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1.
Qian-Kui Zhang Shu-Yu Sun Dr. Ming-Yue Zhou Li-Peng Hou Jia-Lin Liang Shi-Jie Yang Dr. Bo-Quan Li Dr. Xue-Qiang Zhang Prof. Jia-Qi Huang 《Angewandte Chemie (International ed. in English)》2023,62(42):e202306889
The stability of high-energy-density lithium metal batteries depends on the uniformity of solid electrolyte interphase (SEI) on lithium metal anodes. Rationally improving SEI uniformity is hindered by poorly understanding the effect of structure and components of SEI on its uniformity. Herein, a bilayer structure of SEI formed by isosorbide dinitrate (ISDN) additives in localized high-concentration electrolytes was demonstrated to improve SEI uniformity. In the bilayer SEI, LiNxOy generated by ISDN occupies top layer and LiF dominates bottom layer next to anode. The uniformity of lithium deposition is remarkably improved with the bilayer SEI, mitigating the consumption rate of active lithium and electrolytes. The cycle life of lithium metal batteries with bilayer SEI is three times as that with common anion-derived SEI under practical conditions. A prototype lithium metal pouch cell of 430 Wh kg−1 undergoes 173 cycles. This work demonstrates the effect of a reasonable structure of SEI on reforming SEI uniformity. 相似文献
2.
Dr. Dechao Zhang Dr. Yuxuan Liu Zhaoyu Sun Dr. Zhengbo Liu Dr. Xijun Xu Lei Xi Prof. Shaomin Ji Prof. Min Zhu Prof. Jun Liu 《Angewandte Chemie (International ed. in English)》2023,62(44):e202310006
The deployment of lithium metal anode in solid-state batteries with polymer electrolytes has been recognized as a promising approach to achieving high-energy-density technologies. However, the practical application of the polymer electrolytes is currently constrained by various challenges, including low ionic conductivity, inadequate electrochemical window, and poor interface stability. To address these issues, a novel eutectic-based polymer electrolyte consisting of succinonitrile (SN) and poly (ethylene glycol) methyl ether acrylate (PEGMEA) is developed. The research results demonstrate that the interactions between SN and PEGMEA promote the dissociation of the lithium difluoro(oxalato) borate (LiDFOB) salt and increase the concentration of free Li+. The well-designed eutectic-based PAN1.2-SPE (PEGMEA: SN=1: 1.2 mass ratio) exhibits high ionic conductivity of 1.30 mS cm−1 at 30 °C and superior interface stability with Li anode. The Li/Li symmetric cell based on PAN1.2-SPE enables long-term plating/stripping at 0.3 and 0.5 mA cm−2, and the Li/LiFePO4 cell achieves superior long-term cycling stability (capacity retention of 80.3 % after 1500 cycles). Moreover, Li/LiFePO4 and Li/LiNi0.6Co0.2Mn0.2O2 pouch cells employing PAN1.2-SPE demonstrate excellent cycling and safety characteristics. This study presents a new pathway for designing high-performance polymer electrolytes and promotes the practical application of high-stable lithium metal batteries. 相似文献
3.
Tuoya Naren Gui-Chao Kuang Ruheng Jiang Piao Qing Hao Yang Jialin Lin Yuejiao Chen Weifeng Wei Xiaobo Ji Libao Chen 《Angewandte Chemie (International ed. in English)》2023,62(26):e202305287
Lithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li metal batteries (LMBs). However, Li dendrite formation on the anode impedes the proper discharge capacity and practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St-MaI) containing carboxylic acid and cyclic ether moieties which would in situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes and maintain good interfacial contact. The presence of carboxylic acid and cyclic ether pendant groups greatly contribute to the induction of uniform Li ion deposition. In addition, the presence of benzyl rings makes the polymer have a certain mechanical strength and plays a key role in inhibiting the growth of Li dendrites. As a result, the symmetric Li||Li cell with P(St-MaI)@Li layer can stably cycle for over 900 h under 1 mA cm−2 without polarization voltage increasing, while their Li||LiFePO4 full batteries maintain high capacity retention of 96 % after 930 cycles at 1C in carbonate electrolytes. The innovative strategy of artificial SEI is broadly applicable in designing new materials to inhibit Li dendrite growth on Li metal anodes. 相似文献
4.
Chao Wang Xiaoxue Zhao Dabing Li Dr. Chong Yan Qiang Zhang Li-Zhen Fan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(19):e202317856
In solid-state lithium metal batteries (SSLMBs), the inhomogeneous electrolyte-electrode interphase layer aggravates the interfacial stability, leading to discontinuous interfacial ion/charge transport and continuous degradation of the electrolyte. Herein, we constructed an anion-modulated ionic conductor (AMIC) that enables in situ construction of electrolyte/electrode interphases for high-voltage SSLMBs by exploiting conformational transitions under multiple interactions between polymer and lithium salt anions. Anions modulate the decomposition behavior of supramolecular poly (vinylene carbonate) (PVC) at the electrode interface by changing the spatial conformation of the polymer chains, which further enhances ion transport and stabilizes the interfacial morphology. In addition, the AMIC weakens the “Li+-solvation” and increases Li+ vehicle sites, thereby enhancing the lithium-ion transport number (tLi+=~0.67). Consequently, Li || LiNi0.8Co0.1Mn0.1O2 cell maintains about 85 % capacity retention and Coulombic efficiency >99.8 % in 200 cycles at a charge cut-off voltage of 4.5 V. This study provides a new understanding of lithium salt anions regulating polymer chain segment behavior in the solid-state polymer electrolyte (SPE) and highlights the importance of the ion environment in the construction of interfacial phases and ionic conduction. 相似文献
5.
Chuangchao Sun Ruhong Li Suting Weng Chunnan Zhu Long Chen Sen Jiang Long Li Xuezhang Xiao Chengwu Liu Lixin Chen Tao Deng Xuefeng Wang Xiulin Fan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(19):e202400761
Lithium batteries employing Li or silicon (Si) anodes hold promise for the next-generation energy storage systems. However, their cycling behavior encounters rapid capacity degradation due to the vulnerability of solid electrolyte interphases (SEIs). Though anion-derived SEIs mitigate this degradation, the unavoidable reduction of solvents introduces heterogeneity to SEIs, leading to fractures during cycling. Here, we elucidate how the reductive stability of solvents, dominated by the electrophilicity (EPT) and coordination ability (CDA), delineates the SEI formed on Li or Si anodes. Solvents exhibiting lower EPT and CDA demonstrate enhanced tolerance to reduction, resulting in inorganic-rich SEIs with homogeneity. Guided by these criteria, we synthesized three promising solvents tailored for Li or Si anodes. The decomposition of these solvents is dictated by their EPTs under similar solvation structures, imparting distinct characteristics to SEIs and impacting battery performance. The optimized electrolyte, 1 M lithium bis(fluorosulfonyl)imide (LiFSI) in N-Pyrrolidine-trifluoromethanesulfonamide (TFSPY), achieves 600 cycles of Si anodes with a capacity retention of 81 % (1910 mAh g−1). In anode-free Cu||LiNi0.5Co0.2Mn0.3O2 (NCM523) pouch cells, this electrolyte sustains over 100 cycles with an 82 % capacity retention. These findings illustrate that reducing solvent decomposition benefits SEI formation, offering valuable insights for the designing electrolytes in high-energy lithium batteries. 相似文献
6.
Reversible Li Plating on Graphite Anodes through Electrolyte Engineering for Fast-Charging Batteries
Xinyang Yue Jing Zhang Yongteng Dong Yuanmao Chen Zhangqin Shi Xuejiao Xu Xunlu Li Prof. Zheng Liang 《Angewandte Chemie (International ed. in English)》2023,62(19):e202302285
The difficulties to identify the rate-limiting step cause the lithium (Li) plating hard to be completely avoided on graphite anodes during fast charging. Therefore, Li plating regulation and morphology control are proposed to address this issue. Specifically, a Li plating-reversible graphite anode is achieved via a localized high-concentration electrolyte (LHCE) to successfully regulate the Li plating with high reversibility over high-rate cycling. The evolution of solid electrolyte interphase (SEI) before and after Li plating is deeply investigated to explore the interaction between the lithiation behavior and electrochemical interface polarization. Under the fact that Li plating contributes 40 % of total lithiation capacity, the stable LiF-rich SEI renders the anode a higher average Coulombic efficiency (99.9 %) throughout 240 cycles and a 99.95 % reversibility of Li plating. Consequently, a self-made 1.2-Ah LiNi0.5Mn0.3Co0.2O2 | graphite pouch cell delivers a competitive retention of 84.4 % even at 7.2 A (6 C) after 150 cycles. This work creates an ingenious bridge between the graphite anode and Li plating, for realizing the high-performance fast-charging batteries. 相似文献
7.
Electron Delocalization Enables Sulfone-based Single-solvent Electrolyte for Lithium Metal Batteries
Muhammad Mominur Rahman Enyuan Hu 《Angewandte Chemie (International ed. in English)》2023,62(44):e202311051
Li-metal batteries (LMB), although providing high energy density, face the grand challenge of identifying good electrolyte solvents for cycling. Common solvents are either only stable against lithium metal anode or only stable against LiNixMnyCo1-x-yO2 (NMC) cathode. There is significant effort trying to increase the cathode stability for ether electrolytes, which are in general stable against lithium metal anode. In comparison, there is much less effort trying to increase the anode stability of electrolytes that are stable against NMC cathode. One example is the sulfone-based electrolyte. It has good cathode stability but is hindered from practical application because of (1) high viscosity and poor wetting capability and (2) poor anode stability. Here, we solve these issues by modifying the sulfone molecules using resonance and electron withdrawing effect. The viscosity is significantly reduced by delocalizing the electrons through introducing additional oxygen on the molecular backbone and applying appropriate fluorination. The resulting molecule 2,2,2-trifluoroethyl mesylate (TFEM) has decreased Lewis basicity and less reactivity toward Li+. The electrolyte based on TFEM as single solvent enables cycling of LMB under harsh conditions of low N/P ratio (21 mg/cm2 NMC811 and 50 μm Li) with 90 % capacity retention after 160 cycles at C/3 discharge rate. 相似文献
8.
Zehui Sun Yuankun Wang Shenyu Shen Xinyang Li Prof. Xiaofei Hu Prof. Mingyou Hu Prof. Yaqiong Su Prof. Shujiang Ding Prof. Chunhui Xiao 《Angewandte Chemie (International ed. in English)》2023,62(41):e202309622
Controlling lithium (Li) electrocrystallization with preferred orientation is a promising strategy to realize highly reversible Li metal batteries (LMBs) but lack of facile regulation methods. Herein, we report a high-flux solid electrolyte interphase (SEI) strategy to direct (110) preferred Li deposition even on (200)-orientated Li substrate. Bravais rule and Curie-Wulff principle are expanded in Li electrocrystallization process to decouple the relationship between SEI engineering and preferred crystal orientation. Multi-spectroscopic techniques combined with dynamics analysis reveal that the high-flux CF3Si(CH3)3 (F3) induced SEI (F3-SEI) with high LiF and −Si(CH3)3 contents can ingeniously accelerate Li+ transport dynamics and ensure the sufficient Li+ concentration below SEI to direct Li (110) orientation. The induced Li (110) can in turn further promote the surface migration of Li atoms to avoid tip aggregation, resulting in a planar, dendrite-free morphology of Li. As a result, our F3-SEI enables ultra-long stability of Li||Li symmetrical cells for more than 336 days. Furthermore, F3-SEI modified Li can significantly enhance the cycle life of Li||LiFePO4 and Li||NCM811 coin and pouch full cells in practical conditions. Our crystallographic strategy for Li dendrite suppression paves a path to achieve reliable LMBs and may provide guidance for the preferred orientation of other metal crystals. 相似文献
9.
Jing Chen Xuetian Deng Yiyang Gao Yuanjun Zhao Xiangpeng Kong Qiang Rong Junqiao Xiong Demei Yu Shujiang Ding 《Angewandte Chemie (International ed. in English)》2023,62(35):e202307255
All-solid-state lithium metal batteries (LMBs) are considered as the promising higher-energy and improved-safety energy-storage systems. Nevertheless, the electrolyte-electrodes interfacial issues due to the limited solid physical contact lead to discontinuous interfacial charge transport and large interfacial resistance, thereby suffering from unsatisfactory electrochemical performance. Herein, we construct an integrated cathode/polymer electrolyte for all-solid-state LMBs under the action of polymer chains exchange and recombination originating from multiple dynamic bonds in our well-designed dynamic supramolecular ionic conductive elastomers (DSICE) molecular structure. The DSICE acts as polymer electrolytes with excellent electrochemical performance and mechanical properties, achieving the ultrathin pure polymer electrolyte thickness (12 μm). Notably, the DSICE also functions as lithium iron phosphate (LiFePO4, LFP) cathode binders with enhanced adhesive capability. Such well-constructed Li|DSICE|LFP-DSICE cells generate delicate electrolyte-electrodes interfacial contact at the molecular level, providing continuous Li+ transport pathways and promoting uniform Li+ deposition, further delivering superior long-term charge/discharge stability (>600 cycles, Coulombic efficiency, >99.8 %) and high capacity retention (80 % after 400 cycles). More practically, the Li|DSICE|LFP-DSICE pouch cells show stable electrochemical performance, excellent flexibility and safety under abusive tests. 相似文献
10.
Shunqiang Chen JiaJia Fan Zhuangzhuang Cui Lijiang Tan Digen Ruan Xin Zhao Jinyu Jiang Prof. Shuhong Jiao Prof. Xiaodi Ren 《Angewandte Chemie (International ed. in English)》2023,62(23):e202219310
Albeit ethers are favorable electrolyte solvents for lithium (Li) metal anode, their inferior oxidation stability (<4.0 V vs. Li/Li+) is problematic for high-voltage cathodes. Studies of ether electrolytes have been focusing on the archetype glyme structure with ethylene oxide moieties. Herein, we unveil the crucial effect of ion coordination configuration on oxidation stability by varying the ether backbone structure. The designed 1,3-dimethoxypropane (DMP, C3) forms a unique six-membered chelating complex with Li+, whose stronger solvating ability suppresses oxidation side reactions. In addition, the favored hydrogen transfer reaction between C3 and anion induces a dramatic enrichment of LiF (a total atomic ratio of 76.7 %) on the cathode surface. As a result, the C3-based electrolyte enables greatly improved cycling of nickel-rich cathodes under 4.7 V. This study offers fundamental insights into rational electrolyte design for developing high-energy-density batteries. 相似文献
11.
Dr. Xu Liu Dr. Alessandro Mariani Dr. Thomas Diemant Dr. Xu Dong Po-Hua Su Prof. Stefano Passerini 《Angewandte Chemie (International ed. in English)》2023,62(31):e202305840
Lithium metal is a promising anode material for next-generation high-energy-density batteries but suffers from low stripping/plating Coulombic efficiency and dendritic growth particularly at sub-zero temperatures. Herein, a poorly-flammable, locally concentrated ionic liquid electrolyte with a wide liquidus range extending well below 0 °C is proposed for low-temperature lithium metal batteries. Its all-anion Li+ solvation and phase-nano-segregation solution structure are sustained at low temperatures, which, together with a solid electrolyte interphase rich in inorganic compounds, enable dendrite-free operation of lithium metal anodes at −20 °C and 0.5 mA cm−2, with a Coulombic efficiency of 98.9 %. As a result, lithium metal batteries coupling thin lithium metal anodes (4 mAh cm−2) and high-loading LiNi0.8Co0.15Al0.05O2 cathodes (10 mg cm−2) retain 70 % of the initial capacity after 100 cycles at −20 °C. These results, as a proof of concept, demonstrate the applicability of locally concentrated ionic liquid electrolytes for low-temperature lithium metal batteries. 相似文献
12.
Na Yang Yujie Cui Hang Su Jiaying Peng Yongzheng Shi Jin Niu Feng Wang 《Angewandte Chemie (International ed. in English)》2023,62(28):e202304339
Although high ionic conductivities have been achieved in most solid-state electrolytes used in lithium metal batteries (LMBs), rapid and stable lithium-ion transport between solid-state electrolytes and lithium anodes remains a great challenge due to the high interfacial impedances and infinite volume changes of metallic lithium. In this work, a chemical vapor-phase fluorination approach is developed to establish a lithiophilic surface on rubber-derived electrolytes, which results in the formation of a resilient, ultrathin, and mechanically integral LiF-rich layer after electrochemical cycling. The resulting ultraconformal layer chemically connects the electrolyte and lithium anode and maintains dynamic contact during operation, thus facilitating rapid and stable lithium-ion transport across interfaces, as well as promoting uniform lithium deposition and inhibiting side reactions between electrolyte components and metallic lithium. LMBs containing the novel electrolyte have an ultralong cycling life of 2500 h and deliver a high critical current density of 1.1 mA cm−2 in lithium symmetric cells as well as showing good stability over 300 cycles in a full cell. 相似文献
13.
Dr. Yuankun Wang Zhiming Li Dr. Weiwei Xie Dr. Qiu Zhang Zhenkun Hao Chunyu Zheng Jinze Hou Dr. Yong Lu Dr. Zhenhua Yan Prof. Qing Zhao Prof. Jun Chen 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(6):e202310905
Electrolytes that can keep liquid state are one of the most important physical metrics to ensure the ions transfer with stable operation of rechargeable lithium-based batteries at a wide temperature window. It is generally accepted that strong polar solvents with high melting points favor the safe operation of batteries above room temperatures but are susceptible to crystallization at low temperatures (≤−40 °C). Here, a crystallization limitation strategy was proposed to handle this issue. We demonstrate that, although the high melting points of ethylene sulfite (ES, −17 °C) and fluoroethylene carbonate (FEC, ≈23 °C), their mixtures can avoid crystallization at low temperatures, which can be attributed to low intermolecular interactions and altered molecular motion dynamics. A suitable ES/FEC ratio (10 % FEC) can balance the bulk and interface transport of ions, enabling LiNi0.8Mn0.1Co0.1O2||lithium (NCM811||Li) full cells to deliver excellent temperature resilience and cycling stability over a wide temperature range from −50 °C to +70 °C. More than 66 % of the capacity retention was achieved at −50 °C compared to room temperature. The NCM811||Li pouch cells exhibit high cycling stability under realistic conditions (electrolyte weight to cathode capacity ratio (E/C)≤3.5 g Ah−1, negative to positive electrode capacity ratio (N/P)≤1.09) at different temperatures. 相似文献
14.
Dr. Hang-Yu Zhou Yu Ou Shuai-Shuai Yan Dr. Jin Xie Pan Zhou Lei Wan Zi-Ang Xu Dr. Feng-Xiang Liu Dr. Wei-Li Zhang Dr. Yin-Chun Xia Prof. Kai Liu 《Angewandte Chemie (International ed. in English)》2023,62(35):e202306948
Improved durability, enhanced interfacial stability, and room temperature applicability are desirable properties for all-solid-state lithium metal batteries (ASSLMBs), yet these desired properties are rarely achieved simultaneously. Here, in this work, it is noticed that the huge resistance at Li metal/electrolyte interface dominantly impeded the normal cycling of ASSLMBs especially at around room temperature (<30 °C). Accordingly, a supramolecular polymer ion conductor (SPC) with “weak solvation” of Li+ was prepared. Benefiting from the halogen-bonding interaction between the electron-deficient iodine atom (on 1,4-diiodotetrafluorobenzene) and electron-rich oxygen atoms (on ethylene oxide), the O-Li+ coordination was significantly weakened. Therefore, the SPC achieves rapid Li+ transport with high Li+ transference number, and importantly, derives a unique Li2O-rich SEI with low interfacial resistance on lithium metal surface, therefore enabling stable cycling of ASSLMBs even down to 10 °C. This work is a new exploration of halogen-bonding chemistry in solid polymer electrolyte and highlights the importance of “weak solvation” of Li+ in the solid-state electrolyte for room temperature ASSLMBs. 相似文献
15.
Huili Peng Chunting Wang Dongdong Wang Xinxin Song Chenghui Zhang Jian Yang 《Angewandte Chemie (International ed. in English)》2023,62(34):e202308068
Zn metal as one of the promising anodes of aqueous batteries possesses notable advantages, but it faces severe challenges from severe side reactions and notorious dendrite growth. Here, ultrathin nanosheets of α-zirconium phosphate (ZrP) are explored as an electrolyte additive. The nanosheets not only create a dynamic and reversible interphase on Zn but also promote the Zn2+ transportation in the electrolyte, especially in the outer Helmholtz plane near ZrP. Benefited from the enhanced kinetics and dynamic interphase, the pouch cells of Zn||LiMn2O4 using this electrolyte remarkably improve electrochemical performance under harsh conditions, i.e. Zn powders as the Zn anode, high mass loading, and wide temperatures. The results expand the materials available for this dynamic interphase, provide an insightful understanding of the enhanced charge transfer in the electrolyte, and realize the combination of dynamic interphase and enhanced kinetics for all-climate performance. 相似文献
16.
Haikuo Zhang Ruhong Li Long Chen Yingzhu Fan Hao Zhang Ruixin Zhang Lei Zheng Junbo Zhang Shouhong Ding Yongjian Wu Baochen Ma Shuoqing Zhang Dr. Tao Deng Prof. Lixin Chen Prof. Yanbin Shen Prof. Xiulin Fan 《Angewandte Chemie (International ed. in English)》2023,62(11):e202218970
Although great progress has been made in new electrolytes for lithium metal batteries (LMBs), the intrinsic relationship between electrolyte composition and cell performance remains unclear due to the lack of valid quantization method. Here, we proposed the concept of negative center of electrostatic potential (NCESP) and Mayer bond order (MBO) to describe solvent capability, which highly relate to solvation structure and oxidation potential, respectively. Based on established principles, the selected electrolyte with 1.7 M LiFSI in methoxytrimethylsilane (MOTMS)/ (trifluoromethyl)trimethylsilane (TFMTMS) shows unique hyperconjugation nature to stabilize both Li anode and high-voltage cathode. The 4.6 V 30 μm Li||4.5 mAh cm−2 lithium cobalt oxide (LCO) (low N/P ratio of 1.3) cell with our electrolyte shows stable cycling with 91 % capacity retention over 200 cycles. The bottom-up design concept of electrolyte opens up a general strategy for advancing high-voltage LMBs. 相似文献
17.
Tao Song Dr. Da Wang Prof. Hongxia Wang Dr. Jia Yu Prof. Siqi Shi 《Angewandte Chemie (International ed. in English)》2023,62(31):e202305004
Integrating the advantages of both inorganic ceramic and organic polymer solid-state electrolytes, small-molecule solid-state electrolytes represented by LiI-3-hydroxypropionitrile (LiI-HPN) inorganic–organic hybrid systems possess good interfacial compatibility and high modulus. However, their lack of intrinsic Li+ conduction ability hinders potential application in lithium metal batteries until now, despite containing LiI phase composition. Herein, inspired by evolution tendency of ionic conduction behaviors together with first-principles molecular dynamics simulations, we propose a stepped-amorphization strategy to break the Li+ conduction bottleneck of LiI-HPN. It involves three progressive steps of composition (LiI-content increasing), time (long-time standing), and temperature (high-temperature melting) regulations, to essentially construct a small-molecule-based composite solid-state electrolyte with intensified amorphous degree, which realizes efficient conversion from an I− to Li+ conductor and improved conductivity. As a proof, the stepped-optimized LiI-HPN is successfully operated in lithium metal batteries cooperated with Li4Ti5O12 cathode to deliver considerable compatibility and stability over 250 cycles. This work not only clarifies the ionic conduction mechanisms of LiI-HPN inorganic–organic hybrid systems, but also provides a reasonable strategy to broaden the application scenarios of highly compatible small-molecule solid-state electrolytes. 相似文献
18.
Dr. Enhui Wang Dr. Jing Wan Prof. Dr. Yu-Jie Guo Prof. Dr. Qianyu Zhang Wei-Huan He Chao-Hui Zhang Dr. Wan-Ping Chen Prof. Dr. Hui-Juan Yan Prof. Dr. Ding-Jiang Xue Dr. Tiantian Fang Prof. Dr. Fuyi Wang Prof. Dr. Rui Wen Prof. Dr. Sen Xin Prof. Dr. Ya-Xia Yin Prof. Dr. Yu-Guo Guo 《Angewandte Chemie (International ed. in English)》2023,62(4):e202216354
The interfacial stability is highly responsible for the longevity and safety of sodium ion batteries (SIBs). However, the continuous solid-electrolyte interphase(SEI) growth would deteriorate its stability. Essentially, the SEI growth is associated with the electron leakage behavior, yet few efforts have tried to suppress the SEI growth, from the perspective of mitigating electron leakage. Herein, we built two kinds of SEI layers with distinct growth behaviors, via the additive strategy. The SEI physicochemical features (morphology and componential information) and SEI electronic properties (LUMO level, band gap, electron work function) were investigated elaborately. Experimental and calculational analyses showed that, the SEI layer with suppressed growth delivers both the low electron driving force and the high electron insulation ability. Thus, the electron leakage is mitigated, which restrains the continuous SEI growth, and favors the interface stability with enhanced electrochemical performance. 相似文献
19.
Ran He Dr. Kuirong Deng Dr. Daize Mo Xiongcong Guan Dr. Yuanyuan Hu Prof. Kai Yang Prof. Zhenhua Yan Haijiao Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(7):e202317176
High-energy Li metal batteries (LMBs) consisting of Li metal anodes and high-voltage cathodes are promising candidates of the next generation energy-storage systems owing to their ultrahigh energy density. However, it is still challenging to develop high-voltage nonflammable electrolytes with superior anode and cathode compatibility for LMBs. Here, we propose an active diluent-anion synergy strategy to achieve outstanding compatibility with Li metal anodes and high-voltage cathodes by using 1,2-difluorobenzene (DFB) with high activity for yielding LiF as an active diluent to regulate nonflammable dimethylacetamide (DMAC)-based localized high concentration electrolyte (LHCE-DFB). DFB and bis(fluorosulfonyl)imide (FSI−) anion cooperate to construct robust LiF-rich solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), which effectively stabilize DMAC from intrinsic reactions with Li metal anode and enhance the interfacial stability of the Li metal anodes and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes. LHCE-DFB enables ultrahigh Coulombic efficiency (98.7 %), dendrite-free, extremely stable and long-term cycling of Li metal anodes in Li || Cu cells and Li || Li cells. The fabricated NCM811 || Li cells with LHCE-DFB display remarkably enhanced long-term cycling stability and excellent rate capability. This work provides a promising active diluent-anion synergy strategy for designing high-voltage electrolytes for high-energy batteries. 相似文献
20.
Qingshun Nian Tianjiang Sun Yecheng Li Song Jin Shuang Liu Xuan Luo Zihong Wang Bing-Qing Xiong Zhuangzhuang Cui Digen Ruan Prof. Hengxing Ji Prof. Zhanliang Tao Prof. Xiaodi Ren 《Angewandte Chemie (International ed. in English)》2023,62(9):e202217671
Electrolyte freezing under low temperatures is a critical challenge for the development of aqueous batteries (ABs). While lowering the freezing point of the electrolyte has caught major research efforts, limited attention has been paid to the structural evolution during the electrolyte freezing process and regulating the frozen electrolyte structure for low temperature ABs. Here, we reveal the formation process of interconnected liquid regions for ion transport in frozen electrolytes with various in situ variable-temperature technologies. More importantly, the low-temperature performance of ABs was significantly improved with the colloidal electrolyte design using graphene oxide quantum dots (GOQDs), which effectively inhibits the growth of ice crystals and expands the interconnected liquid regions for facial ion transport. This work provides new insights and a promising strategy for the electrolyte design of low-temperature ABs. 相似文献