Energy Storage Materials最新文献_第6页

Dendrite-free aluminum metal anode enabled by work function engineering

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104232

Shunlong Ju , Xiaoyue Zhang , Chaoqun Li , Yingxue Li , Panyu Gao , Sihan Yin , Tengfei Zhang , Guanglin Xia , Baozhong Liu , Xuebin Yu

The uncontrolled deposition behavior, sluggish reaction kinetics and inefficient utilization of Al derived from unstable anode/electrolyte interface have severely impeded the development of aluminum-ion batteries. Here, we discuss the impact of interfacial electron/ion transfer on the electrochemical performance, and as an illustration, propose the construction of Cu@MXene as anodic current collector through work function engineering to simultaneously achieve homogeneous deposition morphology and rapid plating/stripping rate. The difference in work function between Cu nanoparticles and Ti₃C₂ MXene facilitates charge redistribution in the anode/electrolyte interface and enhances the electron availability, optimizing the interfacial electron/ion transfer behavior. This, in turn, endows Cu@MXene with elevated catalytic efficiency for desolvation reactions and robust reduction ability for the Al plating process. As a result, Cu@MXene enables a high coulombic efficiency of 99.87 % even at a high current density of 10 mA cm⁻², and sustains reversible Al plating/stripping cycles for over 3200 h at a typical current density of 1 mA cm⁻². Notably, by coupling graphite cathode and Cu@MXene-Al anode under a limited N/P ratio of 2.2, the full cell exhibits durable lifetime for 2000 cycles with an impressive energy density of 119.6 Wh kg⁻¹ (based on the total mass of cathode and anode). This work highlights a fundamental understanding of interfacial interactions in the Al deposition process and offer sustainability motivations in designing highly reversible anodes for high-energy-density aluminum-ion batteries.

{"title":"Dendrite-free aluminum metal anode enabled by work function engineering","authors":"Shunlong Ju , Xiaoyue Zhang , Chaoqun Li , Yingxue Li , Panyu Gao , Sihan Yin , Tengfei Zhang , Guanglin Xia , Baozhong Liu , Xuebin Yu","doi":"10.1016/j.ensm.2025.104232","DOIUrl":"10.1016/j.ensm.2025.104232","url":null,"abstract":"<div><div>The uncontrolled deposition behavior, sluggish reaction kinetics and inefficient utilization of Al derived from unstable anode/electrolyte interface have severely impeded the development of aluminum-ion batteries. Here, we discuss the impact of interfacial electron/ion transfer on the electrochemical performance, and as an illustration, propose the construction of Cu@MXene as anodic current collector through work function engineering to simultaneously achieve homogeneous deposition morphology and rapid plating/stripping rate. The difference in work function between Cu nanoparticles and Ti3C2 MXene facilitates charge redistribution in the anode/electrolyte interface and enhances the electron availability, optimizing the interfacial electron/ion transfer behavior. This, in turn, endows Cu@MXene with elevated catalytic efficiency for desolvation reactions and robust reduction ability for the Al plating process. As a result, Cu@MXene enables a high coulombic efficiency of 99.87 % even at a high current density of 10 mA cm−2, and sustains reversible Al plating/stripping cycles for over 3200 h at a typical current density of 1 mA cm−2. Notably, by coupling graphite cathode and Cu@MXene-Al anode under a limited N/P ratio of 2.2, the full cell exhibits durable lifetime for 2000 cycles with an impressive energy density of 119.6 Wh kg−1 (based on the total mass of cathode and anode). This work highlights a fundamental understanding of interfacial interactions in the Al deposition process and offer sustainability motivations in designing highly reversible anodes for high-energy-density aluminum-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104232"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776215","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

Trade-off between reversibility and fast Zn2+ kinetics: Toward ultra-stable low-temperature aqueous zinc-ion batteries

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104229

Junye Zhang , Linlin Wang , Yuping Liao , Chen Huang , Hangtian Zhu , Juan Wang , Linying Yuan , Tianchen Shen , Shigang Lu , Luyang Chen

Despite their environmental friendliness, security and high volumetric energy density of zinc anodes, aqueous Zinc-ion batteries (AZIBs) still face poor reversibility of Zn anodes, especially under high current density, originating from various parasitic reactions induced by high activity of water. The hydrated deep eutectic electrolyte (HDEE) effectively suppresses parasitic reactions, but the electrochemical performance still needs to be optimized. Here, our research emphasized the importance of balancing enhanced reversibility and fast Zn²⁺ transfer kinetics. A new green and low-cost HDEE (Zn(ClO₄)₂·6H₂O/Glycerol) is developed, and then an optimized solvation structure [Zn(H₂O)_2.0(Gl)_1.3(ClO₄)_2.7]²⁺ can be formed by adding glycerol (Gl), which not only maintains a high Zn²⁺ diffusion coefficient (1.2 × 10⁻⁷ cm² s⁻¹), but also disrupts the bulk water network via strong H-bonding with ClO₄⁻ and water, significantly lowering the freezing point (−65 °C) and inhibiting the parasitic reactions/cathode dissolution. Furthermore, the evolution of the HDEEs solvation chemistry and its impact on the electrode/electrolyte interfacial stabilities can be understood through precise adjustments of the molar ratios of Zn(ClO₄)₂·6H₂O and Gl, molecular dynamics and COMSOL simulation. The Zn//Zn with the HDEE (Zn|HDEE|Zn cells) can cycle for ∼5000 h without short-circuiting at 1 mA cm⁻², which is roughly 12.5 times more stable than ordinary aqueous electrolyte, indicating effective suppression of parasitic reactions. The Zn//NH₄V₄O₁₀ with HDEE (Zn|HDEE|NH₄V₄O₁₀ cells) can stably cycle 3500 cycles with 120 mAh g⁻¹ at 10 A g⁻¹ at room temperature and 1000 cycles with 95 mAh g⁻¹ at 5 A g⁻¹ at a low temperature of -20 °C. This study provides a path toward the development of HDEE electrolyte and a thorough comprehension of the influence of Zn²⁺ solvation structure on reversibility.

{"title":"Trade-off between reversibility and fast Zn2+ kinetics: Toward ultra-stable low-temperature aqueous zinc-ion batteries","authors":"Junye Zhang , Linlin Wang , Yuping Liao , Chen Huang , Hangtian Zhu , Juan Wang , Linying Yuan , Tianchen Shen , Shigang Lu , Luyang Chen","doi":"10.1016/j.ensm.2025.104229","DOIUrl":"10.1016/j.ensm.2025.104229","url":null,"abstract":"<div><div>Despite their environmental friendliness, security and high volumetric energy density of zinc anodes, aqueous Zinc-ion batteries (AZIBs) still face poor reversibility of Zn anodes, especially under high current density, originating from various parasitic reactions induced by high activity of water. The hydrated deep eutectic electrolyte (HDEE) effectively suppresses parasitic reactions, but the electrochemical performance still needs to be optimized. Here, our research emphasized the importance of balancing enhanced reversibility and fast Zn2+ transfer kinetics. A new green and low-cost HDEE (Zn(ClO4)2·6H2O/Glycerol) is developed, and then an optimized solvation structure [Zn(H2O)2.0(Gl)1.3(ClO4)2.7]²⁺ can be formed by adding glycerol (Gl), which not only maintains a high Zn2+ diffusion coefficient (1.2 × 10−7 cm2 s−1), but also disrupts the bulk water network via strong H-bonding with ClO₄− and water, significantly lowering the freezing point (−65 °C) and inhibiting the parasitic reactions/cathode dissolution. Furthermore, the evolution of the HDEEs solvation chemistry and its impact on the electrode/electrolyte interfacial stabilities can be understood through precise adjustments of the molar ratios of Zn(ClO4)2·6H2O and Gl, molecular dynamics and COMSOL simulation. The Zn//Zn with the HDEE (Zn|HDEE|Zn cells) can cycle for ∼5000 h without short-circuiting at 1 mA cm−2, which is roughly 12.5 times more stable than ordinary aqueous electrolyte, indicating effective suppression of parasitic reactions. The Zn//NH4V4O10 with HDEE (Zn|HDEE|NH4V4O10 cells) can stably cycle 3500 cycles with 120 mAh g−1 at 10 A g−1 at room temperature and 1000 cycles with 95 mAh g−1 at 5 A g−1 at a low temperature of -20 °C. This study provides a path toward the development of HDEE electrolyte and a thorough comprehension of the influence of Zn2+ solvation structure on reversibility.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104229"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766696","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

Prolonged cycle life of composite cathodes via ionically permeable Li3PO4 surface engineering on conductive agents to suppress degradation of sulfide solid electrolytes

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104193

Younghoon Jo , Hongjun Chang , Chaeyeon Ha , Hyeongjun Choi , Taesun Song , Yeonghoon Kim , Janghyuk Moon , Young-Jun Kim

Sulfide-based all-solid-state batteries (ASSBs) are promising candidates for next-generation energy storage systems owing to their notable ionic conductivity and stability against explosions. However, the low chemical stability of sulfide-based solid electrolytes (SSEs) causes problems at their interfaces with other electrode components. Among them, addressing the side reactions between conductive agents and SSEs is crucial for commercialization. Herein, a conductive agent surface-modified with Li₃PO₄ is employed to enhance the interfacial stability of SSEs. Density functional theory-based analysis reveals that Li₃PO₄, characterized by strong inter-element bonding, exhibits high ionic conductivity and stability at the interface with SSEs. Electrochemical measurements confirm that Li₃PO₄-coated conductive agents suppress the interfacial decomposition of SSEs, thereby securing the targeted ionic conductivity in the composite cathode. Consequently, ASSBs adopting surface-engineered conductive agents demonstrate remarkable rate capability (153.6 mAh g⁻¹ at 2 C) and cycle performance (88.8 % retention over 1000 cycles) with a high areal capacity (4 mAh cm⁻²). This study provides a novel concept for conductive agents that enhance charge transport characteristics and mitigate SSE degradation, paving the way for the development of long cycle life ASSBs.

{"title":"Prolonged cycle life of composite cathodes via ionically permeable Li3PO4 surface engineering on conductive agents to suppress degradation of sulfide solid electrolytes","authors":"Younghoon Jo , Hongjun Chang , Chaeyeon Ha , Hyeongjun Choi , Taesun Song , Yeonghoon Kim , Janghyuk Moon , Young-Jun Kim","doi":"10.1016/j.ensm.2025.104193","DOIUrl":"10.1016/j.ensm.2025.104193","url":null,"abstract":"<div><div>Sulfide-based all-solid-state batteries (ASSBs) are promising candidates for next-generation energy storage systems owing to their notable ionic conductivity and stability against explosions. However, the low chemical stability of sulfide-based solid electrolytes (SSEs) causes problems at their interfaces with other electrode components. Among them, addressing the side reactions between conductive agents and SSEs is crucial for commercialization. Herein, a conductive agent surface-modified with Li3PO4 is employed to enhance the interfacial stability of SSEs. Density functional theory-based analysis reveals that Li3PO4, characterized by strong inter-element bonding, exhibits high ionic conductivity and stability at the interface with SSEs. Electrochemical measurements confirm that Li3PO4-coated conductive agents suppress the interfacial decomposition of SSEs, thereby securing the targeted ionic conductivity in the composite cathode. Consequently, ASSBs adopting surface-engineered conductive agents demonstrate remarkable rate capability (153.6 mAh g−1 at 2 C) and cycle performance (88.8 % retention over 1000 cycles) with a high areal capacity (4 mAh cm−2). This study provides a novel concept for conductive agents that enhance charge transport characteristics and mitigate SSE degradation, paving the way for the development of long cycle life ASSBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104193"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703032","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

Towards high-performance sodium-ion batteries: A comprehensive review on NaxNiyFezMn1−(y+z)O2 cathode materials

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104212

Alibi Namazbay , Maksat Karlykan , Lunara Rakhymbay , Zhumabay Bakenov , Natalia Voronina , Seung-Taek Myung , Aishuak Konarov

Sodium-ion batteries (SIBs) are potential candidates for next-generation grid-scale energy storage owing to their safety as well as the abundance of sodium resources. Further progress in SIB technology demands the advancement of cathode materials with outstanding performance. Among various cathode materials, layered transition metal oxides based on Ni, Fe, and Mn (NaNFM) have recently received great attention by combining the positive features of each of them. This review focuses on the most current developments in the study and design of NaNFM (Na_xNi_yFe_zMn_{1−(_y+}_z₎O₂) as a cathode material for SIBs, including synthesis methods, crystal structure/structural evolution during charge–discharging, and the effect of different molar ratios. Adjusting the transition elements enables formation in several phases that promote Na-ion diffusion, resulting in high-rate capability and cycle stability. Moreover, key strategies to improve the electrochemical performance through doping and surface modifications are discussed. Future optimization of these materials shows potential for enormous opportunities for implementing cost-effective and high-performance energy -storage technologies.

{"title":"Towards high-performance sodium-ion batteries: A comprehensive review on NaxNiyFezMn1−(y+z)O2 cathode materials","authors":"Alibi Namazbay , Maksat Karlykan , Lunara Rakhymbay , Zhumabay Bakenov , Natalia Voronina , Seung-Taek Myung , Aishuak Konarov","doi":"10.1016/j.ensm.2025.104212","DOIUrl":"10.1016/j.ensm.2025.104212","url":null,"abstract":"<div><div>Sodium-ion batteries (SIBs) are potential candidates for next-generation grid-scale energy storage owing to their safety as well as the abundance of sodium resources. Further progress in SIB technology demands the advancement of cathode materials with outstanding performance. Among various cathode materials, layered transition metal oxides based on Ni, Fe, and Mn (NaNFM) have recently received great attention by combining the positive features of each of them. This review focuses on the most current developments in the study and design of NaNFM (NaxNiyFezMn1−(y+z)O2) as a cathode material for SIBs, including synthesis methods, crystal structure/structural evolution during charge–discharging, and the effect of different molar ratios. Adjusting the transition elements enables formation in several phases that promote Na-ion diffusion, resulting in high-rate capability and cycle stability. Moreover, key strategies to improve the electrochemical performance through doping and surface modifications are discussed. Future optimization of these materials shows potential for enormous opportunities for implementing cost-effective and high-performance energy -storage technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104212"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723843","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

Polymer dielectrics intercalated with a non-contiguous granular nanolayer for high-temperature pulsed energy storage

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104213

Peng Yin , Li Lei , Qingyang Tang , Davoud Dastan , Yao Liu , Hong Wang , Zhicheng Shi

Polymer dielectrics suffer from significant degradation in energy density and charge–discharge efficiency at high temperatures, and incorporating inorganic nanofillers into polymer is the most straightforward and effective approach to ameliorate this behavior. However, the nanofillers are prone to form aggregated state driven by surface energy and electrostatic forces, compromising high-temperature energy storage performance of dielectrics. Here, we propose a unique non-contiguous granular intercalation strategy to solve the nanofiller aggregation problem. Specifically, an intercalation consisting of non-contiguous distributed aluminum@alumina (Al@AlO_x) core–shell nanoparticles is introduced into polyetherimide (PEI) matrix via sputtering reaction. It should be noted that the non-contiguous distribution of nanoparticles within the intercalation ensures discontinuous charge transport, which prevents the formation of conductive network within the nanocomposite. Additionally, benefiting from charge trap induced by wide-bandgap AlO_x shell and Coulomb blockade effect of Al core, the charge transport is significantly suppressed. The nanocomposite achieves ultrahigh energy densities of 9.0 J cm⁻³ at 150 °C and 6.2 J cm⁻³ at 200 °C, with charge–discharge efficiencies ≥ 90 %. This work offers a promising pathway for the design of high-temperature energy storage dielectrics and holds huge potential for scalable fabrication.

{"title":"Polymer dielectrics intercalated with a non-contiguous granular nanolayer for high-temperature pulsed energy storage","authors":"Peng Yin , Li Lei , Qingyang Tang , Davoud Dastan , Yao Liu , Hong Wang , Zhicheng Shi","doi":"10.1016/j.ensm.2025.104213","DOIUrl":"10.1016/j.ensm.2025.104213","url":null,"abstract":"<div><div>Polymer dielectrics suffer from significant degradation in energy density and charge–discharge efficiency at high temperatures, and incorporating inorganic nanofillers into polymer is the most straightforward and effective approach to ameliorate this behavior. However, the nanofillers are prone to form aggregated state driven by surface energy and electrostatic forces, compromising high-temperature energy storage performance of dielectrics. Here, we propose a unique non-contiguous granular intercalation strategy to solve the nanofiller aggregation problem. Specifically, an intercalation consisting of non-contiguous distributed aluminum@alumina (Al@AlOx) core–shell nanoparticles is introduced into polyetherimide (PEI) matrix via sputtering reaction. It should be noted that the non-contiguous distribution of nanoparticles within the intercalation ensures discontinuous charge transport, which prevents the formation of conductive network within the nanocomposite. Additionally, benefiting from charge trap induced by wide-bandgap AlOx shell and Coulomb blockade effect of Al core, the charge transport is significantly suppressed. The nanocomposite achieves ultrahigh energy densities of 9.0 J cm⁻3 at 150 °C and 6.2 J cm⁻3 at 200 °C, with charge–discharge efficiencies ≥ 90 %. This work offers a promising pathway for the design of high-temperature energy storage dielectrics and holds huge potential for scalable fabrication.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104213"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767710","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

Advanced design strategies for enhancing the thermal stability of Ni-rich co-free cathodes towards high-energy power lithium-ion batteries

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104216

Hao Ge , Bei Huang , Chaoyue Wang , Longhui Xie , Ruicong Pan , Xiaoman Cao , Zhijia Sun

The global market share of electric vehicles has rapidly grown from ∼10 % in 2022 to ∼18 % in 2024. However, safety issue is a crucial obstacle hindering the commercialization of high-energy lithium-ion batteries. The inferior thermal stability exhibited by high-energy Ni-rich cathodes has severely affected their practical application in LIBs. Particularly, Co in Ni-rich cathodes promotes lattice oxygen release, leading to reduced structural and thermal stability. Therefore, the development of Ni-rich Co-free cathode materials (NRCFs) is promising. Herein, the detrimental effects of Co on the thermal stability of Ni-rich layered oxides are demonstrated. Thereafter, we summarize in detail the popular modification strategies and mechanisms for enhancing the thermal stability of NRCFs. Finally, conclusions and future challenges and prospects for boosting the thermal stability of NRCFs are presented. Notably, synergistic modification strategies combining high-entropy doping and surface coating in single-crystal cathode materials is an efficient approach to significantly improve the thermal stability. Understanding the thermal stability of NRCFs has become urgent for the large-scale application of high-energy LIBs. More effective thermal safety strategies will be aroused to promote the development of next-generation power LIBs. This review aims to inspire further exploration of safer NRCFs featuring higher reversible capacity, attracting interest from both academic and industrial communities to accelerate the commercialization of NRCFs and promote the sustainable development of high-energy LIBs.

{"title":"Advanced design strategies for enhancing the thermal stability of Ni-rich co-free cathodes towards high-energy power lithium-ion batteries","authors":"Hao Ge , Bei Huang , Chaoyue Wang , Longhui Xie , Ruicong Pan , Xiaoman Cao , Zhijia Sun","doi":"10.1016/j.ensm.2025.104216","DOIUrl":"10.1016/j.ensm.2025.104216","url":null,"abstract":"<div><div>The global market share of electric vehicles has rapidly grown from ∼10 % in 2022 to ∼18 % in 2024. However, safety issue is a crucial obstacle hindering the commercialization of high-energy lithium-ion batteries. The inferior thermal stability exhibited by high-energy Ni-rich cathodes has severely affected their practical application in LIBs. Particularly, Co in Ni-rich cathodes promotes lattice oxygen release, leading to reduced structural and thermal stability. Therefore, the development of Ni-rich Co-free cathode materials (NRCFs) is promising. Herein, the detrimental effects of Co on the thermal stability of Ni-rich layered oxides are demonstrated. Thereafter, we summarize in detail the popular modification strategies and mechanisms for enhancing the thermal stability of NRCFs. Finally, conclusions and future challenges and prospects for boosting the thermal stability of NRCFs are presented. Notably, synergistic modification strategies combining high-entropy doping and surface coating in single-crystal cathode materials is an efficient approach to significantly improve the thermal stability. Understanding the thermal stability of NRCFs has become urgent for the large-scale application of high-energy LIBs. More effective thermal safety strategies will be aroused to promote the development of next-generation power LIBs. This review aims to inspire further exploration of safer NRCFs featuring higher reversible capacity, attracting interest from both academic and industrial communities to accelerate the commercialization of NRCFs and promote the sustainable development of high-energy LIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104216"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734486","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

Engineering high-performance argyrodite sulfide electrolytes via metal halide doping for all-solid-state lithium metal batteries

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104221

Yang Li , Gang Wu , Xiaomeng Fan , Dabing Li , Hong Liu , Xiaoxue Zhao , Wanqing Ren , Peng Lei , Xianyi Zhao , Xun Wang , Guoxu Wang , Lei Gao , Ce-Wen Nan , Li-Zhen Fan

Solid-state electrolytes (SSEs) play a crucial role in the operation of all-solid-state lithium metal batteries (ASSLMBs). Among them, sulfide SSEs have attracted particular attention due to their high ionic conductivity. However, the incompatibility of sulfide SSEs with lithium anodes and the inherent air instability severely impact battery cycling performance. Here, we successfully synthesize halogen-rich lithium argyrodites with the general formula Li_5.5 ₊ _3xP_1−xCu_xS_4.5Cl_1.5 ₋ _2xBr_2x. The incorporation of Cu and Br alter the spatial arrangement and electronic distribution of structure. Given that the anion disorder positively affects Li-ion dynamics, the ultrahigh ionic conductivity of 10.3 mS cm⁻¹ at room temperature has been achieved in Li_5.8P_0.9Cu_0.1S_4.5Cl_1.3Br_0.2 (LPSC-CB). Importantly, benefiting from the robust and stable interlayer, the lithium symmetric batteries deliver prolonged plating/stripping over 3000 h at 0.2 mA cm⁻². Furthermore, the density functional theory calculations were used to prove the mechanisms of high chemical stability. Notably, the LPSC-CB electrolyte has remarkable applicability in ASSLMBs. The full batteries of FeS₂/LPSC-CB/Li deliver outstanding discharge-specific capacities of 788.9 mAh g⁻¹ and robust cycling stability (>4.02 mAh cm⁻² after 200 cycles). The versatile CuBr₂ substitution in the most promising argyrodite electrolytes is considered as a valid strategy to realize high ionic conductivity and air-stabilized sulfide SSEs for large-scale applications.

{"title":"Engineering high-performance argyrodite sulfide electrolytes via metal halide doping for all-solid-state lithium metal batteries","authors":"Yang Li , Gang Wu , Xiaomeng Fan , Dabing Li , Hong Liu , Xiaoxue Zhao , Wanqing Ren , Peng Lei , Xianyi Zhao , Xun Wang , Guoxu Wang , Lei Gao , Ce-Wen Nan , Li-Zhen Fan","doi":"10.1016/j.ensm.2025.104221","DOIUrl":"10.1016/j.ensm.2025.104221","url":null,"abstract":"<div><div>Solid-state electrolytes (SSEs) play a crucial role in the operation of all-solid-state lithium metal batteries (ASSLMBs). Among them, sulfide SSEs have attracted particular attention due to their high ionic conductivity. However, the incompatibility of sulfide SSEs with lithium anodes and the inherent air instability severely impact battery cycling performance. Here, we successfully synthesize halogen-rich lithium argyrodites with the general formula Li5.5 + 3xP1−xCuxS4.5Cl1.5 − 2xBr2x. The incorporation of Cu and Br alter the spatial arrangement and electronic distribution of structure. Given that the anion disorder positively affects Li-ion dynamics, the ultrahigh ionic conductivity of 10.3 mS cm−1 at room temperature has been achieved in Li5.8P0.9Cu0.1S4.5Cl1.3Br0.2 (LPSC-CB). Importantly, benefiting from the robust and stable interlayer, the lithium symmetric batteries deliver prolonged plating/stripping over 3000 h at 0.2 mA cm−2. Furthermore, the density functional theory calculations were used to prove the mechanisms of high chemical stability. Notably, the LPSC-CB electrolyte has remarkable applicability in ASSLMBs. The full batteries of FeS2/LPSC-CB/Li deliver outstanding discharge-specific capacities of 788.9 mAh g−1 and robust cycling stability (>4.02 mAh cm−2 after 200 cycles). The versatile CuBr2 substitution in the most promising argyrodite electrolytes is considered as a valid strategy to realize high ionic conductivity and air-stabilized sulfide SSEs for large-scale applications.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104221"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737274","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

Plasma-enhanced vacancy engineering for sustainable high-performance recycled silicon in lithium-ion batteries

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104231

Dingyi Zhang , Hong Gao , Jiayi Li , Yiwen Sun , Zeshen Deng , Xinyao Yuan , Congcong Li , Tianxiao Chen , Xingwang Peng , Chao Wang , Yi Xu , Lichun Yang , Xin Guo , Yufei Zhao , Peng Huang , Yong Wang , Guoxiu Wang , Hao Liu

Silicon, renowned for its exceptional theoretical capacity, is a promising lithium-ion battery (LIB) anode material, yet its practical application is hindered by severe lithiation-induced volume expansion, structural instability, and high production costs. This study introduces a sustainable strategy to address these challenges by repurposing recycled photovoltaic (PV) silicon through a plasma-assisted vacancy engineering approach. By combining dielectric barrier discharge plasma-assisted milling with bismuth (Bi) modification, controlled vacancy defects are introduced into silicon microparticles, enhancing ion transport and mitigating internal stress. Bi further stabilizes the anode by absorbing mechanical stress and facilitating lithium-ion accommodation at vacancy sites. The resulting plasma induced silicon/carbon/bismuth composite demonstrates outstanding cycling stability and high-rate performance, retaining 1442 mA h g⁻¹ after 300 cycles at 0.5 A g⁻¹ and 525 mA h g⁻¹ after 1000 cycles at 7 A g⁻¹. This scalable and eco-friendly method not only overcomes the inherent limitations of silicon anodes but also transforms PV waste into high-performance LIB materials, advancing sustainable energy storage technologies.

{"title":"Plasma-enhanced vacancy engineering for sustainable high-performance recycled silicon in lithium-ion batteries","authors":"Dingyi Zhang , Hong Gao , Jiayi Li , Yiwen Sun , Zeshen Deng , Xinyao Yuan , Congcong Li , Tianxiao Chen , Xingwang Peng , Chao Wang , Yi Xu , Lichun Yang , Xin Guo , Yufei Zhao , Peng Huang , Yong Wang , Guoxiu Wang , Hao Liu","doi":"10.1016/j.ensm.2025.104231","DOIUrl":"10.1016/j.ensm.2025.104231","url":null,"abstract":"<div><div>Silicon, renowned for its exceptional theoretical capacity, is a promising lithium-ion battery (LIB) anode material, yet its practical application is hindered by severe lithiation-induced volume expansion, structural instability, and high production costs. This study introduces a sustainable strategy to address these challenges by repurposing recycled photovoltaic (PV) silicon through a plasma-assisted vacancy engineering approach. By combining dielectric barrier discharge plasma-assisted milling with bismuth (Bi) modification, controlled vacancy defects are introduced into silicon microparticles, enhancing ion transport and mitigating internal stress. Bi further stabilizes the anode by absorbing mechanical stress and facilitating lithium-ion accommodation at vacancy sites. The resulting plasma induced silicon/carbon/bismuth composite demonstrates outstanding cycling stability and high-rate performance, retaining 1442 mA h g⁻¹ after 300 cycles at 0.5 A g⁻¹ and 525 mA h g⁻¹ after 1000 cycles at 7 A g⁻¹. This scalable and eco-friendly method not only overcomes the inherent limitations of silicon anodes but also transforms PV waste into high-performance LIB materials, advancing sustainable energy storage technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104231"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776214","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

Advances in electrode and electrolyte materials of fiber-shaped supercapacitors for electrochemical performance improvement and applications extension

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104222

Yuchang Xue , Zhaolun Zhang , Ding Liu , Xiao Yang , Chunyang Wang , Haisheng Chen , Xinghua Zheng , Qihong Li , Ting Zhang

In wearable electronics, fiber-shaped supercapacitors (FSCs) have attracted significant attention due to their excellent flexibility and rapid charge-discharge rates. FSCs can not only conform to the body's contours during large deformations, such as twisting and stretching, but also exhibit faster charge-discharge rates and longer cycle life compared to other energy storage devices, such as lithium-ion fiber batteries and zinc-ion fiber batteries. These characteristics are critical for the durability and short-term response of wearable devices. This paper systematically reviews the latest research progress on fiber electrode materials and gel electrolytes in FSCs, providing an in-depth analysis of their advantages and limitations. To address the limitation of low energy density in FSCs, five effective strategies for optimizing electrochemical performance are discussed, with a focus on both the electrode and electrolyte systems. Furthermore, this paper summarizes recent developments and future trends in integrating multifunctionality (e.g., stretchability, biocompatibility, freeze resistance, fluorescence) and complex systems (e.g., energy harvesting and sensing systems) into single fiber devices.

{"title":"Advances in electrode and electrolyte materials of fiber-shaped supercapacitors for electrochemical performance improvement and applications extension","authors":"Yuchang Xue , Zhaolun Zhang , Ding Liu , Xiao Yang , Chunyang Wang , Haisheng Chen , Xinghua Zheng , Qihong Li , Ting Zhang","doi":"10.1016/j.ensm.2025.104222","DOIUrl":"10.1016/j.ensm.2025.104222","url":null,"abstract":"<div><div>In wearable electronics, fiber-shaped supercapacitors (FSCs) have attracted significant attention due to their excellent flexibility and rapid charge-discharge rates. FSCs can not only conform to the body's contours during large deformations, such as twisting and stretching, but also exhibit faster charge-discharge rates and longer cycle life compared to other energy storage devices, such as lithium-ion fiber batteries and zinc-ion fiber batteries. These characteristics are critical for the durability and short-term response of wearable devices. This paper systematically reviews the latest research progress on fiber electrode materials and gel electrolytes in FSCs, providing an in-depth analysis of their advantages and limitations. To address the limitation of low energy density in FSCs, five effective strategies for optimizing electrochemical performance are discussed, with a focus on both the electrode and electrolyte systems. Furthermore, this paper summarizes recent developments and future trends in integrating multifunctionality (e.g., stretchability, biocompatibility, freeze resistance, fluorescence) and complex systems (e.g., energy harvesting and sensing systems) into single fiber devices.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104222"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737280","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 superior high-temperature capacitance performance in aromatic polyetherimide with bulky fluorine substituent

IF 18.9 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2025-04-01 DOI: 10.1016/j.ensm.2025.104206

Xinru Yang, Yang Feng, Peiyan Liu, Liuhao Jiang, Shuo Zhang, Yifan Wu, Shengtao Li

The rapid development of electronic and electrical power equipment has increased the demand for dielectric materials with high-temperature energy storage performances. However, the mutual restrictions imposed by the glass transition temperature (T_g) and bandgap (E_g) limit the use of commercial polyetherimide (PEI) under extreme conditions. In this work, we propose a strategic modular structure design to balance a high T_g and large E_g by modulating the substituents in the biphenyl structure of modified PEI. Both experimental results and theoretical simulations indicates that owing to its electron-withdrawing nature, a bulky -CF₃ substituent not only increases the bandgap but also decreases the conjugation effect of the biphenyl structure, while having a minimal effect on T_g. This significantly shortens the hopping distance of the carriers, ultimately improving the high-temperature breakdown strength (E_b) and thus the capacitance performance of PEI. The modified PEI with the bulky -CF₃ achieves a discharge energy density (U_e) of 8.01 J/cm³ with an efficiency (η) of 91.9 % at 150 °C and an U_e of 5.3 J/cm³ with an η of 90.4 % at 200 °C, which exceeds the performance of most of current high-temperature dielectric polymers. The results of this study provide technical support for the developing of high-performance, flexible dielectric capacitors.

{"title":"Achieving superior high-temperature capacitance performance in aromatic polyetherimide with bulky fluorine substituent","authors":"Xinru Yang, Yang Feng, Peiyan Liu, Liuhao Jiang, Shuo Zhang, Yifan Wu, Shengtao Li","doi":"10.1016/j.ensm.2025.104206","DOIUrl":"10.1016/j.ensm.2025.104206","url":null,"abstract":"<div><div>The rapid development of electronic and electrical power equipment has increased the demand for dielectric materials with high-temperature energy storage performances. However, the mutual restrictions imposed by the glass transition temperature (Tg) and bandgap (Eg) limit the use of commercial polyetherimide (PEI) under extreme conditions. In this work, we propose a strategic modular structure design to balance a high Tg and large Eg by modulating the substituents in the biphenyl structure of modified PEI. Both experimental results and theoretical simulations indicates that owing to its electron-withdrawing nature, a bulky -CF3 substituent not only increases the bandgap but also decreases the conjugation effect of the biphenyl structure, while having a minimal effect on Tg. This significantly shortens the hopping distance of the carriers, ultimately improving the high-temperature breakdown strength (Eb) and thus the capacitance performance of PEI. The modified PEI with the bulky -CF3 achieves a discharge energy density (Ue) of 8.01 J/cm3 with an efficiency (η) of 91.9 % at 150 °C and an Ue of 5.3 J/cm3 with an η of 90.4 % at 200 °C, which exceeds the performance of most of current high-temperature dielectric polymers. The results of this study provide technical support for the developing of high-performance, flexible dielectric capacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104206"},"PeriodicalIF":18.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695827","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