of Bi/rGO in the KFSI–based electrolyte after 10 cycles (Inset: corresponding enlarged TEM image)[100]
图 9 （a） Si–石墨烯电极的充放电曲线[103]；（b）纯Si电极的充放电曲线[103]；（c）Si–石墨烯电极首周放电和充电的XRD谱图[103]；（d）EC+DEC基电解液在Na–K/石墨和K/石墨电池中析出/沉积钾后的1H-NMR谱图(插图显示了DEC对应的峰强度变化)[105]
Figure 9. (a) Selected charge–discharge curves of the Si–graphene electrode[103]; (b) selected charge–discharge curves of the pure Si electrode[103]; (c) XRD patterns of the initial discharged and charged Si–graphene electrodes[103]; (d) 1H-NMR spectra of the EC/DEC-based electrolytes in Na–K/graphite and K/graphite cells upon potassiation/depotassiation (Inset: corresponding intensity change of the peaks in the DEC solvents)[105]
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