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Fluorine and carbonate regulated nonflammable polymer electrolyte for ultrastable high-voltage Li metal batteries
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104129
Xuan Wang , Daxi Pan , Lisi Xu , Daize Mo , Haijiao Xie , Yuezhong Meng , Kuirong Deng
{"title":"Fluorine and carbonate regulated nonflammable polymer electrolyte for ultrastable high-voltage Li metal batteries","authors":"Xuan Wang ,&nbsp;Daxi Pan ,&nbsp;Lisi Xu ,&nbsp;Daize Mo ,&nbsp;Haijiao Xie ,&nbsp;Yuezhong Meng ,&nbsp;Kuirong Deng","doi":"10.1016/j.ensm.2025.104129","DOIUrl":"10.1016/j.ensm.2025.104129","url":null,"abstract":"<div><div>Polymer electrolytes are promising electrolytes for solid-state Li metal batteries owing to their low flammability, non-leakage, easy processing and good flexibility. However, low ionic conductivity and inferior oxidation stability of conventional polymer electrolytes hinder their application in high-voltage Li metal batteries. Herein, we develop a fluorine and carbonate regulated nonflammable polymer electrolyte (F-HV) for high-voltage Li metal batteries. Fluorinated main chains endow F-HV with high oxidative stability (4.9 V vs. Li<sup>+</sup>/Li) and promote the formation of robust LiF-rich interfaces, effectively enhancing the interfacial stability of LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathodes and Li metal anodes. Carbonate side chains facilitate dissociation and conduction of Li<sup>+</sup>, effectively enhancing the ionic conductivity to 1.97 mS cm<sup>−1</sup>. F-HV possesses excellent flame resistance and favorable dimension stability up to 200 °C. F-HV markedly boosts the performance of Li||NCM811 and Li||LiFePO<sub>4</sub> (LFP) cells, which exhibit an ultralong cycle life of 3000 cycles with an impressive capacity retention of 86.3%. F-HV also enables Li||NCM811 cells with enhanced cycle stability at high temperature (60 °C) and high voltage (4.5 V). This work provides an effective strategy for achieving high-performance solid-state Li metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104129"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Surface-finish induced textured electrodeposition on 20 μm Li-metal anode
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104160
Yuhang Hu , Yong Li , Haorui Hou , Zidong Chen , Yungui Chen , Naseem Iqbal , Wei Liu
{"title":"Surface-finish induced textured electrodeposition on 20 μm Li-metal anode","authors":"Yuhang Hu ,&nbsp;Yong Li ,&nbsp;Haorui Hou ,&nbsp;Zidong Chen ,&nbsp;Yungui Chen ,&nbsp;Naseem Iqbal ,&nbsp;Wei Liu","doi":"10.1016/j.ensm.2025.104160","DOIUrl":"10.1016/j.ensm.2025.104160","url":null,"abstract":"<div><div>Implementing Li metal anode with thickness &lt;50 μm is a key step to achieve high energy density lithium metal batteries. However, the production of thin Li-foils is non-standardized, with the supplier-dependent qualities incurring uncertainties for cell development and evaluation. Here, we demonstrate that Li-foils with varying thicknesses possess distinct surface finishes and bulk-phase textures. As the extrusion-produced 200 μm Li foils are rich in inorganic surface species and (110)-texture, the 20 μm Li produced via rolling feature organic surface species and (100)-Li texture underneath. The surface finish and foil textures are rooted in the angled shear forces and rolling lubricant. Textured Li foils are conducive to epitaxial Li deposition however the native surface passivation layer perturbs the substrate-deposits intimacy and degrades its electrochemical reversibility. Mechanical and chemical polishing were employed to refine the Li surface finish, only the latter achieves an ideal surface finish that reinstates epitaxial Li-electrodeposition. This engenders textured Li deposits, greatly improving the lifespan of lithium metal anodes. Pouch cells employing chemically polished 20 μm Li anodes and 20 mg/cm<sup>2</sup> NCM811 cathodes exhibit capacity retention of 97.1 % after 100 cycles. The benefit of surface-finish in 20 μm Li was verified in &gt;400 Wh/kg Ah-pouch-cells.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104160"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Homogeneous low-tortuosity membrane with fast ion transfer towards life-durable low-temperature zinc metal batteries
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104161
Yongzheng Zhang , Huiqing Zhou , Jianan Gu , Haifeng Yang , Xiaomin Cheng , Jing Zhang , Jitong Wang , Yanli Wang , Hongzhen Lin , Jian Wang , Liang Zhan , Licheng Ling
{"title":"Homogeneous low-tortuosity membrane with fast ion transfer towards life-durable low-temperature zinc metal batteries","authors":"Yongzheng Zhang ,&nbsp;Huiqing Zhou ,&nbsp;Jianan Gu ,&nbsp;Haifeng Yang ,&nbsp;Xiaomin Cheng ,&nbsp;Jing Zhang ,&nbsp;Jitong Wang ,&nbsp;Yanli Wang ,&nbsp;Hongzhen Lin ,&nbsp;Jian Wang ,&nbsp;Liang Zhan ,&nbsp;Licheng Ling","doi":"10.1016/j.ensm.2025.104161","DOIUrl":"10.1016/j.ensm.2025.104161","url":null,"abstract":"<div><div>Aqueous zinc metal batteries (AZMBs) have attracted significant attentions in the energy storage field due to their environmental safety. However, sluggish reaction kinetics of Zn(H<sub>2</sub>O)<sub>6</sub><sup>2+</sup> desolvation and corresponding Zn<sup>2+</sup> ion transfer hinder the low-temperature performance of AZMBs. Herein, the boundary inhibition effect of ion-related pathway is initially uncovered, and a homogeneous low-tortuosity separator membrane (LTSM) with enhanced kinetics of ion desolvation and transfer is proposed. This low-tortuosity structure of LTSM significantly enhances the effectiveness of pore sieving effect toward large Zn(H<sub>2</sub>O)<sub>6</sub><sup>2+</sup> clusters, minimizing ion transfer barriers and homogenizing ion flux, as revealed by Raman and sum frequency generation spectroscopies. Encouragingly, the metallic Zn with LTSM exhibits lower nucleation overpotentials of ∼50 mV, showcasing an ultralong lifespan of over 10,000 h at 0 °C. Even under −10 °C, a cycle life up to 5000 h is also achieved. The as-prepared full cells assembled with LTSM display the specific capacity of 200 mAh g<sup>−1</sup> after 4000 cycles at 8 A g<sup>−1</sup> under 0 °C. Increasing to 6.3 mg cm<sup>−2</sup>, the large areal pouch cell stabilizes for 160 cycles with retained capacity of 315 mAh g<sup>−1</sup>, demonstrating feasibility of eliminating the boundary inhibition effect with low-tortuosity separator membrane for practical applications.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104161"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
State-of-charge mediated short-term low-temperature calendar aging impacts the cycling stability of Ni-rich cathodes in pouch full cells
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104143
Wei Shi , Ling Liu , Ruofan Xu , Rongkun Sun , Jinyang Dong , Xiaohong Kang
{"title":"State-of-charge mediated short-term low-temperature calendar aging impacts the cycling stability of Ni-rich cathodes in pouch full cells","authors":"Wei Shi ,&nbsp;Ling Liu ,&nbsp;Ruofan Xu ,&nbsp;Rongkun Sun ,&nbsp;Jinyang Dong ,&nbsp;Xiaohong Kang","doi":"10.1016/j.ensm.2025.104143","DOIUrl":"10.1016/j.ensm.2025.104143","url":null,"abstract":"<div><div>Both calendar aging and cycling aging significantly affect the practical performance and service life of lithium-ion batteries (LIBs), especially for high-nickel cathodes used in high-energy-density applications. However, limited research has been conducted on how calendar aging influences subsequent cycling performance. This study addresses the gap by examining the effects of state-of-charge (SoC) during short-term low-temperature storage on both calendar aging and cycling degradation in LIBs with high-nickel cathodes. The findings demonstrate that high SoC storage accelerates calendar aging by causing structural degradation at the cathode-electrolyte interface (CEI), leading to phase transitions and increased mechanical stress. However, these conditions also enhance cycling stability by promoting surface reconstruction of the high-nickel cathode, which reduces lattice strain and mitigates detrimental phase transformations. The surface reconstruction improves lithium-ion diffusion and stabilizes the crystal structure, resulting in less mechanical degradation during cycling. Conversely, low SoC storage leads to reduced structural degradation during calendar aging, but the lack of an inert protective layer on the cathode surface causes lattice strain and phase transitions during lithium intercalation, resulting in microcracks that compromise the cathode structure. Concurrently, transition metal dissolution, migration, and deposition accelerate anode degradation by promoting interfacial reactions, which exacerbate solid electrolyte interphase (SEI) formation and degradation, and consume reversible lithium ions. Storage is a critical process in the lifecycle of LIBs in electric vehicles (EVs), necessitating the development of advanced battery management strategies tailored to the SoC-dependent stabilities of active materials. These results emphasize the complex relationship between calendar and cycling aging, providing important insights into optimizing high-energy-density cathodes with long durability.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104143"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477705","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Protonated interface microenvironment design towards stable Zinc-Metal pouch cells
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104162
Shaohui Hu , Wei Huang , Dongliang Yan , Ming Yang , Yuejia Qing , Shunmin Yi , Yanfei Zeng , Qifan Liu , Shengkui Zhong , Dingtao Ma , Peixin Zhang
{"title":"Protonated interface microenvironment design towards stable Zinc-Metal pouch cells","authors":"Shaohui Hu ,&nbsp;Wei Huang ,&nbsp;Dongliang Yan ,&nbsp;Ming Yang ,&nbsp;Yuejia Qing ,&nbsp;Shunmin Yi ,&nbsp;Yanfei Zeng ,&nbsp;Qifan Liu ,&nbsp;Shengkui Zhong ,&nbsp;Dingtao Ma ,&nbsp;Peixin Zhang","doi":"10.1016/j.ensm.2025.104162","DOIUrl":"10.1016/j.ensm.2025.104162","url":null,"abstract":"<div><div>Zinc metal anode is considered to be the major technical shortcoming of building practical aqueous zinc-ion batteries, since random dendrite growth and interfacial chain side reaction would greatly shorten its service life. Herein, a novel protonated diatomaceous earth (DE-ALK)-based artificial interphase is fabricated through a scalable tape-casting strategy. Such protective mechanism not only comes from the physical characteristics but also from the unique protonation interface effect of DE-ALK. As demonstrated, through a strong protonation reaction, the surface charge of DE-ALK shifts from negative to positive of +23.37 mV, result in effectively regulating the anode microenvironment. Benefited from the built-in electrostatic field, the side reactions involving anionic species and HER are suppressed by immobilizing sulfate anions, and the de-solvation of hydrated zinc ions is promoted by weakening the interaction between Zn<sup>2+</sup> and water, thereby accelerating the reaction kinetics and inhibiting the dendrite growth. As a result, DE-ALK@Zn symmetrical cell achieves an impressive lifespan exceeding 2400 h at 8 mA cm⁻². Moreover, stable Na<sub>2</sub>V<sub>6</sub>O<sub>16</sub>·1·5H<sub>2</sub>O (NVO)-based pouch cell was further built, which can deliver 269.8 mAh g<sup>−1</sup> and a capacity retention of ∼98.6 % after 100 cycles at 0.5 A g<sup>−1</sup>. This work offers valuable insights for the industrial advancement of aqueous zinc-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104162"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanistic insight into calendar aging of anode-less all-solid-state batteries
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104164
Junhee Kang , Jisu Kim , Riyul Kim , Young Jun Lim , Jong-Won Lee
{"title":"Mechanistic insight into calendar aging of anode-less all-solid-state batteries","authors":"Junhee Kang ,&nbsp;Jisu Kim ,&nbsp;Riyul Kim ,&nbsp;Young Jun Lim ,&nbsp;Jong-Won Lee","doi":"10.1016/j.ensm.2025.104164","DOIUrl":"10.1016/j.ensm.2025.104164","url":null,"abstract":"<div><div>Anode-less all-solid-state batteries (ASSBs) with thin interlayers have emerged as a promising solution capable of addressing the dendrite issues of Li metal anodes and considerably enhancing the energy density. However, only a few studies have investigated the calendar life of anode-free ASSBs. Herein, we reveal the degradation of an anode-less ASSB with a LiNi<sub>0.88</sub>Co<sub>0.09</sub>Al<sub>0.03</sub>O<sub>2</sub> (NCA) cathode, a Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) electrolyte, and an Ag-C interlayer during storage and provide mechanistic insights into the possible calendar aging process. The cell shows a decline in discharge capacity after long-term storage, depending on the storage conditions and, more importantly, exhibits the reduced capacity retention upon subsequent cycling. No microstructural and electrochemical degradation is observed on the anode side; however, the composite cathode stored at a high state of charge (SOC) suffers from severe degradation upon storage. In-depth chemical and structural analyses, coupled with impedance decoupling, reveal that the high-SOC storage facilitates the detrimental interfacial side reactions between NCA and LPSCl, which are accelerated at elevated temperatures. As a strategy to address this issue, we further demonstrate that increasing the external pressure to tens of MPa during storage facilitates the chemical lithiation of NCA, which can effectively alleviate the calendar aging of anode-less ASSBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104164"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Size- and crystallinity-dependent oxygen vacancy engineering to modulate Fe active sites for enhanced reversible nitrogen fixation in Lithium-nitrogen batteries
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104171
Nengbiao Zhang , Luming Yin , Letian Chen , Bingbing Ma , Yuantonghe Li , Xinyi Zhang , Junqing Liu , Zhen Zhou
{"title":"Size- and crystallinity-dependent oxygen vacancy engineering to modulate Fe active sites for enhanced reversible nitrogen fixation in Lithium-nitrogen batteries","authors":"Nengbiao Zhang ,&nbsp;Luming Yin ,&nbsp;Letian Chen ,&nbsp;Bingbing Ma ,&nbsp;Yuantonghe Li ,&nbsp;Xinyi Zhang ,&nbsp;Junqing Liu ,&nbsp;Zhen Zhou","doi":"10.1016/j.ensm.2025.104171","DOIUrl":"10.1016/j.ensm.2025.104171","url":null,"abstract":"<div><div>Lithium-nitrogen (Li-N<sub>2</sub>) battery is not only an electrochemical energy storage platform, but also an environmentally friendly nitrogen fixation technology. However, a great challenge remains in regulating catalyst activity to accelerate cathode reaction kinetics. Herein, we proposed an oxygen vacancy-mediated modulation of Fe active sites in FeO<em><sub>x</sub></em> nano-particle catalysts and Fe single-atom catalysts to enhance nitrogen reduction reaction in Li-N<sub>2</sub> batteries. High-concentration oxygen vacancy is generated through a size- and crystallinity-dependent oxygen vacancy engineering based on the precise atomic layer deposition of reducible oxides. The oxygen vacancy on FeO<em><sub>x</sub></em> drives the electron redistribution of Fe<sup>3+</sup> d-orbitals to provide electron-donating Fe active sites for N<sub>2</sub> fixation. Meanwhile, oxygen vacancy-rich MoO<em><sub>y</sub></em> is used as a support to anchor Fe single atoms. Adjacent oxygen vacancy drives the stable coordination between Fe single atoms and O atoms to facilitate the directional electron transfer from MoO<em><sub>y</sub></em> to Fe to N<sub>2</sub>. Therefore, the Li-N<sub>2</sub> batteries exhibit large discharge capacity, excellent rate performance, and reliable cycle stability. In addition, the formation and decomposition of the discharge product Li<sub>3</sub>N indicate a reversible N<sub>2</sub> fixation. This work provides a precise regulation mechanism of catalytic active sites based on oxygen vacancy engineering, which is expected to promote the development of high-performance Li-N<sub>2</sub> batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104171"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582485","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-entropy-induced strong dipole moment for accelerating sulfur reduction kinetics lithium-sulfur batteries across a wide range of temperatures
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-03-01 DOI: 10.1016/j.ensm.2025.104147
Chi Zhang , Xinyue Wang , Qi Jin , Zhiguo Zhang , Xitian Zhang , Lili Wu
{"title":"High-entropy-induced strong dipole moment for accelerating sulfur reduction kinetics lithium-sulfur batteries across a wide range of temperatures","authors":"Chi Zhang ,&nbsp;Xinyue Wang ,&nbsp;Qi Jin ,&nbsp;Zhiguo Zhang ,&nbsp;Xitian Zhang ,&nbsp;Lili Wu","doi":"10.1016/j.ensm.2025.104147","DOIUrl":"10.1016/j.ensm.2025.104147","url":null,"abstract":"<div><div>Developing unexpected electrocatalysts is essential for lithium−sulfur batteries operating under harsh environmental conditions. Herein, a high−entropy−induced dipole moment enhancement strategy is proposed to address the problems related to complex temperature variations. In particular, a new platform corresponding to liquid-liquid conversion appears at low temperatures, considered as another rate-determining step. High−entropy oxide La<sub>0.71</sub>Sr<sub>0.29</sub>(Fe<sub>0.19</sub>Co<sub>0.20</sub>Ni<sub>0.20</sub>Zn<sub>0.19</sub>Mn<sub>0.22</sub>)O<sub>3−δ</sub> (HE−LSMO) nanosheets are synthesized by incorporating more metallic ions into LaSrMnO<sub>3</sub>, which would increase the crystal asymmetry, create the redistribution of the electron cloud in the HE−LSMO, thereby enhancing dipole moments and strengthening the dipole−dipole interaction between HE−LSMOs and polar intermediate lithium polysulfides (LiPSs). The HE−LSMO can effectively adsorb LiPSs and greatly promote rapid conversions of LiPSs during the sulfur reduction process at a range of −35 to 50 °C. At 50 °C, the S/HE−LSMO cathode exhibits a high initial specific capacity of 1455.9 mAh g<sup>−1</sup> at 0.5 C, with a capacity retention rate of 71.1 % after 100 cycles. At −35 °C, the S/HE−LSMO cathode maintains an initial capacity of 740.7 mAh g<sup>−1</sup> at 0.5 C, with an impressive capacity retention of 90.4 % after 100 cycles. This work demonstrates the feasibility of the high−entropy−induced dipole moment enhancement strategy for lithium−sulfur batteries under wide temperatures.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104147"},"PeriodicalIF":18.9,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486412","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
“Shooting three birds with one stone”: Bi-conductive and robust binder enabling low-cost micro-silicon anodes for high-rate and long-cycling operation "一石三鸟":双导电性强韧粘结剂实现低成本微硅阳极的高速率和长周期运行
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-02-22 DOI: 10.1016/j.ensm.2025.104140
Wengang Yan , Siyuan Ma , Yuefeng Su , Tinglu Song , Yun Lu , Lai Chen , Qing Huang , Yibiao Guan , Feng Wu , Ning Li
{"title":"“Shooting three birds with one stone”: Bi-conductive and robust binder enabling low-cost micro-silicon anodes for high-rate and long-cycling operation","authors":"Wengang Yan ,&nbsp;Siyuan Ma ,&nbsp;Yuefeng Su ,&nbsp;Tinglu Song ,&nbsp;Yun Lu ,&nbsp;Lai Chen ,&nbsp;Qing Huang ,&nbsp;Yibiao Guan ,&nbsp;Feng Wu ,&nbsp;Ning Li","doi":"10.1016/j.ensm.2025.104140","DOIUrl":"10.1016/j.ensm.2025.104140","url":null,"abstract":"<div><div>High-capacity micro-sized Si-based (μSi) lithium-ion batteries confront notable challenges such as unstable bulk phase structure, thick solid electrolyte interface (SEI), and sluggish ion transport kinetics. In this study, we proposed a bi-conductive and robust binder to alleviate volume expansion, suppress repeated rupture and generation of SEI, and improve the electrochemical reaction kinetics of the μSi electrode. The binder was synthesized through thermal crosslinking of “hard” polyacrylic acid (PAA), “soft” polyvinyl alcohol (PVA) and conductive graphene (denoted as PPG). Utilizing extensive chemical and material characterizations, it has been demonstrated that the electrodes prepared with PPG binder and μSi (μSi-PPG) exhibit superior electrochemical reaction kinetics, highly complete electrode structure, dense and stable SEI during electrochemical cycling. The μSi-PPG electrodes exhibit superior electrochemical performance, with the high capacity of 1913.1 mAh g<sup>−1</sup> and capacity retention of 86.7 % at 1 C after 1000 cycles. More importantly, the μSi-PPG electrode presents an ultra-high capacity of 1451 mAh g<sup>−1</sup> at 5 C. The design concept of this bi-conductive and robust binder provides a new guidance scheme for achieving long-cycling life and high rate performance in high-volume-strain electrode materials.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104140"},"PeriodicalIF":18.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A dual-functional DMDAAC electrode enhancer with hydrophobic effect for highly stable Zn powder composite anode
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-02-22 DOI: 10.1016/j.ensm.2025.104127
Wenying Tang , Lanhe Zhang , Yang Liu , Sen Wang , Jian Zhang
{"title":"A dual-functional DMDAAC electrode enhancer with hydrophobic effect for highly stable Zn powder composite anode","authors":"Wenying Tang ,&nbsp;Lanhe Zhang ,&nbsp;Yang Liu ,&nbsp;Sen Wang ,&nbsp;Jian Zhang","doi":"10.1016/j.ensm.2025.104127","DOIUrl":"10.1016/j.ensm.2025.104127","url":null,"abstract":"<div><div>MXene-modified zinc powder (MXene@Zn-p) anodes have demonstrated the unique effect of inhibiting dendrite growth, thereby enhancing interface stability. However, the insufficient binding force between Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene and Zn powder, endowed with natural hydrophilicity, results in an inevitable failure of MXene@Zn-p anodes during long-term cycles. To address this issue, Dimethyl Diallyl Ammonium Chloride (DMDAAC) is introduced as a dual-functional electrode enhancer to construct a tight hydrophobic interface on the Zn powder composite anode by electrostatic self-assembly while effectively solving the weak adhesion and hydrophilicity of both MXene and Zn powder. The obtained Zn powder composite anode effectively suppresses dendrite growth and corrosion effects, achieving a durable interfacial stability. The DFT and COMSOL simulations further certify that the DMDAAC plays a key role in regulating uniform Zn deposition. As a result, the as-engineered anode achieves a high coulombic efficiency of 99.2% after 300 cycles at 1 mA cm<sup>-2</sup>. Symmetric cells with the composite Zn powder anode demonstrates stble cycling for 300 h at 1 mA g<sup>-1</sup> and 1 mA h g<sup>-1</sup>, extending lifespan by 233 h compared with MXene@Zn-p anode. The assembled two full cells with Zn powder composite anode also exhibit reamrkably high capacity retention and cycling stability (89.8% after 200 cycles at 5 A·g<sup>-1</sup> for MnVO and 82.2% after 1000 cycles at 1 A·g<sup>-1</sup> for MnO<sub>2</sub>). This work provides an efficient strategy for achieving highly stable Zn powder composite anode, thus facilitating the commercialization process of aqueous zinc ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":""},"PeriodicalIF":18.9,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143465422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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