Energy Storage Materials最新文献_第9页

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 , Jisu Kim , Riyul Kim , Young Jun Lim , 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 LiNi0.88Co0.09Al0.03O2 (NCA) cathode, a Li6PS5Cl (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 , Luming Yin , Letian Chen , Bingbing Ma , Yuantonghe Li , Xinyi Zhang , Junqing Liu , Zhen Zhou","doi":"10.1016/j.ensm.2025.104171","DOIUrl":"10.1016/j.ensm.2025.104171","url":null,"abstract":"<div><div>Lithium-nitrogen (Li-N2) 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 FeOx nano-particle catalysts and Fe single-atom catalysts to enhance nitrogen reduction reaction in Li-N2 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 FeOx drives the electron redistribution of Fe3+ d-orbitals to provide electron-donating Fe active sites for N2 fixation. Meanwhile, oxygen vacancy-rich MoOy 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 MoOy to Fe to N2. Therefore, the Li-N2 batteries exhibit large discharge capacity, excellent rate performance, and reliable cycle stability. In addition, the formation and decomposition of the discharge product Li3N indicate a reversible N2 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-N2 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 , Xinyue Wang , Qi Jin , Zhiguo Zhang , Xitian Zhang , 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 La0.71Sr0.29(Fe0.19Co0.20Ni0.20Zn0.19Mn0.22)O3−δ (HE−LSMO) nanosheets are synthesized by incorporating more metallic ions into LaSrMnO3, 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−1 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−1 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 , Siyuan Ma , Yuefeng Su , Tinglu Song , Yun Lu , Lai Chen , Qing Huang , Yibiao Guan , Feng Wu , 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−1 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−1 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 , Lanhe Zhang , Yang Liu , Sen Wang , 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 Ti3C2Tx 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-2. Symmetric cells with the composite Zn powder anode demonstrates stble cycling for 300 h at 1 mA g-1 and 1 mA h g-1, 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-1 for MnVO and 82.2% after 1000 cycles at 1 A·g-1 for MnO2). 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

Lifetime prediction and dynamics modeling of Al-air batteries optimized by Al-Zn energy transfer strategy for efficient energy storage

IF 18.9 1区材料科学

Energy Storage Materials Pub Date : 2025-02-21 DOI: 10.1016/j.ensm.2025.104139

Manhui Wei , Zhenxiong Wang , Meixia Zhang , Hengwei Wang , Daiyuan Zhong , Keliang Wang , Pucheng Pei , Guofeng Fang , Xinglong Liu

{"title":"Lifetime prediction and dynamics modeling of Al-air batteries optimized by Al-Zn energy transfer strategy for efficient energy storage","authors":"Manhui Wei , Zhenxiong Wang , Meixia Zhang , Hengwei Wang , Daiyuan Zhong , Keliang Wang , Pucheng Pei , Guofeng Fang , Xinglong Liu","doi":"10.1016/j.ensm.2025.104139","DOIUrl":"10.1016/j.ensm.2025.104139","url":null,"abstract":"<div><div>Al-air batteries exhibit extraordinary potential for efficient energy storage, but the parasitic hydrogen evolution caused by the contact of Al with free H2O sacrifices the energy efficiency significantly. The protective layer formed by Al-Zn energy transfer strategy has been demonstrated to be conspicuously efficacious in inhibiting anode self-discharge and extending battery's lifetime. However, the transfer dynamics of energy, mass and charge in proposed strategy remains unclear. In this work, the mechanism of Al-Zn energy transfer is analyzed experimentally and a numerical model of the battery is developed theoretically. The results show that the model attains high-accuracy in predicting battery lifetime. The anode mass associated with battery discharge, substitution reaction and hydrogen evolution follows the second-order functions of absolute surface coverage. Furthermore, variations in the concentrations of Al(OH)4-, Zn(OH)42- and OH-, along with changes in electrode overpotential, are identified. Finally, the formation of insoluble metal hydroxide/oxide proves to be a critical barrier, hindering the mass transport and charge transfer of Al anode, thereby limiting the high potential output of the battery.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104139"},"PeriodicalIF":18.9,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463245","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

Electronic structure engineering through strengthened d–p orbital hybridization of sodium ferric sulfate cathode with enhanced electrochemical performance for sodium-ion batteries

IF 18.9 1区材料科学

Energy Storage Materials Pub Date : 2025-02-21 DOI: 10.1016/j.ensm.2025.104138

Qingbo Zhou , Yuhang Xin , Yingshuai Wang , Ziye Wang , Xiangyu Ding , Chang Sun , Lei Liu , Qianchen Wang , Feng Wu , Eslam Sheha , Hongcai Gao

{"title":"Electronic structure engineering through strengthened d–p orbital hybridization of sodium ferric sulfate cathode with enhanced electrochemical performance for sodium-ion batteries","authors":"Qingbo Zhou , Yuhang Xin , Yingshuai Wang , Ziye Wang , Xiangyu Ding , Chang Sun , Lei Liu , Qianchen Wang , Feng Wu , Eslam Sheha , Hongcai Gao","doi":"10.1016/j.ensm.2025.104138","DOIUrl":"10.1016/j.ensm.2025.104138","url":null,"abstract":"<div><div>The Na2+2xFe2-x(SO4)3 (NFS) cathode has garnered significant attention due to its high voltage and affordability. Nevertheless, the low intrinsic conductivity of the NFS results in poor electrochemical properties. In this work, magnesium ions with low electronegativity are strategically incorporated into the iron sites. There is an increased tendency for electrons to migrate toward the bridging oxygen atom (Fe-O-Mg). This asymmetric distribution of electrons is conducive to the reduction of band gap and the improvement of diffusion kinetics. Besides, the s-p orbital hybridization in Mg-O bonds has a lower energy, leading to a more stable lattice structure and strengthened Fe3d-O2p orbital interactions. Hence, the optimised Mg substituted NFS cathode obtains high capacity (96.2 mAh g-1 at 0.1 C) and long cycle stability with low average capacity attenuation rates of 0.52 % and 0.57 % per cycle even at high current densities of 10 C and 20 C. Overall, regulating electronic structure through strengthened d–p orbital hybridization is an effective strategy to design cathode materials with superior electrochemical performance.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104138"},"PeriodicalIF":18.9,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463244","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

Chemical disorder engineering enables high-voltage stable oxide cathodes over –20–25 ℃ in sodium-ion batteries

IF 18.9 1区材料科学

Energy Storage Materials Pub Date : 2025-02-21 DOI: 10.1016/j.ensm.2025.104106

Tianyi Song , Chenchen Wang , Pinit Kidkhunthod , Xiaolong Zhou , Anquan Zhu , Yuanqi Lan , Kunlun Liu , Jianli Liang , Wenjun Zhang , Wenjiao Yao , Yongbing Tang , Chun-Sing Lee

{"title":"Chemical disorder engineering enables high-voltage stable oxide cathodes over –20–25 ℃ in sodium-ion batteries","authors":"Tianyi Song , Chenchen Wang , Pinit Kidkhunthod , Xiaolong Zhou , Anquan Zhu , Yuanqi Lan , Kunlun Liu , Jianli Liang , Wenjun Zhang , Wenjiao Yao , Yongbing Tang , Chun-Sing Lee","doi":"10.1016/j.ensm.2025.104106","DOIUrl":"10.1016/j.ensm.2025.104106","url":null,"abstract":"<div><div>O3-type Mn-Fe-Ni layer oxide cathodes show great commercialization potential due to their high capacities and simple synthesis. Nevertheless, simultaneously achieving high energy density and good cycling stability remains challenging. Herein, we introduce a chemical disordering strategy to create O3-Na0.83Mn0.35Fe0.15Ni0.15Cu0.10Co0.20Sn0.05O2 (MFNCCS) cathode. The chemical disordering strategy was implemented through selective multi-transition metal substitution and quenching during synthesis. The former promotes a high entropy effect, while the latter is beneficial to increasing the quenching disorder degree, functioning a synergy effect in suppressing irreversible multi-phase transitions and promoting cycling stability. As a result, the MFNCCS cathode can retain 91.6 % (∼103.3 mAh g–1) of its capacity after 500 cycles at 200 mA g–1, with an energy density of 285.3 Wh kg⁻1 at the 500th cycle, which is superior to previously reported state-of-the-art layered oxide cathodes in the voltage range of 2.0–4.3 V. Besides, it achieves stable cycling within 2.0–4.3 V over temperature range of –20 to 25 °C. This work offers new insights for high-voltage stable layered cathodes in wide-temperature SIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104106"},"PeriodicalIF":18.9,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143453995","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

Cation-disordered fluoride to facilitate durable interfaces in (all) solid-state Li batteries

IF 18.9 1区材料科学

Energy Storage Materials Pub Date : 2025-02-20 DOI: 10.1016/j.ensm.2025.104136

Dongil Kim , Seungun Shin , Seong Hee Jeong , Woosuk Cho , Myeongsoo Kim , Hyejin Kwon , Min-Sang Song , Duho Kim , Min-Sik Park

{"title":"Cation-disordered fluoride to facilitate durable interfaces in (all) solid-state Li batteries","authors":"Dongil Kim , Seungun Shin , Seong Hee Jeong , Woosuk Cho , Myeongsoo Kim , Hyejin Kwon , Min-Sang Song , Duho Kim , Min-Sik Park","doi":"10.1016/j.ensm.2025.104136","DOIUrl":"10.1016/j.ensm.2025.104136","url":null,"abstract":"<div><div>Nickel (Ni)-rich cathode materials such as LiNi0.8Co0.1Mn0.1O2 (NCM) have received considerable attention as potential candidates for lithium-ion batteries (LIBs) and all-solid-state batteries (ASSBs) owing to their high theoretical capacities. However, the practical application of NCM is limited by its surface instability, which is primarily attributed to its high Ni content and interfacial side reactions with sulfide-based solid electrolytes. In this study, we designed Li2.4Ga1.2F6 (LGF), which exhibits high ionic conductivity and electrochemical stability, as a durable interface based on cationic disordering and vacancy concepts to reduce the interfacial resistance and improve the structural stability of NCM in LIBs and Li6PS5Cl (LPSCl) in ASSBs. The LGF coating layer can modulate the interfacial reactions between NCM particles, conventional liquid electrolytes, and sulfide-based solid electrolytes. The LGF coating layer significantly enhanced Li+ transport and surface stability, effectively suppressed interfacial side reactions, and decreased the internal resistance, resulting in improved reversibility and cycling performance of the NCM cathode. This enables the practical application of LGF, proposed by the cationic point-defect strategy, as effective coating layers for NCM cathode materials in advanced LIBs and ASSBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104136"},"PeriodicalIF":18.9,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452128","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

Achieving ultra-long cycling life for MnO2 cathode: Modulating Mn3+ spin state to suppress Jahn–Teller distortion and manganese dissolution

IF 18.9 1区材料科学

Energy Storage Materials Pub Date : 2025-02-19 DOI: 10.1016/j.ensm.2025.104128

Ziyi Zhang , Jie Zheng , Xinya Chen , Xinyu Yu , Lijie Li , Lixia Bao , Jiong Peng , Xin Li

{"title":"Achieving ultra-long cycling life for MnO2 cathode: Modulating Mn3+ spin state to suppress Jahn–Teller distortion and manganese dissolution","authors":"Ziyi Zhang , Jie Zheng , Xinya Chen , Xinyu Yu , Lijie Li , Lixia Bao , Jiong Peng , Xin Li","doi":"10.1016/j.ensm.2025.104128","DOIUrl":"10.1016/j.ensm.2025.104128","url":null,"abstract":"<div><div>MnO2 is emerging as an electrode material for sodium-ion capacitors due to its high specific capacity and low cost. However, Jahn-teller distortion and manganese dissolution pose a formidable challenge in practical applications. Herein, the Mn3+ spin state, causing J-T distortion, is modulated to address these issues, which is achieved through strategically incorporating Co into the MnO2 lattice to increase electron occupancy in the t2g orbital. The transition from a high-spin Mn3+ to a low-spin state leads to electron movement from the dx2-y2 orbitals to the dxy orbitals, which effectively lowers the energy level of the eg orbitals, reduces orbital degeneracy, and enhances the stability of the Mn-O bond. DFT calculations, In situ Raman and inductively coupled plasma optical emission spectroscopy (ICP-OES) demonstrate that the distortion of [MnO6] and Mn dissolution of Co-MnO2 are reduced by 69 % and 80 % respectively compared with MnO2 during the charge-discharge cycle. Consequently, Co-MnO2 exhibits approximately 98 % capacity retention after 40,000 cycles at 10 A/g, achieving exceptional long-term stability. This study provides new insights into the relationships among J-T distortion, manganese dissolution and spin state, provides a novel approach to enhance the stability of MnO2 for electrochemistry applications.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"76 ","pages":"Article 104128"},"PeriodicalIF":18.9,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143452131","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