锂硫电池的动力学调控策略

doi:10.11949/0438-1157.20221071

摘要/Abstract

摘要：

锂硫（Li-S）电池因其超高的理论能量密度（2600 Wh·kg^-1）有望成为下一代高能量密度电池的候选者之一。然而，它存在硫利用率低、容量衰减快以及多硫化锂（LiPSs）发生“流失效应”等问题，这使得Li-S电池反应动力学缓慢，严重限制了其实际应用。物理限制、化学吸附等方法可以加速硫、LiPSs和Li₂S之间的氧化还原反应，减少LiPSs的流失，加速动力学过程，使电池具有高能量密度和长循环稳定性。基于整体电化学反应过程，对近些年使用的材料如何促进动力学进程、阻止LiPSs的流失，以及相应策略的评价进行了综述，以指导提升电池动力学性能的合理设计和Li-S电池的实际应用。

关键词: 锂硫电池, 动力学, 多硫化锂, 电化学, 吸附, 催化, 流失效应

Abstract:

Lithium-sulfur (Li-S) batteries are expected to be one of the candidates for next-generation high-energy-density batteries because of their ultra-high theoretical energy density (2600 Wh·kg^-1). However, it suffers from low sulfur utilization, rapid capacity fading, and the “lost effect” of lithium polysulfides (LiPSs). These problems make the reaction kinetics of Li-S batteries sluggish, severely limiting their practical applications. Methods such as physical confinement and chemical adsorption can accelerate the redox reaction between sulfur, LiPSs, and Li₂S, reduce the loss of LiPSs, and accelerate the kinetic process, which enable the battery with high energy density and long-cycle stability. Based on the overall electrochemical reaction process, this article reviews how materials used in recent years can facilitate the kinetic process, prevent the loss of LiPSs, and evaluate the corresponding strategies. The purpose of this review is to help guide the rational design of improved battery kinetics and the practical application of Li-S batteries.

Key words: lithium-sulfur batteries, kinetics, lithium polysulfides, electrochemistry, adsorption, catalysis, lost effect

中图分类号:

TM 912.9

焦巡, 童成, 李存璞, 魏子栋. 锂硫电池的动力学调控策略[J]. 化工学报, 2023, 74(1): 170-191.

Xun JIAO, Cheng TONG, Cunpu LI, Zidong WEI. Kinetic regulation strategies in lithium-sulfur batteries[J]. CIESC Journal, 2023, 74(1): 170-191.

图/表 14

图1 （a）Li-S电池的结构示意图；（b）Li-S电池的一般电位分布[12]

Fig.1 (a) Schematic illustration of the construction of a Li-S battery cell; (b) General potential profile of a Li-S battery[12]

图2 （a）制造S-PGC-CFF正极的过程示意图和每个组件的微观结构[46]；（b）CCG底物制备及其相应配置的示意图[48]

Fig.2 (a) Schematic illustration of the procedure for fabricating S-PGC-CFF cathode and the microstructures of each component[46]; (b) Schematic of the CCG substrate preparation and its corresponding configurations[48]

图3 （a）3DG@NPC和3DG@NPC/S的合成过程示意图[55]；（b）Ni@N-CNSs薄膜的制造工艺示意图[56]

Fig.3 (a) Schematic synthesis process of 3DG@NPC and 3DG@NPC/S[55]; (b) Schematic fabrication process of Ni@N-CNSs films[56]

图4 （a）LiPSs与羟基之间相互作用的示意图[57]；（b）Co-NC@TpBD-Me2正极的制备工艺及其作为硫正极的工作机理[58]

Fig.4 (a) Schematic illustration of the interactions between polysulfides and hydroxyl groups[57]; (b) Preparation procedure of Co-NC@TpBD-Me2 cathode and its working mechanism as sulfur cathode[58]

图5 （a）MP的化学结构以及PP-C-St-MP隔膜实现可逆的咬合效果[62]；（b）PDPP改性隔膜的示意图以及其在Li-S电池中作用的效果图[63]；（c）TA-Co隔膜的Li-S电池示意图[64]；（d）具有EVA微球涂层隔膜的Li-S电池示意图[65]

Fig.5 (a) Chemical structure of MP and PP-C-St-MP diaphragm for reversible clinching effect[62]; (b) Schematic diagram of PDPP modified separator and its effect in Li-S battery[63]; (c) Schematic diagram of TA-Co separator in Li-S battery[64]; (d) Schematic illustration of the Li-S battery with EVA microspheres-coated separators[65]

图6 （a）不同金属氧化物与LiPSs的化学反应性作为氧化还原电势与Li/Li+的函数，叠加了典型的Li-S循环伏安曲线（以红色显示）[69]；（b）VO2@rGO/S产品的制造过程示意图[70]；（c）核壳结构中超薄δ-MnO2纳米片的催化转化机理[72]；（d）S/CC@NiCo2O4复合材料的合成步骤示意图，NiCo2O4纳米纤维阵列可以有效吸附和催化LiPSs的转化反应[73]

Fig.6 (a) Chemical reactivity of different metal oxides with LiPSs as a function of redox potential versus Li/Li+, superimposed with a typical Li-S cyclic voltammetry curve (shown in red)[69]; (b) Schematic of the fabrication processes of VO2@rGO/S product[70]; (c) Catalytic conversion mechanism of ultrathin δ-MnO2 nanosheets in the core-shell structure[72]; (d) Schematic of the synthesis steps for the S/CC@NiCo2O4 composite, the NiCo2O4 nanoﬁber arrays can effectively adsorb and catalyze the conversion reaction of LiPSs[73]

图7 （a）S/CoS2-NC复合材料的合成过程示意图[74]；（b）PCN-SnS2复合材料的制备示意图[75]；（c）NiCo2S4/S复合材料合成过程示意图[76]；（d）MoS2@CNF和S@MoS2@CNF复合材料的制备[77]

Fig.7 (a) Schematic illustration of the synthesis process of S/CoS2-NC composites[74]; (b) Schematic illustration of the preparation of PCN-SnS2 composites[75]; (c) Schematic illustration of the synthetic processes of NiCo2S4/S composite[76]; (d) Preparation of MoS2@CNF and S@MoS2@CNF composite[77]

图8 （a）~(c）WN、VN和Mo2N的SEM图[78]；（d）、（e）TiN中空纳米球的SEM图和TEM图[79]

Fig.8 (a)—(c) SEM images of WN, VN and Mo2N[78]; (d), (e) SEM image and TEM image of TiN hollow nanospheres[79]

图9 （a）Ti3C2@CF制备示意图以及作为多功能正极材料改善Li-S电池性能的示意图[80]；（b）S@ZnSe/NHC正极对Li-S电池的作用示意图[81]

Fig.9 (a) Schematic illustration of Ti3C2@CF preparation and as a multifunctional cathode material to ameliorate the performance of Li-S batteries[80]; (b) Schematic diagram of the effect of S@ZnSe/NHC cathode on Li-S batteries[81]

图10 （a）~（c）钙钛矿促进剂对工作中Li-S电池中LiPSs抑制和Li2S调节的作用及Ba0.5Sr0.5Co0.8Fe0.2O3-δ PrNP的晶体结构[82]；（d）Li2S在常规导电表面（左）和具有均匀分布的成核位点的导电与催化纳米三相界面（右）上成核和生长的示意图[83]；（e）LiPSs氧化还原反应和Li2S成核示意图[83]

Fig.10 (a)—(c) The role of perovskite promoter on LiPSs suppression and Li2S regulation in a working Li-S battery and the crystal structure of Ba0.5Sr0.5Co0.8Fe0.2O3-δ PrNP[82]; (d) Schematic illustration of the Li2S nucleation and growth on routine conductive surface (left) and on conductive and catalytic nanotriple-phase interface with uniformly distributed nucleation sites (right)[83]; (e) Schematic illustration of polysulfide redox reaction and Li2S nucleation[83]

图11 Li2S6 LiPSs吸附试验：（a）候选材料的光学照片；（b）无候选材料的DOL/DME溶液中不同浓度Li2S6的UV-Vis数据；（c）、(d）候选材料添加到3.0 mmol·L-1 Li2S6中的UV-Vis数据[84]

Fig.11 Li2S6 polysulfide adsorption test: (a) Optical photos of candidate materials; (b) UV-Vis data of varying concentrations of Li2S6 in DOL/DME solution without candidate materials; (c), (d) UV-Vis data of candidate materials added in 3.0 mmol·L-1 Li2S6[84]

图12 Li-S电池在0.2 C第2次循环的GITT测试结果

Fig.12 GITT results for Li-S battery at 0.2 C on 2nd cycle

图13 MoO2（a）、α-MoC（b）和MoO2/α-MoC（c）在2.09 V时的无量纲瞬态曲线；MoO2、α-MoC和MoO2/α-MoC电极放电到最大电流[（d）~(f）]和Li2S沉积后[（g）~(i）]的SEM图像[89]

Fig.13 Dimensionless transient profiles of MoO2 (a), α-MoC (b) and MoO2/α-MoC (c) at 2.09 V; SEM images of MoO2, α-MoC and, MoO2/α-MoC electrodes after discharged to maximum current [(d)—(f)] and after Li2S deposition [(g)—(i)][89]

图14 （a）液相LiPSs被Co9S8强烈吸附，因此不能转移到MoS2上以实现快速转化；（b）硫空位可以协调组分的化学吸附以均匀吸附LiPSs；（c）~(e）CMG-L、CMG-M和CMG-H在1.6~2.8 V电压范围内不同扫描速率下的CV曲线；（f）CMG-L、CMG-M和CMG-H在不同扫描速度下的NTR值；（g）CMG-L、CMG-M和CMG-H在0.5 C下的长循环性能图[91]

Fig.14 (a) Liquid-phase LiPSs are strongly adsorbed by Co9S8 and therefore cannot be transferred to MoS2 to accomplish fast conversion; (b) Sulfur vacancies can harmonize the chemisorption of components to uniformly adsorb LiPSs; (c)—(e) CV curves within the voltage range of 1.6—2.8 V at different sweep rates of CMG-L, CMG-M and CMG-H; (f) The NTR values of CMG-L, CMG-M and CMG-H at different sweep rates; (g) Long cycle performances of CMG-L, CMG-M and CMG-H at 0.5 C[91]

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