The order of molecular aggregation at the donor-acceptor interface strongly affects the charge generation and extraction properties, determining the performance of organic electronic devices. Herein, we focused on bilayer organic solar cells and selected a combination of solid- and solvent-additives, namely 1-chloronaphthalene (CN) and trans-bis (dimesitylboron) stilbene (BBS), to tune the acceptor’s molecular arrangement in the bilayer active layer structure. When CN alone was added, the molecular orientation in the acceptor film changed from face-on to edge-on, and the crystallinity of the thin film significantly increased owing to the J-aggregation of the acceptor. While dual additives were used, a flocculent morphology was attained, leading to further increased crystallinity and improved order of the molecular aggregations, thus reducing the trap states in the acceptor layer. As a result, using dual additives resulted in decreased trap-assisted charge recombination and enhanced charge extraction, hence an excellent fill factor and optimum efficiency of 19.32%. The findings elucidate that morphology optimization using dual additives to strengthen the molecular arrangement order, which is a practical approach for high-performed bilayer organic solar cells.
{"title":"Molecular Order Manipulation with Dual Additives Suppressing Trap Density in Non-Fullerene Acceptors Enables Efficient Bilayer Organic Solar Cells","authors":"Zhenmin Zhao, Sein Chung, Lixing Tan, Jingjing Zhao, Yuan Liu, Xin Li, Liang Bai, Hyunji Lee, Minyoung Jeong, Kilwon Cho, Zhipeng Kan","doi":"10.1039/d4ee05070c","DOIUrl":"https://doi.org/10.1039/d4ee05070c","url":null,"abstract":"The order of molecular aggregation at the donor-acceptor interface strongly affects the charge generation and extraction properties, determining the performance of organic electronic devices. Herein, we focused on bilayer organic solar cells and selected a combination of solid- and solvent-additives, namely 1-chloronaphthalene (CN) and trans-bis (dimesitylboron) stilbene (BBS), to tune the acceptor’s molecular arrangement in the bilayer active layer structure. When CN alone was added, the molecular orientation in the acceptor film changed from face-on to edge-on, and the crystallinity of the thin film significantly increased owing to the J-aggregation of the acceptor. While dual additives were used, a flocculent morphology was attained, leading to further increased crystallinity and improved order of the molecular aggregations, thus reducing the trap states in the acceptor layer. As a result, using dual additives resulted in decreased trap-assisted charge recombination and enhanced charge extraction, hence an excellent fill factor and optimum efficiency of 19.32%. The findings elucidate that morphology optimization using dual additives to strengthen the molecular arrangement order, which is a practical approach for high-performed bilayer organic solar cells.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"139 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192674","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}
Wenhao Xu, Libo Li, Yangmingyue Zhao, Suo Li, Hang Yang, Hao Tong, Zhixuan Wang
In the pursuit of sustainable energy, lithium-ion batteries (LIBs) have revolutionized storage solutions and advanced the development of electric vehicles. However, as LIBs near their energy density limits and face raw material shortages, a critical challenge arises: enhancing battery life without compromising cost-effectiveness. This review introduces dual-ion batteries (DIBs) as an emerging technology to address these issues, garnering attention for their high operational voltages, excellent safety, and environmental friendliness. The development trajectory of DIBs is delineated with a deep dive into unexplored foundational details, including operational principles, battery potential, capacity characteristics, energy density, and electrolyte usage. The potential of interface engineering and high-stability electrolytes is emphasized, including cathode electrolyte interphase (CEI), electrochemical stability windows (ESW), and solvation structures. We also meticulously discuss the latest advancements and prospects for DIBs in quasi-solid-state electrolytes (QSSEs). This review maps out strategies to overcome existing bottlenecks, highlighting the critical importance of fundamental and detailed research to propel the practical application of DIB technology, foster a more sustainable battery ecosystem, and strengthen the drive toward renewable energy transformation.
{"title":"Some basics and details for a better dual-ion battery","authors":"Wenhao Xu, Libo Li, Yangmingyue Zhao, Suo Li, Hang Yang, Hao Tong, Zhixuan Wang","doi":"10.1039/d4ee04063e","DOIUrl":"https://doi.org/10.1039/d4ee04063e","url":null,"abstract":"In the pursuit of sustainable energy, lithium-ion batteries (LIBs) have revolutionized storage solutions and advanced the development of electric vehicles. However, as LIBs near their energy density limits and face raw material shortages, a critical challenge arises: enhancing battery life without compromising cost-effectiveness. This review introduces dual-ion batteries (DIBs) as an emerging technology to address these issues, garnering attention for their high operational voltages, excellent safety, and environmental friendliness. The development trajectory of DIBs is delineated with a deep dive into unexplored foundational details, including operational principles, battery potential, capacity characteristics, energy density, and electrolyte usage. The potential of interface engineering and high-stability electrolytes is emphasized, including cathode electrolyte interphase (CEI), electrochemical stability windows (ESW), and solvation structures. We also meticulously discuss the latest advancements and prospects for DIBs in quasi-solid-state electrolytes (QSSEs). This review maps out strategies to overcome existing bottlenecks, highlighting the critical importance of fundamental and detailed research to propel the practical application of DIB technology, foster a more sustainable battery ecosystem, and strengthen the drive toward renewable energy transformation.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"62 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258617","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}
The successive introduction of silicon (Si) graphite composite anodes into the global market highlights the tremendous commercial potential of Si anodes. Good kinetic performance related to fast charging capability is the central topic of next-generation Si anodes. However, there is a lack of critical reviews to explore the fundamental limiting factors affecting the kinetics of Si and evaluate the effectiveness of the current strategies. In this review, we deconstruct the particle-interface-electrode integration to analyze key limiting factors of kinetics from a practical application perspective for the first time, involving long Li+ diffusion distance and poor conductivity for particles, high Li+ migration impedance at the interface, and insufficient or even interrupted Li+ diffusion paths inside the electrodes. Then, the kinetics enhancement strategies on progressively addressing the above issues are systematically investigated and the quantitative relationships between kinetics and these strategies are deeply discussed. Accordingly, the necessary challenges in quantification and balance for fast-charging Si anodes are identified as the remaining issues, and potential solutions are provided. This review can provide valuable guidance on fast-charging Si anodes and suggest promising directions in commercial-oriented Si anode studies.
{"title":"Revisiting the Kinetics Enhancement Strategies of Si Anode through Deconstructing Particle-Interface-Electrode Integration","authors":"Pingshan Jia, Junpo Guo, Qing Li, Yinan Liu, Yun Zheng, Yan Guo, Yike Huang, Yingying Shen, Lifen Long, Hebin Zhang, Rong Chen, Congcong Zhang, Zhiyuan Zhang, Jingjun Shen, Shengyang Dong, Jiangmin Jiang, Meinan Chang, Xupo Liu, Xiaobing Wang, Yuxin Tang, Huaiyu Shao","doi":"10.1039/d4ee05595k","DOIUrl":"https://doi.org/10.1039/d4ee05595k","url":null,"abstract":"The successive introduction of silicon (Si) graphite composite anodes into the global market highlights the tremendous commercial potential of Si anodes. Good kinetic performance related to fast charging capability is the central topic of next-generation Si anodes. However, there is a lack of critical reviews to explore the fundamental limiting factors affecting the kinetics of Si and evaluate the effectiveness of the current strategies. In this review, we deconstruct the particle-interface-electrode integration to analyze key limiting factors of kinetics from a practical application perspective for the first time, involving long Li+ diffusion distance and poor conductivity for particles, high Li+ migration impedance at the interface, and insufficient or even interrupted Li+ diffusion paths inside the electrodes. Then, the kinetics enhancement strategies on progressively addressing the above issues are systematically investigated and the quantitative relationships between kinetics and these strategies are deeply discussed. Accordingly, the necessary challenges in quantification and balance for fast-charging Si anodes are identified as the remaining issues, and potential solutions are provided. This review can provide valuable guidance on fast-charging Si anodes and suggest promising directions in commercial-oriented Si anode studies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"15 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192369","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}
Achieving high-performance organic photovoltaics (OPVs) hinges on optimizing the phase separation and interfaces within the active layer, which is crucial for efficient charge generation and transport. While a fibril-like phase-separated network has been widely recognized as desirable morphology across various blend systems, robust methods to consistently achieve this structure remain elusive, limiting further efficiency gains. Here, we introduce a morphological control strategy using an imide-functionalized benzotriazole polymer, PTzBI-dF, within a D18:L8-BO blend to enhance fibrillar morphology. PTzBI-dF exhibits preferential miscibility with D18, fostering π-π stacking and increasing crystallinity, which result in a well-defined fibrillar network that optimizes electrical and photophysical properties. Therefore, the D18:PTzBI-dF:L8-BO device achieves a remarkable power conversion efficiency of 19.6% for 0.04 cm2 devices and a certified 18.35% for 1 cm2 devices, representing the highest value reported so far for 1 cm2 devices. Furthermore, such guest-polymer-assisted fibrillization shows versatility across various blend systems, offering a promising approach for enhancing OPV performance.
{"title":"Achieving 19.6% efficiency in organic photovoltaics through guest-polymer assisted morphological fibrillization","authors":"Zhenye Li, Jiefeng Xie, Wenquan Wang, Zhiyuan Yang, Lixuan Kan, Zaiyu Wang, Ming Zhang, Wenyu Yang, Feng Peng, Wenkai Zhong, Ying Lei","doi":"10.1039/d4ee03461a","DOIUrl":"https://doi.org/10.1039/d4ee03461a","url":null,"abstract":"Achieving high-performance organic photovoltaics (OPVs) hinges on optimizing the phase separation and interfaces within the active layer, which is crucial for efficient charge generation and transport. While a fibril-like phase-separated network has been widely recognized as desirable morphology across various blend systems, robust methods to consistently achieve this structure remain elusive, limiting further efficiency gains. Here, we introduce a morphological control strategy using an imide-functionalized benzotriazole polymer, PTzBI-dF, within a D18:L8-BO blend to enhance fibrillar morphology. PTzBI-dF exhibits preferential miscibility with D18, fostering π-π stacking and increasing crystallinity, which result in a well-defined fibrillar network that optimizes electrical and photophysical properties. Therefore, the D18:PTzBI-dF:L8-BO device achieves a remarkable power conversion efficiency of 19.6% for 0.04 cm2 devices and a certified 18.35% for 1 cm2 devices, representing the highest value reported so far for 1 cm2 devices. Furthermore, such guest-polymer-assisted fibrillization shows versatility across various blend systems, offering a promising approach for enhancing OPV performance.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258618","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}
Aqueous metal batteries are advantageous in providing high energy density and excellent compatibility with various cathode materials, attracting more attention. However, the corrosion of metallic anodes seriously deteriorates the battery performance in terms of capacity loss, retarding reaction kinetics, and shorten cycling life. This review comprehensively discusses and summarizes the fundamental corrosion mechanisms of metallic anodes in aqueous electrolytes and key influence factors. Subsequently, recent achievements in corrosion inhibition are summarized and categorized to evaluate the vantages and inferiorities of various strategies. Advanced characterization techniques are introduced in corrosion mechanism analyses and protection assessments. Current challenges in addressing the corrosion issue and potential developments in this field are also presented.
{"title":"Corrosion of metallic anodes in aqueous batteries","authors":"Xuejin Li, Pengyun Liu, Cuiping Han, Tonghui Cai, Yongpeng Cui, Wei Xing, Chunyi Zhi","doi":"10.1039/d5ee00075k","DOIUrl":"https://doi.org/10.1039/d5ee00075k","url":null,"abstract":"Aqueous metal batteries are advantageous in providing high energy density and excellent compatibility with various cathode materials, attracting more attention. However, the corrosion of metallic anodes seriously deteriorates the battery performance in terms of capacity loss, retarding reaction kinetics, and shorten cycling life. This review comprehensively discusses and summarizes the fundamental corrosion mechanisms of metallic anodes in aqueous electrolytes and key influence factors. Subsequently, recent achievements in corrosion inhibition are summarized and categorized to evaluate the vantages and inferiorities of various strategies. Advanced characterization techniques are introduced in corrosion mechanism analyses and protection assessments. Current challenges in addressing the corrosion issue and potential developments in this field are also presented.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143192372","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}
Qi Liu, Panzhe Qiao, Di Shen, Ying Xie, Baoluo Wang, Tianyu Han, Hongtu Shi, Lei Wang, Honggang Fu
Enhancing the bifunctional activity of electrocatalysts for oxygen reduction/evolution reactions (ORR/OER), along with improving water retention in gel-polymer electrolytes, is essential for developing high-performance flexible zinc–air batteries (FZABs). Herein, we synthesize a structure that combines Fe single atom sites with FeN4 configuration and clusters of four coordinated Fe atoms anchored on worm-like polypyrrole (FeSA/FeAC@PPy/CC) using an electrochemical deposition strategy. It shows a promoted bifunctional ORR/OER activity with a small potential gap of 0.694 V. Theoretical calculations indicate that Fe single atom sites lower the energy barrier of the rate-determining step for both ORR and OER, while Fe clusters optimize the energy barriers associated with oxygen-containing intermediates. The interaction between Fe single atom sites and clusters shifts the d-band center of the metal closer to the Fermi level, leading to electron depletion at the Fe centers. Such adjustment triggers a rearrangement of the orbital electrons and enhances the adsorption interaction with oxygen orbitals, thereby improving both the ORR and OER activities. Additionally, a water-locking hydrogen bonding network electrolyte composed of polyacrylamide and ethylene glycol is utilized to enhance low-temperature tolerance. Thus, the assembled FeSA/FeAC@PPy/CC-based FZAB demonstrates ultra-stable operation for 210 h at 25 °C and 167 h at −40 °C.
{"title":"Iron clusters and single atom sites cooperatively promote bifunctional oxygen reaction activity in ultra-stable flexible zinc-air battery","authors":"Qi Liu, Panzhe Qiao, Di Shen, Ying Xie, Baoluo Wang, Tianyu Han, Hongtu Shi, Lei Wang, Honggang Fu","doi":"10.1039/d4ee05508j","DOIUrl":"https://doi.org/10.1039/d4ee05508j","url":null,"abstract":"Enhancing the bifunctional activity of electrocatalysts for oxygen reduction/evolution reactions (ORR/OER), along with improving water retention in gel-polymer electrolytes, is essential for developing high-performance flexible zinc–air batteries (FZABs). Herein, we synthesize a structure that combines Fe single atom sites with FeN4 configuration and clusters of four coordinated Fe atoms anchored on worm-like polypyrrole (FeSA/FeAC@PPy/CC) using an electrochemical deposition strategy. It shows a promoted bifunctional ORR/OER activity with a small potential gap of 0.694 V. Theoretical calculations indicate that Fe single atom sites lower the energy barrier of the rate-determining step for both ORR and OER, while Fe clusters optimize the energy barriers associated with oxygen-containing intermediates. The interaction between Fe single atom sites and clusters shifts the d-band center of the metal closer to the Fermi level, leading to electron depletion at the Fe centers. Such adjustment triggers a rearrangement of the orbital electrons and enhances the adsorption interaction with oxygen orbitals, thereby improving both the ORR and OER activities. Additionally, a water-locking hydrogen bonding network electrolyte composed of polyacrylamide and ethylene glycol is utilized to enhance low-temperature tolerance. Thus, the assembled FeSA/FeAC@PPy/CC-based FZAB demonstrates ultra-stable operation for 210 h at 25 °C and 167 h at −40 °C.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"55 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124800","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}
Lin Liu, Zi-Jian Chen, Guo-Yu Zhu, Bai-Hua Huang, Bo Wang, Yu Yao, De-Shan Bin, Xianhong Rui, Yan Yu
Low concentration electrolytes (LCEs) show various advantages, such as lower cost, better wettability, wider temperature operation, and greater variety of salt species options, which have inspired numerous research interests for a series of rechargeable batteries. Recent years have witnessed numerous successes in LCEs designs, but LCEs are still in an early development stage with insufficient scientific cognition and dissatisfactory electrochemical performances. It is therefore essential to understand more about the LCEs chemistry and gain more insight into design principles if practical applications of LCEs are expected. This review outlines the current knowledge on the LCEs designs and applications for different battery systems. The solvation/desolvation behaviors of the LCEs and the interfacial structures of the electrodes are discussed with focus on the structure-function correlations. The critical issues for the applications of LCEs are highlighted and perspectives for potential strategies to accelerate the further development of LCEs with a higher level of functionality are provided. This review will spark new endeavor to build better LCEs toward practical applications for rechargeable batteries.
{"title":"Low concentration electrolytes for rechargeable batteries: A Review","authors":"Lin Liu, Zi-Jian Chen, Guo-Yu Zhu, Bai-Hua Huang, Bo Wang, Yu Yao, De-Shan Bin, Xianhong Rui, Yan Yu","doi":"10.1039/d4ee06096b","DOIUrl":"https://doi.org/10.1039/d4ee06096b","url":null,"abstract":"Low concentration electrolytes (LCEs) show various advantages, such as lower cost, better wettability, wider temperature operation, and greater variety of salt species options, which have inspired numerous research interests for a series of rechargeable batteries. Recent years have witnessed numerous successes in LCEs designs, but LCEs are still in an early development stage with insufficient scientific cognition and dissatisfactory electrochemical performances. It is therefore essential to understand more about the LCEs chemistry and gain more insight into design principles if practical applications of LCEs are expected. This review outlines the current knowledge on the LCEs designs and applications for different battery systems. The solvation/desolvation behaviors of the LCEs and the interfacial structures of the electrodes are discussed with focus on the structure-function correlations. The critical issues for the applications of LCEs are highlighted and perspectives for potential strategies to accelerate the further development of LCEs with a higher level of functionality are provided. This review will spark new endeavor to build better LCEs toward practical applications for rechargeable batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"61 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124423","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}
The utilization of high-capacity lithium-rich layered oxide (LRLO) in lithium-ion batteries is hampered by its severe interface reactions and poor interface dynamics. Herein, an OG gate (OG) is constructed on the surface of LRLO to alleviate its interface issues. The OR gate, consisted of layered hydrotalcite with a negatively charged interlayer and high dielectric constant, enable selectively enhance the Li+ transportation. Benefited from the Li+ selectivity, OG-coated LRLO shows outstanding cycle performance, with a capacity retention rate of 91.9 % after 100 cycles at 1C (from 197.9 mAh g−1 to 182.0 mAh g−1). Moreover, the OG demonstrates a good voltage-division effect and interface stability, making it suitable for solid polymer electrolyte (SPE) systems. Interestingly, when combined with an SPE, the OG-coated LRLO delivers a capacity retention rate of 80.0 % after 150 cycles at 0.2 C and an ultrahigh electrode-electrolyte energy density of 437.2 Wh Kg−1. This approach presents a simple and effective mechanism for adapting LRLO to solid-state battery, enhancing the practical utilization of high-energy-density solid-state batteries.
{"title":"Lithium-selective “OR-gate” enables fast-kinetics and ultra-stable Li-rich cathodes for polymer-based solid-state batteries","authors":"Qin Wang, Yiming Zhang, Meng Yao, Kang Li, Lv Xu, Haitao Zhang, Xiaopeng Wang, Yun Zhang","doi":"10.1039/d4ee05264a","DOIUrl":"https://doi.org/10.1039/d4ee05264a","url":null,"abstract":"The utilization of high-capacity lithium-rich layered oxide (LRLO) in lithium-ion batteries is hampered by its severe interface reactions and poor interface dynamics. Herein, an OG gate (OG) is constructed on the surface of LRLO to alleviate its interface issues. The OR gate, consisted of layered hydrotalcite with a negatively charged interlayer and high dielectric constant, enable selectively enhance the Li+ transportation. Benefited from the Li+ selectivity, OG-coated LRLO shows outstanding cycle performance, with a capacity retention rate of 91.9 % after 100 cycles at 1C (from 197.9 mAh g−1 to 182.0 mAh g−1). Moreover, the OG demonstrates a good voltage-division effect and interface stability, making it suitable for solid polymer electrolyte (SPE) systems. Interestingly, when combined with an SPE, the OG-coated LRLO delivers a capacity retention rate of 80.0 % after 150 cycles at 0.2 C and an ultrahigh electrode-electrolyte energy density of 437.2 Wh Kg−1. This approach presents a simple and effective mechanism for adapting LRLO to solid-state battery, enhancing the practical utilization of high-energy-density solid-state batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"28 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124801","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}
The electrolyte concentration plays a pivotal role in determining the efficacy of rechargeable batteries. While prior research has primarily focused on high electrolyte concentrations, the potential of dilute electrolytes remains largely unexplored. This investigation introduces a ternary electrolyte system for zinc-ion batteries, comprising water, acetonitrile (AN), and dimethyl sulfoxide (DMSO), with a remarkably low concentration of 0.3 M Zn(OTf)2. This innovative electrolyte exhibits a compelling suite of advantages, including environmental benignity, enhanced safety, cost-effectiveness, an expanded electrochemical window, high ionic conductivity, and a broad operating temperature range. The solvated structure of the ultra-low concentration electrolyte is primarily in the form of contact ion pairs (CIPs), which are made up of AN, DMSO, H2O, and OTf−. This interplay results in the formation of a unique rigid-soft coupled electrolyte interface that promotes ordered zinc plating, concurrently reducing viscosity and accelerating the migration rate of zinc ions, thereby significantly enhancing the rate performance of the battery. The symmetric cell, utilizing this electrolyte, demonstrates exceptional durability, characterized by a negligible hysteresis voltage of 32 mV after 3000 hours of cycling at a current density of 1 mA cm−2 and 1 mA h cm−2. Furthermore, the cell exhibits an impressive cycle life exceeding 8000 hours. The Zn‖W–VO2 full cell, utilizing this TSIS-0.3 electrolyte, not only maintains a capacity comparable to that achieved with a 3 M Zn(OTf)2 electrolyte, but also showcases superior cycle life and capacity retention. Notably, it retains over 92% of its capacity after 540 cycles at a current density of 0.5 A g−1. Concurrently, it can sustain the high-voltage positive ZnHCF cycle for 200 cycles at 0.2 A g−1, exhibiting a capacity retention rate above 100%. Furthermore, TSIS-0.3 facilitates the effective operation of Zn batteries across an extensive temperature range from −30 to 40 °C. Investigating low-concentration electrolytes is crucial as it enhances more selectivity for zinc salts and significantly increases the economic feasibility of zinc-ion batteries due to their low cost.
{"title":"Constructing a gradient soft-coupled SEI film using a dilute ternary electrolyte system towards high-performance zinc-ion batteries with wide temperature stability","authors":"Tiantian Wang, Yuao Wang, Peng Cui, Heshun Geng, Yusheng Wu, Fang Hu, Junhua You, Kai Zhu","doi":"10.1039/d4ee05894a","DOIUrl":"https://doi.org/10.1039/d4ee05894a","url":null,"abstract":"The electrolyte concentration plays a pivotal role in determining the efficacy of rechargeable batteries. While prior research has primarily focused on high electrolyte concentrations, the potential of dilute electrolytes remains largely unexplored. This investigation introduces a ternary electrolyte system for zinc-ion batteries, comprising water, acetonitrile (AN), and dimethyl sulfoxide (DMSO), with a remarkably low concentration of 0.3 M Zn(OTf)<small><sub>2</sub></small>. This innovative electrolyte exhibits a compelling suite of advantages, including environmental benignity, enhanced safety, cost-effectiveness, an expanded electrochemical window, high ionic conductivity, and a broad operating temperature range. The solvated structure of the ultra-low concentration electrolyte is primarily in the form of contact ion pairs (CIPs), which are made up of AN, DMSO, H<small><sub>2</sub></small>O, and OTf<small><sup>−</sup></small>. This interplay results in the formation of a unique rigid-soft coupled electrolyte interface that promotes ordered zinc plating, concurrently reducing viscosity and accelerating the migration rate of zinc ions, thereby significantly enhancing the rate performance of the battery. The symmetric cell, utilizing this electrolyte, demonstrates exceptional durability, characterized by a negligible hysteresis voltage of 32 mV after 3000 hours of cycling at a current density of 1 mA cm<small><sup>−2</sup></small> and 1 mA h cm<small><sup>−2</sup></small>. Furthermore, the cell exhibits an impressive cycle life exceeding 8000 hours. The Zn‖W–VO<small><sub>2</sub></small> full cell, utilizing this TSIS-0.3 electrolyte, not only maintains a capacity comparable to that achieved with a 3 M Zn(OTf)<small><sub>2</sub></small> electrolyte, but also showcases superior cycle life and capacity retention. Notably, it retains over 92% of its capacity after 540 cycles at a current density of 0.5 A g<small><sup>−1</sup></small>. Concurrently, it can sustain the high-voltage positive ZnHCF cycle for 200 cycles at 0.2 A g<small><sup>−1</sup></small>, exhibiting a capacity retention rate above 100%. Furthermore, TSIS-0.3 facilitates the effective operation of Zn batteries across an extensive temperature range from −30 to 40 °C. Investigating low-concentration electrolytes is crucial as it enhances more selectivity for zinc salts and significantly increases the economic feasibility of zinc-ion batteries due to their low cost.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124979","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}
Ion transport in known polymer electrolytes highly depends on the segmental motion of polymer chains and they have low ionic conductivity due to a single-ion transport pathway. Novel design paradigms are required to enhance the performance of polymer electrolytes beyond traditional systems. Here the role of an ultrasmall nanoparticle-assisted-migration is shown to significantly enhance the ionic conductivity of polyethylene oxide (PEO) polymer electrolytes. PEGylated nanoparticles with a size of much smaller than the gyration radius of the PEO chain diffuse rapidly within the PEO matrix and function as ion nanorobots for the transport of Li-ions. The ultrasmall nanoparticles also act as lubricants that further enhance the chain mobility of the bulk PEO backbone. The ultrasmall nanoparticle migration synergistically with accelerated segmental motion of the PEO form a dual-channel Li+ transport pathway, leading to an increase of the Li+ conductivity of the PEO-based electrolyte by three orders of magnitude. The electrolyte enables stable symmetric cell-cycling performance of > 1800 h and long-term charge/discharge stability for 980 cycles when used a Li|LiFePO4 full battery at 50 °C. This work highlights the potential of activating hopping of nanoparticles in composite polymer electrolytes to construct high-performance polymer-based all-solid-state battery.
{"title":"Li-Ion Nanorobots with Enhanced Mobility for Fast-Ion Conducting Polymer Electrolytes","authors":"Mingshen Tu, Ziheng Wang, Qionghai Chen, Zaiping Guo, Feifei Cao, Huan Ye","doi":"10.1039/d4ee05881j","DOIUrl":"https://doi.org/10.1039/d4ee05881j","url":null,"abstract":"Ion transport in known polymer electrolytes highly depends on the segmental motion of polymer chains and they have low ionic conductivity due to a single-ion transport pathway. Novel design paradigms are required to enhance the performance of polymer electrolytes beyond traditional systems. Here the role of an ultrasmall nanoparticle-assisted-migration is shown to significantly enhance the ionic conductivity of polyethylene oxide (PEO) polymer electrolytes. PEGylated nanoparticles with a size of much smaller than the gyration radius of the PEO chain diffuse rapidly within the PEO matrix and function as ion nanorobots for the transport of Li-ions. The ultrasmall nanoparticles also act as lubricants that further enhance the chain mobility of the bulk PEO backbone. The ultrasmall nanoparticle migration synergistically with accelerated segmental motion of the PEO form a dual-channel Li+ transport pathway, leading to an increase of the Li+ conductivity of the PEO-based electrolyte by three orders of magnitude. The electrolyte enables stable symmetric cell-cycling performance of > 1800 h and long-term charge/discharge stability for 980 cycles when used a Li|LiFePO4 full battery at 50 °C. This work highlights the potential of activating hopping of nanoparticles in composite polymer electrolytes to construct high-performance polymer-based all-solid-state battery.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"25 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124799","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}