Jichao Zhai, Wang Zhao, Lei Wang, Jianbo Shuai, Ruwei Chen, Wenjiao Ge, Yu Zong, Guanjie He, Xiaohui Wang
The increasing demand for personalized health monitoring has driven the development of wearable electronics. Flexible zinc-ion batteries (FZIBs) are ideal power sources for wearable devices, but their low volumetric energy densities have been a limitation for practical application. We present an ultrathin cellulose-based electrolyte (DCG) with a gradient hydropenic interface designed for stable and high-energy FZIBs to address this. The gradient hydropenic interface composed of deep eutectic solvent (DES) residuals effectively mitigates moisture-induced side reactions and guides planar zinc deposition. The resulting zinc anode with the ultrathin DCG shows 99.9% coulombic efficiency (CE) and a cycle life exceeding 4000 hours in symmetrical configuration. Under stringent conditions, including a 66% depth of discharge (DOD) and reduced DCG thickness (10 μm), the flexible zinc battery demonstrates stable cycling with energy densities of 222 Wh kg⁻¹ and 214.3 Wh L⁻¹ and successfully applied in wearable watches, comparable to lithium-ion batteries and outperforming previously reported zinc batteries.
{"title":"Ultrathin cellulosic gel electrolyte with gradient hydropenic interface for stable, high-energy and flexible zinc batteries","authors":"Jichao Zhai, Wang Zhao, Lei Wang, Jianbo Shuai, Ruwei Chen, Wenjiao Ge, Yu Zong, Guanjie He, Xiaohui Wang","doi":"10.1039/d5ee00158g","DOIUrl":"https://doi.org/10.1039/d5ee00158g","url":null,"abstract":"The increasing demand for personalized health monitoring has driven the development of wearable electronics. Flexible zinc-ion batteries (FZIBs) are ideal power sources for wearable devices, but their low volumetric energy densities have been a limitation for practical application. We present an ultrathin cellulose-based electrolyte (DCG) with a gradient hydropenic interface designed for stable and high-energy FZIBs to address this. The gradient hydropenic interface composed of deep eutectic solvent (DES) residuals effectively mitigates moisture-induced side reactions and guides planar zinc deposition. The resulting zinc anode with the ultrathin DCG shows 99.9% coulombic efficiency (CE) and a cycle life exceeding 4000 hours in symmetrical configuration. Under stringent conditions, including a 66% depth of discharge (DOD) and reduced DCG thickness (10 μm), the flexible zinc battery demonstrates stable cycling with energy densities of 222 Wh kg⁻¹ and 214.3 Wh L⁻¹ and successfully applied in wearable watches, comparable to lithium-ion batteries and outperforming previously reported zinc batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"69 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618816","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 zinc-ion batteries (AZIBs) possess a tremendous prospect for large-scale energy storage. Nevertheless, the interfacial stability and cyclic reversibility for Zn anode are impeded by the unregulated growth of Zn dendrites and active H2O-induced side reactions. Here, an organic compound bis(2-hydroxyethyl) disulfide (BHED) is proposed as a multifunctional and efficient electrolyte additive, characterized by hydrophilic hydroxyl groups and dynamic sacrificial bonding disulfide bonds. It is discovered that BHED can optimize the Zn2+ solvation structure and construct a water-blocking barrier on the Zn anode surface. Besides, BHED undergoes reductive decomposition, promoting the in-situ formation of a self-assembled monolayer (SAM) with highly active zincophilic sites on the Zn anode surface. Notably, the unique SAM serves a dual function. It stabilizes the anode/electrolyte interface by trapping active H2O and guides Zn2+ to deposit uniformly and orderly onto the (002) crystal plane. As a result, the Zn||Zn symmetric cells containing BHED additive achieve Zn2+ uniform plating/stripping exceeding 6300 h at 0.5 mA cm-2 and 0.5 mAh cm-2. Furthermore, the Zn||NH4V4O10 full cells maintain a capacity retention rate of 73.9% following 3000 stabilized cycles at 5 A g-1. This work offers novel perspectives for the advancement of stable and long-lasting AZIBs.
{"title":"Multifunctional additive with dynamic sacrificial S-S bond for building self-assembled monolayers of Zn-ion battery with improved stability and longevity","authors":"Shuang Han, Haijun Niu, Wanan Cai, Minghai Li, Qiyu Fan, Zhuoyi Han, Xuewen Ming, Wen Wang","doi":"10.1039/d4ee05922k","DOIUrl":"https://doi.org/10.1039/d4ee05922k","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) possess a tremendous prospect for large-scale energy storage. Nevertheless, the interfacial stability and cyclic reversibility for Zn anode are impeded by the unregulated growth of Zn dendrites and active H<small><sub>2</sub></small>O-induced side reactions. Here, an organic compound bis(2-hydroxyethyl) disulfide (BHED) is proposed as a multifunctional and efficient electrolyte additive, characterized by hydrophilic hydroxyl groups and dynamic sacrificial bonding disulfide bonds. It is discovered that BHED can optimize the Zn<small><sup>2+</sup></small> solvation structure and construct a water-blocking barrier on the Zn anode surface. Besides, BHED undergoes reductive decomposition, promoting the in-situ formation of a self-assembled monolayer (SAM) with highly active zincophilic sites on the Zn anode surface. Notably, the unique SAM serves a dual function. It stabilizes the anode/electrolyte interface by trapping active H<small><sub>2</sub></small>O and guides Zn<small><sup>2+</sup></small> to deposit uniformly and orderly onto the (002) crystal plane. As a result, the Zn||Zn symmetric cells containing BHED additive achieve Zn<small><sup>2+</sup></small> uniform plating/stripping exceeding 6300 h at 0.5 mA cm<small><sup>-2</sup></small> and 0.5 mAh cm<small><sup>-2</sup></small>. Furthermore, the Zn||NH<small><sub>4</sub></small>V<small><sub>4</sub></small>O<small><sub>10</sub></small> full cells maintain a capacity retention rate of 73.9% following 3000 stabilized cycles at 5 A g<small><sup>-1</sup></small>. This work offers novel perspectives for the advancement of stable and long-lasting AZIBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618820","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 failure of zinc metal batteries usually involves the instability of the protection layer of zinc metal anode due to the water penetrating and dissolution during long-term operation, leading to the uncontrollably erratic electrode/electrolyte interface and hydrogen evolution reaction. Here, we propose an ultrathin, water-repellent, Zn2+-selective layer to prevent the undesirable water layer and avoid the water penetrating and dissolution. This interface, with an ultrathin thickness of 16.9 nm, is composed of a water repellent didodecyldimethylammonium organic top layer and an open three-dimensional framework structure of inorganic layer with subnanometer pores and redox-active Fe centers that function as faradaic ion pumps, facilitating rapid Zn2+ transport. This ultrathin solid contact layer acts as semi-permeable membrane with low water permeance of 0.000028 mol m-2 h-1 Pa-1, while facilitating fast Zn2+ transport, thus suppressing hydrogen evolution. As a result, this layer enables over 10,000 stable plating/stripping cycles at 5 mA cm-2 with an average Coulombic efficiency of 99.91%. At a high rate of 150 C, the Zn-I2 cell operates for an unprecedented 65,000 cycles. Moreover, Ah-level Zn-I2 pouch cells were verified, demonstrating scalable applicability towards grid-scale energy storage device. Our work demonstrates the importance of designing stable and functional interface layer for metal anode towards high-energy metal battery.
{"title":"Suppression of Interfacial Water Layer with Solid Contact by an Ultrathin Water Repellent and Zn2+ Selective Layer for Ah-Level Zinc Metal Battery","authors":"Ziwei Xu, Junpeng Li, Yifan Fu, Junjie Ba, Fengxue Duan, Yingjin Wei, Chunzhong Wang, Kangning Zhao, Yizhan Wang","doi":"10.1039/d4ee05905k","DOIUrl":"https://doi.org/10.1039/d4ee05905k","url":null,"abstract":"The failure of zinc metal batteries usually involves the instability of the protection layer of zinc metal anode due to the water penetrating and dissolution during long-term operation, leading to the uncontrollably erratic electrode/electrolyte interface and hydrogen evolution reaction. Here, we propose an ultrathin, water-repellent, Zn2+-selective layer to prevent the undesirable water layer and avoid the water penetrating and dissolution. This interface, with an ultrathin thickness of 16.9 nm, is composed of a water repellent didodecyldimethylammonium organic top layer and an open three-dimensional framework structure of inorganic layer with subnanometer pores and redox-active Fe centers that function as faradaic ion pumps, facilitating rapid Zn2+ transport. This ultrathin solid contact layer acts as semi-permeable membrane with low water permeance of 0.000028 mol m-2 h-1 Pa-1, while facilitating fast Zn2+ transport, thus suppressing hydrogen evolution. As a result, this layer enables over 10,000 stable plating/stripping cycles at 5 mA cm-2 with an average Coulombic efficiency of 99.91%. At a high rate of 150 C, the Zn-I2 cell operates for an unprecedented 65,000 cycles. Moreover, Ah-level Zn-I2 pouch cells were verified, demonstrating scalable applicability towards grid-scale energy storage device. Our work demonstrates the importance of designing stable and functional interface layer for metal anode towards high-energy metal battery.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"89 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618907","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}
Hao Xu, Jinshuo Mi, Jiabin Ma, Zhuo Han, Shun Lv, Likun Chen, Jiameng Zhang, Ke Yang, Boyu Li, Yuhang Li, Xufei An, Yuetao Ma, Shaoke Guo, Hai Su, Peiran Shi, Ming Liu, Feiyu Kang, Yanbing He
In situ polymerized solid-state polymer electrolytes (SPEs) have attracted much attention due to their good machinability and excellent interface contact with electrodes. However, the undesirable stability to lithium metal and high-voltage electrodes hinders their application in high energy density solid-state lithium batteries. Herein, a poly(1,3-dioxolane) composite SPE possessing high interfacial stability with both lithium metal anode and high voltage cathode was fabricated via in-situ polymerization initiated by a Mg2+-containing montmorillonite filler. The strong coordination between Mg2+ and anions of lithium salts not only improves the antioxidant stability of the polymer chains, but also optimizes the lithium ion coordination structure and constructs robust MgF2-containing interphases on both anode and cathode. As a result, the composite SPE exhibits an improved homogeneous polymer chain distribution, a high lithium-ion transference number of 0.60 and an extended electrochemical window of 5.3 V. The Li/Li symmetric cells exhibit outstanding cycling stability for 6000 hours and the Li/LiNi0.8Co0.1Mn0.1O2 cells demonstrate excellent rate capability and cycle stability over 500 cycles. This work provides a promising pathway for the SPEs toward practical high energy density solid-state batteries.
{"title":"Mg2+ Initiated in-situ Polymerization of Dioxolane Enabling Stable Interfaces in Solid-State Lithium Metal Batteries","authors":"Hao Xu, Jinshuo Mi, Jiabin Ma, Zhuo Han, Shun Lv, Likun Chen, Jiameng Zhang, Ke Yang, Boyu Li, Yuhang Li, Xufei An, Yuetao Ma, Shaoke Guo, Hai Su, Peiran Shi, Ming Liu, Feiyu Kang, Yanbing He","doi":"10.1039/d4ee05606j","DOIUrl":"https://doi.org/10.1039/d4ee05606j","url":null,"abstract":"In situ polymerized solid-state polymer electrolytes (SPEs) have attracted much attention due to their good machinability and excellent interface contact with electrodes. However, the undesirable stability to lithium metal and high-voltage electrodes hinders their application in high energy density solid-state lithium batteries. Herein, a poly(1,3-dioxolane) composite SPE possessing high interfacial stability with both lithium metal anode and high voltage cathode was fabricated via in-situ polymerization initiated by a Mg2+-containing montmorillonite filler. The strong coordination between Mg2+ and anions of lithium salts not only improves the antioxidant stability of the polymer chains, but also optimizes the lithium ion coordination structure and constructs robust MgF2-containing interphases on both anode and cathode. As a result, the composite SPE exhibits an improved homogeneous polymer chain distribution, a high lithium-ion transference number of 0.60 and an extended electrochemical window of 5.3 V. The Li/Li symmetric cells exhibit outstanding cycling stability for 6000 hours and the Li/LiNi0.8Co0.1Mn0.1O2 cells demonstrate excellent rate capability and cycle stability over 500 cycles. This work provides a promising pathway for the SPEs toward practical high energy density solid-state batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"54 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618817","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}
Jieun Kim, Injun Choi, Ju Seong Kim, Hyokkee Hwang, Byongyong Yu, Sang Cheol Nam, Inchul Park
Lithium-rich layered oxides (LRLOs) hold great promise as cathode materials for lithium-ion batteries, but they face challenges due to their complex electrochemical behavior and structural instability. Here, we propose an unsupervised analysis framework that applies Principal Component Analysis (PCA) to a large dataset of over 30,000 LRLO charge curves to identify fundamental degradation factors and enhance predictability. By incorporating ex situ Mn L-edge and O K-edge soft X-ray absorption spectroscopy (sXAS), along with electrochemical impedance spectroscopy (EIS), we connect each principal component to physical phenomena such as Mn reduction and rising charge transfer resistance. Leveraging these insights, we demonstrate robust predictive models that can accurately reconstruct full charge curves and reliably detect outliers or abnormal cycling patterns. By bridging mechanistic domain knowledge with unsupervised learning, this framework underscores the value of combining data-driven methodologies with mechanistic insights, paving the way for more reliable and high-performance materials in next-generation battery systems.
{"title":"Data-driven insights into reaction mechanism of Li-rich cathodes","authors":"Jieun Kim, Injun Choi, Ju Seong Kim, Hyokkee Hwang, Byongyong Yu, Sang Cheol Nam, Inchul Park","doi":"10.1039/d4ee05222f","DOIUrl":"https://doi.org/10.1039/d4ee05222f","url":null,"abstract":"Lithium-rich layered oxides (LRLOs) hold great promise as cathode materials for lithium-ion batteries, but they face challenges due to their complex electrochemical behavior and structural instability. Here, we propose an unsupervised analysis framework that applies Principal Component Analysis (PCA) to a large dataset of over 30,000 LRLO charge curves to identify fundamental degradation factors and enhance predictability. By incorporating ex situ Mn L-edge and O K-edge soft X-ray absorption spectroscopy (sXAS), along with electrochemical impedance spectroscopy (EIS), we connect each principal component to physical phenomena such as Mn reduction and rising charge transfer resistance. Leveraging these insights, we demonstrate robust predictive models that can accurately reconstruct full charge curves and reliably detect outliers or abnormal cycling patterns. By bridging mechanistic domain knowledge with unsupervised learning, this framework underscores the value of combining data-driven methodologies with mechanistic insights, paving the way for more reliable and high-performance materials in next-generation battery systems.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"22 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618908","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}
Jemin Lee, Wonwoo Choi, Eunbin Jang, Hyunjin Kim, Jeeyoung Yoo
Ionic liquid electrolytes (ILEs) provide promising thermal and electrochemical stability characteristics for safer lithium metal batteries (LMBs). However, their development faces challenges due to their low ionic conductivity and poor wettability on separators. In this study, we introduce a dual-anion locally concentrated ionic-liquid electrolyte (D-LCILE), designed with a diluent and two distinct anions to significantly improve the ionic conductivity and wettability. These improvements were confirmed through electrochemical impedance spectroscopy (EIS) measurements on stainless steel symmetric cells, contact angle tests, and rate capability assessments on a 300 µm thick lithium metal half-cell. Notably, the dual-anion design enhances the interfacial stability, as density functional theory (DFT) calculations revealed a more stable solvation shell structure, further supported by molecular dynamics (MD) simulations. Additionally, scanning electron microscopy (SEM) experiments confirmed the deposition of a thin and, dense lithium layer, while X-ray photoelectron spectroscopy (XPS) depth profile analysis showed a stable solid electrolyte interphase (SEI) with increased LiF content. Performance tests on a 20 µm-thick Li||LiFePO4 full cell revealed an average Coulombic efficiency exceeding 99.90% and capacity retention >99.93% after 200 cycles at 1C, making D-LCILE a highly promising candidate for next-generation, high-performance LMBs.
{"title":"Dual-Anion Ionic Liquid Electrolytes: A Strategy for Achieving High Stability and Conductivity in Lithium Metal Battery","authors":"Jemin Lee, Wonwoo Choi, Eunbin Jang, Hyunjin Kim, Jeeyoung Yoo","doi":"10.1039/d5ee00119f","DOIUrl":"https://doi.org/10.1039/d5ee00119f","url":null,"abstract":"Ionic liquid electrolytes (ILEs) provide promising thermal and electrochemical stability characteristics for safer lithium metal batteries (LMBs). However, their development faces challenges due to their low ionic conductivity and poor wettability on separators. In this study, we introduce a dual-anion locally concentrated ionic-liquid electrolyte (D-LCILE), designed with a diluent and two distinct anions to significantly improve the ionic conductivity and wettability. These improvements were confirmed through electrochemical impedance spectroscopy (EIS) measurements on stainless steel symmetric cells, contact angle tests, and rate capability assessments on a 300 µm thick lithium metal half-cell. Notably, the dual-anion design enhances the interfacial stability, as density functional theory (DFT) calculations revealed a more stable solvation shell structure, further supported by molecular dynamics (MD) simulations. Additionally, scanning electron microscopy (SEM) experiments confirmed the deposition of a thin and, dense lithium layer, while X-ray photoelectron spectroscopy (XPS) depth profile analysis showed a stable solid electrolyte interphase (SEI) with increased LiF content. Performance tests on a 20 µm-thick Li||LiFePO4 full cell revealed an average Coulombic efficiency exceeding 99.90% and capacity retention >99.93% after 200 cycles at 1C, making D-LCILE a highly promising candidate for next-generation, high-performance LMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"15 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608365","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}
Xintong Li, guanzhen chen, Yan Liu, Ruihu Lu, Chao Ma, Ziyun Wang, Yunhu Han, Dingsheng Wang
Precisely regulating the electron transfer capacity and Ru-O covalency of RuO2-based catalysts is crucial and challenging for resolving the inadequate performance of RuO2-based acidic oxygen evolution reaction (OER) catalysts in proton exchange membrane water electrolyzers (PEMWEs). Here, we propose to select Cr, an element with an atomic radius similar to that of Ru, for continuous doping of RuO2, and to achieve continuous regulation of the electron transfer capacity and Ru-O covalency of RuO2-based catalysts via adjusting the Cr content, thus optimizing the activity and stability of RuO2-based catalysts. According to the experimental results, it was found that the acidic OER stability of the Cr-doped RuO2 catalysts (CrxRu1-xO2) tended to increase and then decrease with the gradual increase of the Cr doping level, and the tendency was almost consistent with the variation of the Ru-O covalency predicted by theoretical calculations. The RuO2-based catalyst (Cr0.31Ru0.69O2) showed optimal stability at a Cr/Ru ratio of 0.31/0.69 (Cr content similar to theoretical prediction), and was operated stably for over 1400 hours at a 10 mA cm-2 current density with almost no degradation. Moreover, as the catalyst also has the best electron transfer ability, its activity is also the highest, requiring an overpotential of only 176 mV to deliver a 10 mA cm-2 current density. Most importantly, the catalyst can be operated for at least 2300 hours at a 300 mA cm-2 current density when applied to a PEMWE’s anode, which strongly demonstrates its great potential for practical applications.
{"title":"Optimal selection of RuO2 for durable oxygen evolution reactions in acid by continuous regulating of Ru-O covalency","authors":"Xintong Li, guanzhen chen, Yan Liu, Ruihu Lu, Chao Ma, Ziyun Wang, Yunhu Han, Dingsheng Wang","doi":"10.1039/d4ee04861j","DOIUrl":"https://doi.org/10.1039/d4ee04861j","url":null,"abstract":"Precisely regulating the electron transfer capacity and Ru-O covalency of RuO2-based catalysts is crucial and challenging for resolving the inadequate performance of RuO2-based acidic oxygen evolution reaction (OER) catalysts in proton exchange membrane water electrolyzers (PEMWEs). Here, we propose to select Cr, an element with an atomic radius similar to that of Ru, for continuous doping of RuO2, and to achieve continuous regulation of the electron transfer capacity and Ru-O covalency of RuO2-based catalysts via adjusting the Cr content, thus optimizing the activity and stability of RuO2-based catalysts. According to the experimental results, it was found that the acidic OER stability of the Cr-doped RuO2 catalysts (CrxRu1-xO2) tended to increase and then decrease with the gradual increase of the Cr doping level, and the tendency was almost consistent with the variation of the Ru-O covalency predicted by theoretical calculations. The RuO2-based catalyst (Cr0.31Ru0.69O2) showed optimal stability at a Cr/Ru ratio of 0.31/0.69 (Cr content similar to theoretical prediction), and was operated stably for over 1400 hours at a 10 mA cm-2 current density with almost no degradation. Moreover, as the catalyst also has the best electron transfer ability, its activity is also the highest, requiring an overpotential of only 176 mV to deliver a 10 mA cm-2 current density. Most importantly, the catalyst can be operated for at least 2300 hours at a 300 mA cm-2 current density when applied to a PEMWE’s anode, which strongly demonstrates its great potential for practical applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608366","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}
Developing efficient catalysts is essential for mitigating the shuttle effect and accelerating the conversion kinetics of polysulfides in lithium-sulfur (Li-S) batteries. To date, numerous strategies have been employed to optimize the performance of catalysts. Among these strategies, regulating the spin state of metal sites can modulate the d orbital occupancy and enable precise control over catalyst-polysulfide interactions, which provides an effective approach for the catalysts to optimize the balance between adsorption and catalysis toward polysulfide conversion. This review offers a comprehensive overview of spin-state engineering of the catalysts for Li-S batteries for the first time, detailing the strategies for spin-state modulation and the relevant characterization techniques for monitoring these changes. Finally, we underscore the critical role of spin-state tuning in optimizing catalytic active centers and propose future research directions in this emerging field.
{"title":"Engineering Spin State of Metal Sites toward Advanced Lithium-Sulfur Batteries","authors":"Xiaomin Zhang, Xiaoyu Zhang, Xingbo Wang, Guoliang Cui, Hongge Pan, Wenping Sun","doi":"10.1039/d4ee05582a","DOIUrl":"https://doi.org/10.1039/d4ee05582a","url":null,"abstract":"Developing efficient catalysts is essential for mitigating the shuttle effect and accelerating the conversion kinetics of polysulfides in lithium-sulfur (Li-S) batteries. To date, numerous strategies have been employed to optimize the performance of catalysts. Among these strategies, regulating the spin state of metal sites can modulate the d orbital occupancy and enable precise control over catalyst-polysulfide interactions, which provides an effective approach for the catalysts to optimize the balance between adsorption and catalysis toward polysulfide conversion. This review offers a comprehensive overview of spin-state engineering of the catalysts for Li-S batteries for the first time, detailing the strategies for spin-state modulation and the relevant characterization techniques for monitoring these changes. Finally, we underscore the critical role of spin-state tuning in optimizing catalytic active centers and propose future research directions in this emerging field.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"30 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599075","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}
Printing of electrodes to replace thermal evaporation of metals for back contacts in perovskite solar cells (PSCs) is essential for scalable manufacturing. However, PSCs incorporating printed electrodes typically exhibit lower power conversion efficiencies (PCE) than those with evaporated metals. Low-melting-point alloys (LMPAs) are promising candidates for PSC electrodes due to their matched work functions, high electrical conductivities, and chemical stability. This study proposes a convenient strategy of blade printing to pattern In-Sn-Bi LMPAs as back electrodes in inverted PSCs. These LMPAs, with moderate melting points (62°C, 80°C, and 120°C), are printed above their melting points and solidify at room temperature without additional post-treatment. PSCs with LMPA electrodes show high built-in potential and fast charge extraction, achieving PCEs of 22.48%, comparable to evaporated-metal counterparts. Charge transport and recombination dynamics reveal that PSCs with LMPA electrodes are more stable than those with evaporated copper electrodes after aging in air without encapsulation. Morphological analysis of LMPA and perovskite layers after aging shows no noticeable corrosion. PSCs with blade-printed LMPA electrodes retain ~80% of their peak PCE after 1,500 hours of aging, demonstrating significantly higher stability than PSCs with evaporated copper or silver electrodes.
{"title":"Blade Printing of Low-Melting-Point-Alloys as Back Electrodes for High-Efficiency and Stable Inverted Perovskite Solar Cells","authors":"Bo Jiang, Boyang Yu, Yong Zhang, Weiwei Deng, Baomin Xu, Xinyan Zhao","doi":"10.1039/d5ee00269a","DOIUrl":"https://doi.org/10.1039/d5ee00269a","url":null,"abstract":"Printing of electrodes to replace thermal evaporation of metals for back contacts in perovskite solar cells (PSCs) is essential for scalable manufacturing. However, PSCs incorporating printed electrodes typically exhibit lower power conversion efficiencies (PCE) than those with evaporated metals. Low-melting-point alloys (LMPAs) are promising candidates for PSC electrodes due to their matched work functions, high electrical conductivities, and chemical stability. This study proposes a convenient strategy of blade printing to pattern In-Sn-Bi LMPAs as back electrodes in inverted PSCs. These LMPAs, with moderate melting points (62°C, 80°C, and 120°C), are printed above their melting points and solidify at room temperature without additional post-treatment. PSCs with LMPA electrodes show high built-in potential and fast charge extraction, achieving PCEs of 22.48%, comparable to evaporated-metal counterparts. Charge transport and recombination dynamics reveal that PSCs with LMPA electrodes are more stable than those with evaporated copper electrodes after aging in air without encapsulation. Morphological analysis of LMPA and perovskite layers after aging shows no noticeable corrosion. PSCs with blade-printed LMPA electrodes retain ~80% of their peak PCE after 1,500 hours of aging, demonstrating significantly higher stability than PSCs with evaporated copper or silver electrodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"4 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599073","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}
Pengcheng Du, Tianhao Liu, Tuoyu Chen, Meihui Jiang, Hongyu Zhu, Yitong Shang, Hui Hwang Goh, Zhao HaiSen Zhao HaiSen, Chao Huang, Fannie Kong, Tonni Agustiono Kurniawan, Kai Chen Goh, Yu Du, Dongdong Zhang
Vehicle-to-Grid accelerates the transition to renewable, low-carbon power systems by integrating electric vehicles. This study analyzes the 2023 U.S. electric vehicle charging demand, variable renewable energy capacities, and charging infrastructure numbers in China, the U.S., and the EU. Moreover, an assessment of electric vehicle lifecycle carbon emissions using IEA data are conducted. Results indicate that V2G offers significant economic feasibility and environmental benefits by balancing grid supply and demand, absorbing renewable energy, conserving electricity, reducing CO₂ emissions, and supporting Sustainable Development Goals. Key underlying technologies are investigated to guide future V2G advancements. An orderly regulation framework for the EV-Grid-Aggregator system is provided, specifying market incentives and charging management measures to promote EV participation in V2G. Additionally, charging infrastructure planning strategies that integrate power and transportation networks are developed to facilitate decarbonization. By analyzing global policy contexts and market incentives, effective policies for advancing V2G implementation are emphasized. Finally, future development directions are proposed based on existing research, offering a roadmap for sustainable V2G development.
{"title":"Enhancing Green Mobility through Vehicle-to-Grid: Potential, Technological Barriers, and Policy Implications","authors":"Pengcheng Du, Tianhao Liu, Tuoyu Chen, Meihui Jiang, Hongyu Zhu, Yitong Shang, Hui Hwang Goh, Zhao HaiSen Zhao HaiSen, Chao Huang, Fannie Kong, Tonni Agustiono Kurniawan, Kai Chen Goh, Yu Du, Dongdong Zhang","doi":"10.1039/d5ee00116a","DOIUrl":"https://doi.org/10.1039/d5ee00116a","url":null,"abstract":"Vehicle-to-Grid accelerates the transition to renewable, low-carbon power systems by integrating electric vehicles. This study analyzes the 2023 U.S. electric vehicle charging demand, variable renewable energy capacities, and charging infrastructure numbers in China, the U.S., and the EU. Moreover, an assessment of electric vehicle lifecycle carbon emissions using IEA data are conducted. Results indicate that V2G offers significant economic feasibility and environmental benefits by balancing grid supply and demand, absorbing renewable energy, conserving electricity, reducing CO₂ emissions, and supporting Sustainable Development Goals. Key underlying technologies are investigated to guide future V2G advancements. An orderly regulation framework for the EV-Grid-Aggregator system is provided, specifying market incentives and charging management measures to promote EV participation in V2G. Additionally, charging infrastructure planning strategies that integrate power and transportation networks are developed to facilitate decarbonization. By analyzing global policy contexts and market incentives, effective policies for advancing V2G implementation are emphasized. Finally, future development directions are proposed based on existing research, offering a roadmap for sustainable V2G development.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"38 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599077","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}
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