Jieun Kim, Injun Choi, Ju Seong Kim, Hyokkee Hwang, Byongyong Yu, Sang Cheol Nam, Inchul Park
{"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
{"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
{"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}
{"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}
{"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
{"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}
Mayank Kedia, Chittaranjan Das, Malgorzata Kot, Yenal Yalcinkaya, Weiwei Zuo, Kenedy Tabah Tanko, Peter Matvija, Mikel Ezquer, Iñaki Cornago, Wolfram Hempel, Florian Kauffmann, Paul Plate, Monica Lira-Cantu, Stefan A.L. Weber, Michael Saliba
{"title":"Mitigating the amorphization of perovskite solar cells by using atomic layer deposition alumina","authors":"Mayank Kedia, Chittaranjan Das, Malgorzata Kot, Yenal Yalcinkaya, Weiwei Zuo, Kenedy Tabah Tanko, Peter Matvija, Mikel Ezquer, Iñaki Cornago, Wolfram Hempel, Florian Kauffmann, Paul Plate, Monica Lira-Cantu, Stefan A.L. Weber, Michael Saliba","doi":"10.1039/d4ee05703a","DOIUrl":"https://doi.org/10.1039/d4ee05703a","url":null,"abstract":"Atomic layer deposition of aluminum oxide (ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small>) layers has been extensively studied for stabilizing perovskite solar cells (PSCs) against environmental stressors, such as humidity and oxygen. In addition, the ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> layer acts as a protective barrier, mitigating the pernicious halide ion migration from the perovskite toward the hole transport interface. However, its effectiveness in preventing the infiltration of ions and additives from the hole-transport layer into perovskites remains insufficiently understood. Herein, we demonstrate the deposition of a compact ultrathin (~0.75 nm) ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> layer that conformally follows the morphology of a triple-cation perovskite film over a large area. This promotes effective mechanical adhesion of the spiro-OMeTAD layer on top of the perovskite, thereby improving the charge carrier collection between these two layers. Upon systematically investigating the layer-by-layer structure of the PSC stack, we discovered that ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> also acts as a diffusion barrier for the degraded species from the adjacent transport layer into the perovskite. In addition to all protection capabilities, ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> impedes the transition of crystalline perovskites to an undesired amorphous phase instead of a yellow delta phase. Consequently, the dual functionality (i.e., enhanced mechanical adhesion and diffusion barrier) of the ALD-Al2O3 protection enhanced the device performance from 19.1% to 20.5%, retaining 98% of its initial power conversion efficiency compared to <10% for pristine devices after 1500 h of outdoor testing under ambient conditions. Finally, this study deepens our understanding of the mechanism of ALD-Al<small><sub>2</sub></small>O<small><sub>3</sub></small> as a two-way diffusion barrier, highlighting the multifaceted role of buffer layers in interfacial engineering for the long-term stability of PSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"19 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599074","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}
{"title":"Aramid dielectric co-polymer: from molecular engineering to roll-to-roll scalability for high-temperature capacitive energy storage","authors":"Rui Yang, Ding Ai, Sidi Fan, Wenqi Zhang, Xiao Yang, Fangcheng Lv, Yonghong Cheng, Xiang Yu","doi":"10.1039/d5ee00368g","DOIUrl":"https://doi.org/10.1039/d5ee00368g","url":null,"abstract":"Aromatic polymer films with high glass transition temperatures (Tg) exhibit superior thermal stability, making them ideal for high-temperature dielectric capacitors in advanced electrical and electronic systems. However, the leakage current can be intensified at high temperatures due to stronger π-electron delocalization, leading to energy loss and degrading capacitive performance. Here, we present a poly sulfonated aramid (PSA) derived from aramid by molecular engineering, with Tg > 300°C. Sulfone groups with a non-planar structure are introduced to break strong π-π conjugation and subsequently suppress intramolecular charge transfer. Moreover, their large dipole moments contribute to a high dielectric constant. To suppress intermolecular charge transfer, organic small molecules of triptycene (TE) are filled at an optimized content, breaking π-π stacking among PSA chains. The activation energy for trapped carriers is further increased, while the hopping distance is shortened. The PSA/TE all-organic film achieves an energy density (Ud) of 5.71 J·cm−3 at an efficiency exceeding 90% and a maximum Ud of 9.03 J·cm-3 at 150°C. Additionally, sulfone groups also aid self-healing by generating more gaseous products during pyrolysis. A roll-to-roll production line is established for continuously fabricating large-scale and high-quality PSA-based films, allowing for industrial potential for high-temperature capacitive energy storage.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599078","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}
Gaofeng Du, Shuhao Wang, Zhaoming Tong, Xinyu Ji, Xinqi Wei, Quanbin Zha, Tianyou Zhai, Huiqiao Li
{"title":"Dual thermal-stimulated self-adhesive mixed-phase interface to enable ultra-long cycle life of solid-state sodium metal batteries","authors":"Gaofeng Du, Shuhao Wang, Zhaoming Tong, Xinyu Ji, Xinqi Wei, Quanbin Zha, Tianyou Zhai, Huiqiao Li","doi":"10.1039/d4ee05140h","DOIUrl":"https://doi.org/10.1039/d4ee05140h","url":null,"abstract":"The pursuit of low-cost and intrinsically safe high-energy storage has significantly triggered the development of solid-state sodium–metal batteries. The solid–solid interface between the sodium anode and rigid electrolytes plays a critical role in the stable cycling of solid-state batteries. Undesirable interfacial contact during sodium deposition and stripping tends to induce the generation of voids and dendrites, leading to interface deterioration and cell failure. Herein, we constructed a self-adhesive and mixed-phase interface <em>via</em> a dual thermal stimulation strategy to enable an ultra-long cycling life of over 17 000 h (close to 2 years). A dense and robust SnF<small><sub>2</sub></small> interface layer was constructed on the surface of the solid electrolyte <em>via</em> a melting and self-adhesive effect induced by a physical thermal stimulation treatment. A secondary thermal activation was performed to trigger the <em>in situ</em> transformation of the interface layer into an ion/electron mixed ionic/electric conductor. Due to the robust contact and high conductivity of this self-adhesive mixed-phase interfacial layer, the cycling life of the sodium symmetric cell was dramatically increased from 50 h to 17 000 h with stable charging/discharging curves. Additionally, full cells coupled with the Na<small><sub>3</sub></small>V<small><sub>2</sub></small>(PO<small><sub>4</sub></small>)<small><sub>3</sub></small> cathode provided a capacity of 102.2 mA h g<small><sup>−1</sup></small> with a coulombic efficiency of 99.72% in the first cycle. The capacity maintained was 91.3 mA h g<small><sup>−1</sup></small> after 2000 cycles, with a capacity retention rate above 89.3%. This work provides a new strategy for constructing a robust and long-lasting stable interface in solid-state sodium–metal batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"54 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590016","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}