Moonsu Yoon, Jin-sung Park, Weiyin Chen, Yimeng Huang, Tao Dai, Yumin Lee, Jungmin Shin, Seungmi Lee, Yongil Kim, Dongsoo Lee, Daiha Shin, Jaephil Cho, Yanhao Dong, Ju Li
The rapid growth in lithium-ion battery technology underscores the urgent need for sustainable recycling to address the environmental and economic challenges of battery wastes. This study introduces a liquified-salts-assisted upcycling approach to transform spent medium-Ni cathodes into high-performance Ni-rich single-crystalline cathodes. Utilizing LiOH‒LiNO3‒ Ni(NO3)2·6H2O eutectic, this method leverages planetary centrifugal mixing to create a liquid-like environment for accelerated elemental diffusion and microstructural refinement. The in situ liquification of these salts ensures seamless precursor integration, achieving compositional uniformity and minimizing impurity formation. Compared to conventional solid-state methods, our method significantly suppresses rock-salt phase formation, and improves electrochemical performance with superior cycling stability and rate capability. The environmental and economic advantages of our approach highlight its potential to reduce greenhouse gas emissions and energy consumption. This scalable, energy-efficient strategy offers a transformative solution for battery waste management, paving the way for the sustainable production of next-generation cathode materials.
{"title":"Upcycling spent medium-Ni cathodes via novel liquified salts sourcing","authors":"Moonsu Yoon, Jin-sung Park, Weiyin Chen, Yimeng Huang, Tao Dai, Yumin Lee, Jungmin Shin, Seungmi Lee, Yongil Kim, Dongsoo Lee, Daiha Shin, Jaephil Cho, Yanhao Dong, Ju Li","doi":"10.1039/d5ee01086a","DOIUrl":"https://doi.org/10.1039/d5ee01086a","url":null,"abstract":"The rapid growth in lithium-ion battery technology underscores the urgent need for sustainable recycling to address the environmental and economic challenges of battery wastes. This study introduces a liquified-salts-assisted upcycling approach to transform spent medium-Ni cathodes into high-performance Ni-rich single-crystalline cathodes. Utilizing LiOH‒LiNO<small><sub>3</sub></small>‒ Ni(NO<small><sub>3</sub></small>)<small><sub>2</sub></small>·6H<small><sub>2</sub></small>O eutectic, this method leverages planetary centrifugal mixing to create a liquid-like environment for accelerated elemental diffusion and microstructural refinement. The in situ liquification of these salts ensures seamless precursor integration, achieving compositional uniformity and minimizing impurity formation. Compared to conventional solid-state methods, our method significantly suppresses rock-salt phase formation, and improves electrochemical performance with superior cycling stability and rate capability. The environmental and economic advantages of our approach highlight its potential to reduce greenhouse gas emissions and energy consumption. This scalable, energy-efficient strategy offers a transformative solution for battery waste management, paving the way for the sustainable production of next-generation cathode materials.<span><style>text-decoration:underline\"</style><small><sup></sup></small></span>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"38 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806159","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}
Junming Kang, Jiajia Zhang, Wan Wang, Zhimin Zhai, Ganxiong Liu, Ying Ge, Lequan Wang, Chao Wang, Hongbin Lu
Aqueous zinc-iodine (Zn-I2) batteries are highly desirable for grid energy storage but subjected to polyiodide shuttling, which leads to low Coulombic efficiency (less than 98%), severe self-discharge (over 10% after 2 days) and low iodine utilization (below 80%). In this study, we in-situ constructed a dynamic interlayer on the cathode surface using an electrolyte additive that can rapidly reacts with polyiodides. This interlayer effectively prevents polyiodide dissolution and migration in the electrolyte, achieving a high Coulombic efficiency of 99.8% at 0.2 A g–1 and an ultralow self-discharge rate of 2.9% after 7 days of resting. Remarkably, the interlayer also exhibits good electrochemical activity during cycling. The reacted polyiodides can be reduced to I⁻ ions during discharge, contributing to the cell capacity and improving iodine utilization rate to 89.1% at a high capacity of 2.9 mAh cm–2. Moreover, the additive greatly enhances zinc plating behavior, resulting in an extended cycle life of over 36,000 without capacity decay at 5.0 A g–1. At a high mass loading of 15 mg cm–2 and a low N/P ratio of 1.85, the battery shows 100% capacity retention after 330 cycles with an impressive energy density of 98 Wh kg–1.
{"title":"Dynamic Cathode Interlayer for Ultralow Self-Discharge and High Iodide Utilization in Zinc-Iodine Batteries","authors":"Junming Kang, Jiajia Zhang, Wan Wang, Zhimin Zhai, Ganxiong Liu, Ying Ge, Lequan Wang, Chao Wang, Hongbin Lu","doi":"10.1039/d4ee05584e","DOIUrl":"https://doi.org/10.1039/d4ee05584e","url":null,"abstract":"Aqueous zinc-iodine (Zn-I<small><sub>2</sub></small>) batteries are highly desirable for grid energy storage but subjected to polyiodide shuttling, which leads to low Coulombic efficiency (less than 98%), severe self-discharge (over 10% after 2 days) and low iodine utilization (below 80%). In this study, we in-situ constructed a dynamic interlayer on the cathode surface using an electrolyte additive that can rapidly reacts with polyiodides. This interlayer effectively prevents polyiodide dissolution and migration in the electrolyte, achieving a high Coulombic efficiency of 99.8% at 0.2 A g<small><sup>–1</sup></small> and an ultralow self-discharge rate of 2.9% after 7 days of resting. Remarkably, the interlayer also exhibits good electrochemical activity during cycling. The reacted polyiodides can be reduced to I⁻ ions during discharge, contributing to the cell capacity and improving iodine utilization rate to 89.1% at a high capacity of 2.9 mAh cm<small><sup>–2</sup></small>. Moreover, the additive greatly enhances zinc plating behavior, resulting in an extended cycle life of over 36,000 without capacity decay at 5.0 A g<small><sup>–1</sup></small>. At a high mass loading of 15 mg cm<small><sup>–2</sup></small> and a low N/P ratio of 1.85, the battery shows 100% capacity retention after 330 cycles with an impressive energy density of 98 Wh kg<small><sup>–1</sup></small>.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"25 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806160","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}
Uncontrollable dendrite growth and parasitic reactions lead to poor reversibility of zinc (Zn) anodes, which seriously hinders the commercialization of aqueous Zn metal batteries. A promising strategy to address these issues is to rationally regulate the preferred orientation of crystal planes and form compact layers during the deposition process. Herein, the host-guest interaction in supramolecular chemistry is reported to induce (002)-texture preferred Zn deposition. It is demonstrated that the supramolecular complex units synergistically enhance the selectivity and adsorption ability for Zn crystal planes, facilitating homogeneous Zn(002) deposition at high current densities and areal capacities. Meanwhile, the steric hindrance at the interface of the order-anchored supramolecular complex units on the Zn surface not only constructs a water-poor microenvironment to effectively inhibit aggressive side reactions, but also functions as an ionic buffer zone to moderate the rapid electrochemical redox kinetics, thus homogenizing the ionic fluid and electric field. Benefitting from the above advantages of the supramolecular complex units, the assembled Zn symmetric cell exhibits remarkable cycling stability (5800 h, equal to 241 days). In the cyclic-intermittent testing mode, the symmetric cell still operates stably with a cumulative resting time of 1750 h, showing an exceptional anti-calendar aging performance. Furthermore, the assembled Zn/MnO2 pouch cell achieves a long lifespan (1000 cycles at 1 A g−1) with a capacity retention of 84.9%. Therefore, this strategy of constructing supramolecular complex units to regulate the crystal orientation is expected to shed new light on aqueous battery chemistry.
{"title":"Synergistically enhancing the selective adsorption for crystal planes to regulate the (002)-texture preferred Zn deposition via supramolecular host-guest units","authors":"Lequan Wang, Yizhen Shao, Zhongheng Fu, Xianfu Zhang, Junming Kang, Xingxiu Yang, Zhimin Zhai, Ying Ge, Long Zhang, Yanglong Hou, Hongbin Lu","doi":"10.1039/d5ee00763a","DOIUrl":"https://doi.org/10.1039/d5ee00763a","url":null,"abstract":"Uncontrollable dendrite growth and parasitic reactions lead to poor reversibility of zinc (Zn) anodes, which seriously hinders the commercialization of aqueous Zn metal batteries. A promising strategy to address these issues is to rationally regulate the preferred orientation of crystal planes and form compact layers during the deposition process. Herein, the host-guest interaction in supramolecular chemistry is reported to induce (002)-texture preferred Zn deposition. It is demonstrated that the supramolecular complex units synergistically enhance the selectivity and adsorption ability for Zn crystal planes, facilitating homogeneous Zn(002) deposition at high current densities and areal capacities. Meanwhile, the steric hindrance at the interface of the order-anchored supramolecular complex units on the Zn surface not only constructs a water-poor microenvironment to effectively inhibit aggressive side reactions, but also functions as an ionic buffer zone to moderate the rapid electrochemical redox kinetics, thus homogenizing the ionic fluid and electric field. Benefitting from the above advantages of the supramolecular complex units, the assembled Zn symmetric cell exhibits remarkable cycling stability (5800 h, equal to 241 days). In the cyclic-intermittent testing mode, the symmetric cell still operates stably with a cumulative resting time of 1750 h, showing an exceptional anti-calendar aging performance. Furthermore, the assembled Zn/MnO2 pouch cell achieves a long lifespan (1000 cycles at 1 A g−1) with a capacity retention of 84.9%. Therefore, this strategy of constructing supramolecular complex units to regulate the crystal orientation is expected to shed new light on aqueous battery chemistry.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"183 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806163","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}
Angel T. Garcia-Esparza, Xiang Li, Finn Babbe, Jinkyu Lim, K. Dean Skoien, Philipp Stefan Simon, Junko Yano, Dimosthenis Sokaras
Accessing the electrode-electrolyte interface under operating conditions and capturing time-resolved kinetics challenge electrochemical studies. Copper’s interfacial oxidation dynamics remain unclear despite extensive research. Modulation excitation X-ray absorption spectroscopy (ME-XAS) probes Cu in 100 mM KHCO₃ with sub-second sensitivity, revealing hydroxide forming 30±10 ms before Cu₂O at positive potentials (0 to 0.5 V RHE) near open-circuit conditions. From -0.4 to 0.8 V RHE, hydroxide reaches 49% with balanced Cu(I) and Cu(II) oxides. These insights into Cu interfacial redox under intermittent renewable energy operation—relevant to CO₂ electrolyzer durability—enhance our fundamental understanding of electrochemical interfaces.
{"title":"The electrode-electrolyte interface of Cu via modulation excitation X-ray absorption spectroscopy","authors":"Angel T. Garcia-Esparza, Xiang Li, Finn Babbe, Jinkyu Lim, K. Dean Skoien, Philipp Stefan Simon, Junko Yano, Dimosthenis Sokaras","doi":"10.1039/d5ee01068c","DOIUrl":"https://doi.org/10.1039/d5ee01068c","url":null,"abstract":"Accessing the electrode-electrolyte interface under operating conditions and capturing time-resolved kinetics challenge electrochemical studies. Copper’s interfacial oxidation dynamics remain unclear despite extensive research. Modulation excitation X-ray absorption spectroscopy (ME-XAS) probes Cu in 100 mM KHCO₃ with sub-second sensitivity, revealing hydroxide forming 30±10 ms before Cu₂O at positive potentials (0 to 0.5 V RHE) near open-circuit conditions. From -0.4 to 0.8 V RHE, hydroxide reaches 49% with balanced Cu(I) and Cu(II) oxides. These insights into Cu interfacial redox under intermittent renewable energy operation—relevant to CO₂ electrolyzer durability—enhance our fundamental understanding of electrochemical interfaces.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806456","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}
Ru Guo, Hang Luo, Shaoshuai He, Xin Xia, Tingting Hou, Haoyu WANG, Chaojie Chen, Dou Zhang, Yunlong Zi
The state-of-the-art studies have promoted the output energy density of the triboelectric nanogenerator (TENG) to be 10^5 J m^-3 level, while the current major barrier lies on the breakdown discharge limit. The universal performance metrics to reveal the maximized energy output ability of TENG approaching the breakdown limit are highly desirable, yet remaining a major challenge. Herein, this work proposed performance metrics for charge density and output energy density, quantitatively characterizing the output performance based on sliding-freestanding TENG with charge excitation strategy. A series of parameters of different dielectric materials were systematically investigated to reveal their impacts on the performance metrics. Consequently, the maximum output energy density of 10 kinds tribo-dielectrics were evaluated based on voltage-charge (V-Q) curve, validating the proposed performance metrics. Guided by this new standard, we developed a stretched P(VDF-TrFE) film with synergistically improved permittivity and breakdown strength, achieving record-high charge density and output energy density of 2.8 mC m^-2 and 6.2×10^5 J m^-3, respectively. Furthermore, a self-driven charge excitation system is explored in rotary-mode TENGs, showing excellent output capability to light up 15 series bulbs directly. This work establishes a basic standard and guideline for improving the TENG’s energy output, highlighting TENG’s potential applications for energy harvesting.
{"title":"Performance Metrics of Triboelectric Nanogenerator toward Record-High Output Energy Density","authors":"Ru Guo, Hang Luo, Shaoshuai He, Xin Xia, Tingting Hou, Haoyu WANG, Chaojie Chen, Dou Zhang, Yunlong Zi","doi":"10.1039/d5ee00376h","DOIUrl":"https://doi.org/10.1039/d5ee00376h","url":null,"abstract":"The state-of-the-art studies have promoted the output energy density of the triboelectric nanogenerator (TENG) to be 10^5 J m^-3 level, while the current major barrier lies on the breakdown discharge limit. The universal performance metrics to reveal the maximized energy output ability of TENG approaching the breakdown limit are highly desirable, yet remaining a major challenge. Herein, this work proposed performance metrics for charge density and output energy density, quantitatively characterizing the output performance based on sliding-freestanding TENG with charge excitation strategy. A series of parameters of different dielectric materials were systematically investigated to reveal their impacts on the performance metrics. Consequently, the maximum output energy density of 10 kinds tribo-dielectrics were evaluated based on voltage-charge (V-Q) curve, validating the proposed performance metrics. Guided by this new standard, we developed a stretched P(VDF-TrFE) film with synergistically improved permittivity and breakdown strength, achieving record-high charge density and output energy density of 2.8 mC m^-2 and 6.2×10^5 J m^-3, respectively. Furthermore, a self-driven charge excitation system is explored in rotary-mode TENGs, showing excellent output capability to light up 15 series bulbs directly. This work establishes a basic standard and guideline for improving the TENG’s energy output, highlighting TENG’s potential applications for energy harvesting.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"75 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806162","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}
Muhammad Ali, Abubakar Isah, Nurudeen Yekeen, Aliakbar Hassanpouryouzband, Mohammad Sarmadivaleh, Rita Okoroafor, Mohammed Al Kobaisi, Mohamed Mahmoud, Volker Vahrenkamp, Hussein Hoteit
With the global population anticipated to reach 9.9 billion by 2050 and rapid industrialization and economic growth, global energy demand is projected to increase by nearly 50%. Fossil fuels meet 80% of this demand, resulting in considerable greenhouse gas emissions and environmental challenges. Hydrogen (H2) offers a promising alternative due to its potential for clean combustion and integration into renewable energy systems. Underground H2 storage (UHS) enables long-term, large-scale storage to achieve equilibrium between seasonal supply and demand. This review synthesizes recent advancements in UHS, highlighting progress and persistent challenges. The review explores the complex mechanisms of H2 trapping and its implications for storage security and efficiency. The challenges these mechanisms present compared to other gases are discussed, emphasizing the unique properties of H2. The exploration covers interactions between H2 and geological formations, focusing on the wettability, interfacial tension, and sorption characteristics of rock–H2–brine systems. Advanced experimental methods are evaluated alongside the effects of critical parameters, including temperature, pressure, salinity, and organic contaminants. Findings from innovative imaging, core-flooding techniques, and computational methods (e.g., molecular dynamics simulations and machine learning) are incorporated. These approaches are vital for understanding H2 behavior in subsurface environments and developing robust, efficient storage solutions. This review offers a comprehensive update on recent progress, identifying and addressing the remaining gaps in UHS research. This work also highlights the significance of interdisciplinary research and technological innovation in overcoming these challenges. By providing insight into recent theoretical research, practical applications, and technological development, the findings support the successful incorporation of H2 into the global energy infrastructure, contributing to implementing a sustainable H2 economy successfully and fostering energy security and environmental protection for future generations.
{"title":"Recent Progress in Underground Hydrogen Storage","authors":"Muhammad Ali, Abubakar Isah, Nurudeen Yekeen, Aliakbar Hassanpouryouzband, Mohammad Sarmadivaleh, Rita Okoroafor, Mohammed Al Kobaisi, Mohamed Mahmoud, Volker Vahrenkamp, Hussein Hoteit","doi":"10.1039/d4ee04564e","DOIUrl":"https://doi.org/10.1039/d4ee04564e","url":null,"abstract":"With the global population anticipated to reach 9.9 billion by 2050 and rapid industrialization and economic growth, global energy demand is projected to increase by nearly 50%. Fossil fuels meet 80% of this demand, resulting in considerable greenhouse gas emissions and environmental challenges. Hydrogen (H2) offers a promising alternative due to its potential for clean combustion and integration into renewable energy systems. Underground H2 storage (UHS) enables long-term, large-scale storage to achieve equilibrium between seasonal supply and demand. This review synthesizes recent advancements in UHS, highlighting progress and persistent challenges. The review explores the complex mechanisms of H2 trapping and its implications for storage security and efficiency. The challenges these mechanisms present compared to other gases are discussed, emphasizing the unique properties of H2. The exploration covers interactions between H2 and geological formations, focusing on the wettability, interfacial tension, and sorption characteristics of rock–H2–brine systems. Advanced experimental methods are evaluated alongside the effects of critical parameters, including temperature, pressure, salinity, and organic contaminants. Findings from innovative imaging, core-flooding techniques, and computational methods (e.g., molecular dynamics simulations and machine learning) are incorporated. These approaches are vital for understanding H2 behavior in subsurface environments and developing robust, efficient storage solutions. This review offers a comprehensive update on recent progress, identifying and addressing the remaining gaps in UHS research. This work also highlights the significance of interdisciplinary research and technological innovation in overcoming these challenges. By providing insight into recent theoretical research, practical applications, and technological development, the findings support the successful incorporation of H2 into the global energy infrastructure, contributing to implementing a sustainable H2 economy successfully and fostering energy security and environmental protection for future generations.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"26 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797669","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 development of high-capacity anodes is of paramount importance to address the rapidly increasing demand for high-energy-density lithium-ion batteries (LIBs). While the commercialization of nanoscale silicon (Si) and microscale silicon monoxide (SiO) anodes represents a significant milestone, their widespread adoption remains constrained by challenges such as high production costs, severe interfacial side reactions, and substantial initial capacity losses. Recently, a new class of micro-sized Si-C anodes has emerged, fabricated via the co-pyrolysis of silane and gaseous hydrocarbons into porous carbon scaffolds using chemical vapor deposition (CVD). These anodes demonstrate promising performance and improved economic viability. However, the unclear mechanisms governing their structural and interfacial evolution pose significant barriers to their practical application. In this perspective, we critically summarize recent advances in understanding the intrinsic phase transition properties and the dynamic evolution of the solid-electrolyte interphase (SEI), with particular emphasis on the “breathing” effect of the SEI during cycling that leads to failure. From both dynamic and static perspectives, we highlight various strategies to address these challenges, especially under demanding conditions such as fast charging and extreme temperatures (high and low). By providing a comprehensive framework for addressing these issues, this perspective aims to offer valuable insights into enhancing the overall performance of this emerging class of anodes and accelerating their industrial adoption.
{"title":"Micro-Sized CVD-Derived Si-C Anodes: Challenges, Strategies, and Prospects for Next-Generation High-Energy Lithium-Ion Batteries","authors":"Zhexi Xiao, Haojun Wu, Lijiao Quan, Fanghong Zeng, Ruoyu Guo, Zekai Ma, Xiaoyu Chen, Jiaqi Zhan, Kang Xu, Lidan Xing, Weishan Li","doi":"10.1039/d5ee01568e","DOIUrl":"https://doi.org/10.1039/d5ee01568e","url":null,"abstract":"The development of high-capacity anodes is of paramount importance to address the rapidly increasing demand for high-energy-density lithium-ion batteries (LIBs). While the commercialization of nanoscale silicon (Si) and microscale silicon monoxide (SiO) anodes represents a significant milestone, their widespread adoption remains constrained by challenges such as high production costs, severe interfacial side reactions, and substantial initial capacity losses. Recently, a new class of micro-sized Si-C anodes has emerged, fabricated via the co-pyrolysis of silane and gaseous hydrocarbons into porous carbon scaffolds using chemical vapor deposition (CVD). These anodes demonstrate promising performance and improved economic viability. However, the unclear mechanisms governing their structural and interfacial evolution pose significant barriers to their practical application. In this perspective, we critically summarize recent advances in understanding the intrinsic phase transition properties and the dynamic evolution of the solid-electrolyte interphase (SEI), with particular emphasis on the “breathing” effect of the SEI during cycling that leads to failure. From both dynamic and static perspectives, we highlight various strategies to address these challenges, especially under demanding conditions such as fast charging and extreme temperatures (high and low). By providing a comprehensive framework for addressing these issues, this perspective aims to offer valuable insights into enhancing the overall performance of this emerging class of anodes and accelerating their industrial adoption.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"37 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797677","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 development of high-capacity, quick-charging, long-lasting cathodes are crucial for the advancement of aqueous zinc ion battery (AZIBs). However, it is still challenging for most developed electrodes to simultaneously satisfy these interconnected requirements. Starting from the customized high-crystalline material by physical vapor transport method, this report unlocks the design of unique VSSe-V2O5 core-shell composite with the crystalline-amorphous characteristic, which was enabled by electrochemical scanning of VSSe to form the amorphous heterogeneous surface. In detail, the superior conductivity of metallic VSSe core directly facilitate rapid electron transfer. Meanwhile, the amorphous V2O5 shell presents prominent hydrophilic and zincophilic traits that bolster spontaneous adsorption of zinc ion. When at the heterogeneous interface, the interaction between VSSe and V2O5 generates a unique built-in electric field, enhancing rectification behavior from the core outward. Benefited from such crystalline-amorphous core-shell heterogeneous structure, this electrode displays superior rate performance with a discharge capacity of 162 mAh g-1 at ultrahigh current density of 50 A g-1. Beyond that, it enables delivering a specific capacity of 176 mAh g-1 at 30 A g-1 with a remarkable 17000-cycle lifespan and a capacity retention of 93%. In addition, such customized paradigm can be extended to other VS0.5Se1.5, VS1.5Se0.5, and MnS0.5Se0.5 materials. This work underscores the impressive storage performance of the crystalline-amorphous rectifying heterogeneous cathode, and highlighting the surface amorphous heterogenization of customized material as a promising direction for developing robust cathodes and advanced aqueous zinc-ion batteries.
{"title":"Customizable Crystalline-Amorphous Rectifying Heterostructure Cathodes for Durable and Super-Fast Zinc Storage","authors":"Ming Yang, Mingyan Chuai, Mengnan Lai, Jianhui Zhu, Yanyi Wang, Qicheng Hu, Minfeng Chen, Jizhang Chen, Kang Fang, Guoliang Chai, Hongwei Mi, Lingna Sun, Chuanxin He, Dingtao Ma, Peixin Zhang","doi":"10.1039/d5ee00304k","DOIUrl":"https://doi.org/10.1039/d5ee00304k","url":null,"abstract":"The development of high-capacity, quick-charging, long-lasting cathodes are crucial for the advancement of aqueous zinc ion battery (AZIBs). However, it is still challenging for most developed electrodes to simultaneously satisfy these interconnected requirements. Starting from the customized high-crystalline material by physical vapor transport method, this report unlocks the design of unique VSSe-V2O5 core-shell composite with the crystalline-amorphous characteristic, which was enabled by electrochemical scanning of VSSe to form the amorphous heterogeneous surface. In detail, the superior conductivity of metallic VSSe core directly facilitate rapid electron transfer. Meanwhile, the amorphous V2O5 shell presents prominent hydrophilic and zincophilic traits that bolster spontaneous adsorption of zinc ion. When at the heterogeneous interface, the interaction between VSSe and V2O5 generates a unique built-in electric field, enhancing rectification behavior from the core outward. Benefited from such crystalline-amorphous core-shell heterogeneous structure, this electrode displays superior rate performance with a discharge capacity of 162 mAh g-1 at ultrahigh current density of 50 A g-1. Beyond that, it enables delivering a specific capacity of 176 mAh g-1 at 30 A g-1 with a remarkable 17000-cycle lifespan and a capacity retention of 93%. In addition, such customized paradigm can be extended to other VS0.5Se1.5, VS1.5Se0.5, and MnS0.5Se0.5 materials. This work underscores the impressive storage performance of the crystalline-amorphous rectifying heterogeneous cathode, and highlighting the surface amorphous heterogenization of customized material as a promising direction for developing robust cathodes and advanced aqueous zinc-ion batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"59 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143797670","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 rapid growth of the crystalline silicon (Si) photovoltaic industry has led to a steady increase in the production of waste silicon (wSi) generated during the cutting of Si ingots. Nevertheless, intrinsic oxidation and trace impurities in wSi make it difficult to retain or enhance its value for further use. Herein, we proposed a value-added recycling strategy to flash convert wSi into high performance amorphous Si nanowires (a-SiNWs). This method fully leverages the intrinsic oxidation properties of wSi and utilizes a high temperature gradient thermal field generated by carbon thermal shock to drive the directional diffusion of Si atoms within an oxide-limited domain environment. Copper nanoparticles are introduced to modulate the surface energy of Si atoms, inducing the formation of a-SiNWs. The a-SiNWs grow in situ on a carbon substrate, forming a self-supporting electrode material (identified as a-SiNWs@CC). The prepared a-SiNWs@CC is directly used as the anode of lithium-ion batteries, demonstrating excellent initial coulombic efficiency (ICE, 91.35%) and lithium storage capacity (up to 2150 mA h g−1 at 2 A g−1 for more than 250 cycles). The results hold great promise for the high-value utilization of wSi and the development of Si anodes.
{"title":"Conversion of photovoltaic waste silicon into amorphous silicon nanowire anodes","authors":"Liao Shen, Kaiwen Sun, Fengshuo Xi, Zhitao Jiang, Shaoyuan Li, Yanfeng Wang, Zhongqiu Tong, Jijun Lu, Wenhui Ma, Martin A. Green, Xiaojing Hao","doi":"10.1039/d5ee00020c","DOIUrl":"https://doi.org/10.1039/d5ee00020c","url":null,"abstract":"The rapid growth of the crystalline silicon (Si) photovoltaic industry has led to a steady increase in the production of waste silicon (wSi) generated during the cutting of Si ingots. Nevertheless, intrinsic oxidation and trace impurities in wSi make it difficult to retain or enhance its value for further use. Herein, we proposed a value-added recycling strategy to flash convert wSi into high performance amorphous Si nanowires (a-SiNWs). This method fully leverages the intrinsic oxidation properties of wSi and utilizes a high temperature gradient thermal field generated by carbon thermal shock to drive the directional diffusion of Si atoms within an oxide-limited domain environment. Copper nanoparticles are introduced to modulate the surface energy of Si atoms, inducing the formation of a-SiNWs. The a-SiNWs grow <em>in situ</em> on a carbon substrate, forming a self-supporting electrode material (identified as a-SiNWs@CC). The prepared a-SiNWs@CC is directly used as the anode of lithium-ion batteries, demonstrating excellent initial coulombic efficiency (ICE, 91.35%) and lithium storage capacity (up to 2150 mA h g<small><sup>−1</sup></small> at 2 A g<small><sup>−1</sup></small> for more than 250 cycles). The results hold great promise for the high-value utilization of wSi and the development of Si anodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"59 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143789713","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}
Anion regulation to generate LiF-rich solid electrolyte interfaces (SEIs) represents a highly effective, convenient, and economical approach. The anion decomposition process is influenced by charge density and anion concentration. However, current research primarily concentrates on increasing charge density to enhance anion decomposition. Herein, the spontaneous cascade optimization strategy driven by the double enrichment of anions and charges is proposed by utilizing NH2-MIL-101(Fe)@Copc (MOF@Copc). Specifically, NH2-MIL-101(Fe) functions as the TFSI- anion trap via the Lewis acid-base interactions and synergistic hydrogen bonding, thereby achieving primary optimization. Subsequently, the rich electronic structure of Copc facilitates charge delocalization and lowers the energy barrier for anion decomposition, allowing the C-F bonding to break more readily, thereby enabling further optimization. The π-π stacking interaction between the MOF and Copc facilitates the close association of adsorption and catalytic sites, allowing the continuous breakdown of the C- F series products in a chain reaction. The assembled LFP (19.26 mg cm⁻²) demonstrates a commercial-grade cathode area capacity, maintaining over 90% capacity retention across 350 cycles at 1 C, with a capacity decay rate of only 0.02% per cycle. More importantly, this strategy enables the industrial-scale production of Ah-class anode-free lithium-metal pouch batteries exceeding 300 Wh kg-1. Optimizing anion decomposition provides a novel perspective to advance the practical application of lithium-metal batteries.
{"title":"The Spontaneous Cascade Optimization Strategy of the Double Enrichment Improves Anion-Derived Solid Electrolyte Interphases to Enable Stable Lithium-Metal Batteries","authors":"Fengxu Zhen, Hong Liu, Yingbin Wu, Xinjia Zhou, Weiping Lin, Yuzhi Chen, Yuke Zhou, Haoyang Wang, Xiangkai Yin, Shujiang Ding, Xiaodong Chen, Wei Yu","doi":"10.1039/d5ee01219h","DOIUrl":"https://doi.org/10.1039/d5ee01219h","url":null,"abstract":"Anion regulation to generate LiF-rich solid electrolyte interfaces (SEIs) represents a highly effective, convenient, and economical approach. The anion decomposition process is influenced by charge density and anion concentration. However, current research primarily concentrates on increasing charge density to enhance anion decomposition. Herein, the spontaneous cascade optimization strategy driven by the double enrichment of anions and charges is proposed by utilizing NH2-MIL-101(Fe)@Copc (MOF@Copc). Specifically, NH2-MIL-101(Fe) functions as the TFSI- anion trap via the Lewis acid-base interactions and synergistic hydrogen bonding, thereby achieving primary optimization. Subsequently, the rich electronic structure of Copc facilitates charge delocalization and lowers the energy barrier for anion decomposition, allowing the C-F bonding to break more readily, thereby enabling further optimization. The π-π stacking interaction between the MOF and Copc facilitates the close association of adsorption and catalytic sites, allowing the continuous breakdown of the C- F series products in a chain reaction. The assembled LFP (19.26 mg cm⁻²) demonstrates a commercial-grade cathode area capacity, maintaining over 90% capacity retention across 350 cycles at 1 C, with a capacity decay rate of only 0.02% per cycle. More importantly, this strategy enables the industrial-scale production of Ah-class anode-free lithium-metal pouch batteries exceeding 300 Wh kg-1. Optimizing anion decomposition provides a novel perspective to advance the practical application of lithium-metal batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"63 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-04-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782888","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：