Lukas Ihlbrock, Anne Sehnal, Moritz Gutsch and Simon Lux
{"title":"Future energy demand for automotive and stationary lithium- and sodium-ion battery production towards a European circular economy","authors":"Lukas Ihlbrock, Anne Sehnal, Moritz Gutsch and Simon Lux","doi":"10.1039/D5EE02287H","DOIUrl":"10.1039/D5EE02287H","url":null,"abstract":"<p >Europe is currently heavily dependent on imports for the critical raw materials needed for lithium-ion battery (LIB) production, as most of these resources are distributed outside the region. Despite this dependency, Europe accounts for around 25% of global electric vehicle (EV) sales. This creates an indirect form of energy dependency, as much of the energy used in battery cell production is embedded in imported materials and cells. Persistent supply chain bottlenecks have made battery access a strategic priority for automakers, prompting efforts to build more resilient domestic supply chains. However, this shift also means that a significant amount of energy will need to be sourced within Europe itself, raising concerns about energy consumption amid surging European battery capacity demand – an important factor that will shape strategic decisions in both industry and policy. This work addresses the future energy demand of LIBs and their potential near-term competitors, sodium-ion batteries, by quantifiying the cradle-to-gate and cradle-to-cradle cumulative energy demand for large-format prismatic cells, using primary machinery data on gigafactory scale. The European energy demand forecast until 2070 is conducted using a novel circular economy simulation model, considering recycling, second use and the use phase of EVs and stationary energy storage (SES) applications. We show that the local European energy demand to establish a domestic battery cell production and to be self-sufficient by 2050 will rise to 250 TWh annually. Including the use phase of EVs and SES, a total of 450–500 TWh will be needed within Europe starting in 2040, offset by savings of approx. 90 TWh from reduced fossil fuel upstream energy. The comprehensive analysis provides a quantitative framework for understanding the energy flows associated with large-scale battery cell production in Europe. We highlight processes with significant reduction potential, while also identifying factors that could increase energy demand in the future.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 19","pages":" 8724-8743"},"PeriodicalIF":30.8,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ee/d5ee02287h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987617","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dahu Ren, Liping Yang, Xuemei Zhang, Qianying Li, Xiaochuan Li, Qianxi Yang, Haiyang Feng, Zheng Peng, Yi Xi, Huake Yang and Changsheng Wu
{"title":"Comprehensive output performance optimization of ternary constant DC triboelectric nanogenerators via dual-phase symmetric step-down conversion","authors":"Dahu Ren, Liping Yang, Xuemei Zhang, Qianying Li, Xiaochuan Li, Qianxi Yang, Haiyang Feng, Zheng Peng, Yi Xi, Huake Yang and Changsheng Wu","doi":"10.1039/D5EE02837J","DOIUrl":"10.1039/D5EE02837J","url":null,"abstract":"<p >Achieving high and stable output performance remains a critical challenge for the practical application of constant direct current triboelectric nanogenerators (C-DC-TENGs). While ternary DC-TENGs (T-DC-TENGs) outperform other C-DC-TENGs, they face significant limitations including output charge thresholds, high internal impedance, and uncontrollable high voltages. To address these, we present a novel power management circuit (PMC) based on a dual-phase symmetric step-down converter (DSSC) with collaborative switches, termed a DSSC-TENG. For rotating T-DC-TENGs at 120 rpm, this approach yields remarkable improvements: a 6.6-fold increase in output charge density (4.8 mC m<small><sup>−2</sup></small> per cycle), a 1.7-fold enhancement in average power density (4.94 W m<small><sup>−2</sup></small> Hz<small><sup>−1</sup></small>), and a reduction in output impedance to 10 MΩ, setting a benchmark among ternary-structure-based TENGs. The PMC reduces output voltage by 54.7% while improving output stability, as confirmed by Fourier analysis showing that the AC/DC component ratio decreased from 0.6% to 0.05%. The demonstrated DSSC-TENG directly powers electronic devices including a calculator, a watch, 2400 LEDs, and parallel 10 W lamps without pre-charging capacitors, and achieves a 67.2% increase in a methyl orange degradation rate compared to the case without a DSSC. This work introduces the first PMC specifically designed for C-DC-TENGs, substantially advancing their potential for real-world implementation in self-powered systems.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9205-9216"},"PeriodicalIF":30.8,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987799","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}
Haotian Zhu, Haikuo Zhang, Shuoqing Zhang, Ruhong Li, Ruixin Zhang, Shouhong Ding, Liuhui Zhu, Baochen Ma, Long Chen, Tao Zhou, Jinze Wang, Long Li, Yuntong Ma, Shihao Duan, Menglu Li, Junyi Hua, Wei Liu, Lixin Chen, Tao Deng and Xiulin Fan
{"title":"Energy-landscape-tailored solvation switching dynamics enable stable lithium batteries","authors":"Haotian Zhu, Haikuo Zhang, Shuoqing Zhang, Ruhong Li, Ruixin Zhang, Shouhong Ding, Liuhui Zhu, Baochen Ma, Long Chen, Tao Zhou, Jinze Wang, Long Li, Yuntong Ma, Shihao Duan, Menglu Li, Junyi Hua, Wei Liu, Lixin Chen, Tao Deng and Xiulin Fan","doi":"10.1039/D5EE03077C","DOIUrl":"10.1039/D5EE03077C","url":null,"abstract":"<p >Solvation structures play a crucial role in electrolyte design, yet traditional strategies have primarily emphasized static solvation configurations, overlooking the inherently dynamic nature of solvation processes at the electrode interface. This oversight critically limits electrolyte performance, particularly where dynamic interfacial solvation layers govern ion-flux uniformity and the stability of interphase formation. Here, we propose a dynamic design framework based on an energy-landscape-tailored solvation switching mechanism that prioritizes dynamic adaptability over static equilibrium, thereby addressing the longstanding challenge of optimizing solvation dynamics at the interface. To quantitatively assess these dynamics, we developed a solvation switching energy index (SSEI), which exhibits a strong correlation with interfacial electrochemical behavior. Combining machine-learning molecular dynamics (MLMD) simulations with femtosecond transient absorption spectroscopy (fs-TAS), we directly probe and elucidate real-time solvation switching phenomena. Energetically, we uncover a constitutive control mechanism that enhances solvation diversity in traditional strategies, and further propose a contextual control strategy that is distinct from conventional lithium-salt-concentration and molecular-polarity regulation for minimizing the energy barrier for solvation transitions. This contextual control fundamentally transforms intrinsically diluted electrolytes, enabling exceptional interfacial performance, including a Coulombic efficiency (CE) of 99.8% for lithium metal plating/stripping and the effective suppression of solvent co-intercalation in graphite electrodes. This work redefines solvation dynamics as a central pillar in electrolyte engineering, bridging dynamics insights and high-performance energy storage systems.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9263-9273"},"PeriodicalIF":30.8,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987673","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}
Yangdong Zhou, Weijia Guo, Lixin Xing, Jiayang Li, Ning Wang, Ling Meng, Siyu Ye, Xiaohua Yang, Hao Chen and Lei Du
{"title":"Stability/durability challenges of cathode catalysts for PEM fuel cells: experiments, mechanisms, and perspectives beyond three-electrode systems","authors":"Yangdong Zhou, Weijia Guo, Lixin Xing, Jiayang Li, Ning Wang, Ling Meng, Siyu Ye, Xiaohua Yang, Hao Chen and Lei Du","doi":"10.1039/D5EE03461B","DOIUrl":"10.1039/D5EE03461B","url":null,"abstract":"<p >The sluggish oxygen reduction reaction (ORR) determines the performance and lifetime of proton exchange membrane (PEM) fuel cells. Commercialized cathodic ORR catalysts are synthesized using platinum-group-metal (PGM)-based chemicals, which suffer from low geological reserves; hence, PGM-free catalysts are emerging as alternatives. However, PGM and PGM-free catalysts suffer from insufficient stability/durability. The stability/durability test protocols for ORR catalysts, especially for PGM-free catalysts, have not been well agreed—different groups use different stability/durability test protocols in their experiments, particularly in membrane electrode assembly (MEA) tests; some false comparison may be overlooked by researchers. However, a deep understanding of degradation mechanisms and the development of efficient strategies to improve stability/durability have become the research frontier in this field. In this regard, we herein discuss the key experimental factors influencing the accuracy of stability/durability tests in three-electrode systems and MEAs and discuss critical degradation mechanisms and material-based solutions to improve catalyst stability/durability. We hope this discussion will highlight the importance of stability/durability studies and promote PEM fuel cell development.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9054-9092"},"PeriodicalIF":30.8,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144930926","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":"Asymmetric Functional Gel Polymer Electrolyte Enables Superior Interfacial Compatibility for Wide Temperature Lithium Metal Batteries","authors":"Haixia Yang, Jiaxin Yan, Shuyang Gao, Xin Chen, Yuanheng Wang, Hua Huo, Chuankai Fu, Chunyu Du, Pengjian Zuo","doi":"10.1039/d5ee03838c","DOIUrl":"https://doi.org/10.1039/d5ee03838c","url":null,"abstract":"Lithium metal batteries (LMBs) represent a promising candidate for next-generation energy storage systems, yet their practical application is constrained by limited cycle life owing to slow interface Li+ ion transport and severe interfacial side reactions, particularly in extreme temperature conditions. Herein, a novel asymmetric gel polymer electrolyte (GPE) is constructed through sequential electrospinning and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) filler integration to achieve high compatibility with Li anode and high-voltage cathode over wide temperature range. The polyethylene oxide (PEO)/poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix adjacent to the Li anode homogenizes Li⁺ ion flux and facilitates the formation of stable solid electrolyte interphase (SEI) through dynamic interfacial remodeling. At the cathode side, the polyacrylonitrile (PAN)/PVDF-HFP matrix exhibits outstanding high-voltage tolerance, effectively suppressing transition metal dissolution and electrolyte decomposition. The incorporated LLZTO enhances LiPF6 dissociation via selective adsorption. The highly porous asymmetric polymer framework architecture facilitates the elimination of macroscopic interfaces among dissimilar materials, achieving fast Li⁺ ion transport. Consequently, the Li||Ni0.8Co0.1Mn0.1O2 cells exhibit outstanding wide temperature cycling of -30 to 70 °C. This asymmetric structure design of GPE offers valuable insights into interfacial engineering exploration for all-climate LMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"2 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144919045","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}
Miao Yu Lin, Wen Jing Li, Hao Yang Lin, Sheng Dai, Zhen Xin Lou, Jia Chen Wu, Huai Qin Fu, Song Ru Fang, Hao Fan, Xiao Xiao Mao, Xue Qing Chen, Hai Yang Yuan, Peng Fei Liu, Hua Gui Yang and Yu Hou
{"title":"A self-healing non-precious metal oxide anode in proton exchange membrane electrolysis beyond 1000 h stability at 2 A cm−2","authors":"Miao Yu Lin, Wen Jing Li, Hao Yang Lin, Sheng Dai, Zhen Xin Lou, Jia Chen Wu, Huai Qin Fu, Song Ru Fang, Hao Fan, Xiao Xiao Mao, Xue Qing Chen, Hai Yang Yuan, Peng Fei Liu, Hua Gui Yang and Yu Hou","doi":"10.1039/D5EE02703A","DOIUrl":"10.1039/D5EE02703A","url":null,"abstract":"<p >The development of non-precious metal-based anode electrocatalysts is a crucial step towards the large-scale deployment of proton exchange membrane water electrolysis (PEMWE). However, the significant dissolution of non-precious metal materials poses a substantial challenge to their application in PEMWE. In this study, we introduce a dynamically stable anode material consisting of lanthanum-doped cobalt manganese oxide that operates under ampere-level current densities. This anode material exhibits bulk structural stability and maintains a dynamic equilibrium of active sites on its surface. The anode demonstrates sustained performance for over 200 hours at 5 amperes per square centimeter and 1200 hours at 2 amperes per square centimeter in PEMWE. Experimental and computational analyses confirm that the re-deposition of active species at the working potential is responsible for achieving dynamic stability at ampere-level current densities. This innovative concept of a dynamically stable electrocatalyst expands the potential of non-precious metal oxide anodes in PEMWE, reducing reliance on the limited supply of iridium without compromising hydrogen production rates.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9183-9193"},"PeriodicalIF":30.8,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144916229","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}
Zhongwei Jiang, Junyang Liu, Ke Yue, Man Pang, Yixuan Peng, Chongyang Luo, Ziqing Yao, Tao Pan, Yuanyuan Wang, Yujie Li, Qingpeng Guo, Chunman Zheng, Weiwei Sun, Xinyong Tao and Shuangke Liu
{"title":"Achieving a stable 518 Wh kg−1 Li metal pouch cell via SEI reconstruction engineering for high Li+ conductive hetero-grain boundaries","authors":"Zhongwei Jiang, Junyang Liu, Ke Yue, Man Pang, Yixuan Peng, Chongyang Luo, Ziqing Yao, Tao Pan, Yuanyuan Wang, Yujie Li, Qingpeng Guo, Chunman Zheng, Weiwei Sun, Xinyong Tao and Shuangke Liu","doi":"10.1039/D5EE02670A","DOIUrl":"10.1039/D5EE02670A","url":null,"abstract":"<p >Carbonate electrolytes are highly corrosive to lithium (Li) metal, leading to side reactions, dendrite growth and dead Li, which pose critical challenges in achieving stable high-energy Li metal batteries under a lean electrolyte. Here, we introduce a molecular surface reconstruction strategy to engineer a LiF/Li<small><sub>2</sub></small>O-rich solid electrolyte interphase (SEI) featuring high Li<small><sup>+</sup></small>-conductive hetero-grain boundaries. By spraying fluorinated ether-based carboxylic acid (PFOA) onto the Li metal surface, we eliminate the native oxide layer and engineer a self-optimized inorganic interphase that integrates exceptional mechanical robustness with rapid Li<small><sup>+</sup></small> transport along the hetero-grain boundaries. This dual functional interphase effectively suppresses Li dendrite growth and dead Li accumulation, as evidenced by microscopy visualization and isotope-labeled mass spectrometry titration (MST) techniques, with MST quantifying a significant reduction in dead Li and LiH within the modified SEI. Benefiting from the surface reconstruction strategy, a 5.8 Ah Li metal pouch cell achieves a high energy density of 518 Wh kg<small><sup>−1</sup></small> (based on the total mass of the cell) with an ultra-lean carbonate electrolyte (1.12 g Ah<small><sup>−1</sup></small>) and maintains stable cycling over 100 cycles. Our findings on surface reconstruction for a high Li<small><sup>+</sup></small> conductive hetero-grain boundary passivation layer point to a new pathway towards achieving stable cycling for energy dense Li metal batteries.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9240-9253"},"PeriodicalIF":30.8,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144915848","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}
Lu Zhang, Zuliang Zhuo, Xiaoling Ma, Hongyue Tian, Xingchao Zhao, Yongchao Xie, Kaixuan Yang, Byung Hui Lee, Xixiang Zhu, Han Young Woo, Chuluo Yang, Xiang Nie and Fujun Zhang
{"title":"19.6% efficiency of layer-by-layer organic photovoltaics with decreased energy loss via incorporating TADF materials with intrinsic reverse intersystem crossing","authors":"Lu Zhang, Zuliang Zhuo, Xiaoling Ma, Hongyue Tian, Xingchao Zhao, Yongchao Xie, Kaixuan Yang, Byung Hui Lee, Xixiang Zhu, Han Young Woo, Chuluo Yang, Xiang Nie and Fujun Zhang","doi":"10.1039/D5EE03118D","DOIUrl":"10.1039/D5EE03118D","url":null,"abstract":"<p >In this work, a thermally activated delayed fluorescence (TADF) material BN-STO is incorporated into the PM1 layer for preparing layer-by-layer organic photovoltaics (LOPVs) due to the intrinsic reverse intersystem crossing and long emission lifetime of BN-STO. The power conversion efficiency (PCE) of LOPVs can be enhanced from 18.54% to 19.65% by introducing 0.5 wt% BN-STO in the PM1 layer, originating from the increased exciton diffusion distance and reduced energy loss. The exciton diffusion distance in the PM1 layer can be increased from 33.06 nm to 59.93 nm by introducing 0.5 wt% BN-STO, which can be deduced from the photoluminescence dynamic decay process of PM1:BN-STO films and special layered PM1:BN-STO/C<small><sub>60</sub></small> films. The energy loss of optimal LOPVs is reduced from 0.5539 eV to 0.5379 eV due to the reverse intersystem crossing in L8-BO induced by BN-STO incorporation, which can be confirmed from the variation of singlet and triplet exciton excited state absorption peaks and intensity according to transient absorption spectra of L8-BO, L8-BO:PtOEP and L8-BO:PtOEP:BN-STO films. This work indicates that the performance improvement of LOPVs can be enhanced through improving the exciton diffusion distance assisted by energy transfer and decreasing energy loss <em>via</em> incorporating TADF materials with intrinsic intramolecular reverse intersystem crossing.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9171-9182"},"PeriodicalIF":30.8,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144915849","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}
Nan-Hai Li, Xiao-Lei Shi, Chao Zhang, Meng Li, Xiaodong Wang, Min Zhang, Wen-Yi Chen, Yong-Qi Chen, Dmitri Golberg, Dong-Chen Qi and Zhi-Gang Chen
{"title":"Manganese doping induced record-high medium-temperature AgCuTe thermoelectrics","authors":"Nan-Hai Li, Xiao-Lei Shi, Chao Zhang, Meng Li, Xiaodong Wang, Min Zhang, Wen-Yi Chen, Yong-Qi Chen, Dmitri Golberg, Dong-Chen Qi and Zhi-Gang Chen","doi":"10.1039/D5EE02875B","DOIUrl":"10.1039/D5EE02875B","url":null,"abstract":"<p >AgCuTe, a superionic conductor with high carrier mobility, ultra-low lattice thermal conductivity, unique crystal structure, and strong tunability of electron and phonon transport, is considered one of the most promising candidates for medium-temperature thermoelectric applications. However, its practical deployment has been hindered by insufficient optimization strategies, resulting in limited thermoelectric performance. In this study, we achieved a high dimensionless figure of merit (<em>ZT</em>) of ∼1.88 at 773 K in p-type manganese-doped polycrystalline AgCuTe, which is one of the highest reported values for AgCuTe-based materials and is comparable to other state-of-the-art medium-temperature thermoelectrics. This enhancement stems from band convergence and valence band flattening without compromising the intrinsically low thermal conductivity. Manganese doping effectively optimizes the electronic band structure to improve the power factor and simultaneously reduces lattice thermal conductivity through intensified lattice defects. These combined effects yield superior thermoelectric performance and higher average <em>ZT</em> values than previously reported p-type AgCuTe materials. Furthermore, a single-leg segmented thermoelectric module incorporating this material and commercial p-type (Bi, Sb)<small><sub>2</sub></small>Te<small><sub>3</sub></small> achieved a high energy conversion efficiency of ∼13.3% under a temperature difference of ∼462 K. This work highlights the effectiveness of electronic band structure engineering in enhancing the thermoelectric performance of superionic conductors.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 19","pages":" 8860-8875"},"PeriodicalIF":30.8,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144911130","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":"Deciphering failure mechanisms of Zn–S batteries: anion–cation synergy for dual-interface stabilization toward dendrite-free zinc and reversible sulfur conversion","authors":"Xiaolang Liu, Runming Tao, Gaoxu Huang, Yuxi Yang, Haiping Wang, Huiyu Yuan, Deyu Wang, Zhihong Liu, Jiyan Liu and Jiyuan Liang","doi":"10.1039/D5EE03758A","DOIUrl":"10.1039/D5EE03758A","url":null,"abstract":"<p >Rechargeable aqueous zinc–sulfur batteries (ZSBs) are promising candidates for large-scale energy storage due to their high theoretical capacity and cost-effectiveness. Generally, the reversible specific capacity of ZSBs can be enhanced by adding iodide catalysts, but their long-term cyclability remains an issue. Herein, this work comprehensively reveals that the loss of iodide ions (I<small><sup>−</sup></small>) on the cathode side is a major cause of limited cyclability. As a proof of concept, an anion–cation synergistic strategy is developed to effectively inhibit the loss of I<small><sup>−</sup></small> on the cathode side by introducing a choline cation (Ch<small><sup>+</sup></small>) for enhanced ZSB performance. Systematic electrochemical analyses and theoretical computational studies reveal that Ch<small><sup>+</sup></small> disrupts the hydrogen-bonding network of water, reduces reactive water activity, and modulates uniform Zn deposition, while Ch<small><sup>+</sup></small> and I<small><sup>−</sup></small> accelerate the redox kinetics of S through their synergistic action. Owing to the advantage of the strong adsorption of Ch<small><sup>+</sup></small> on the electrode interface, it not only inhibits the shuttle effect of iodine and improves the reversibility of the S cathode, but also inhibits the corrosion of the Zn anode. The ZSB catalyzed by I<small><sup>−</sup></small> with Ch<small><sup>+</sup></small> as the medium delivers a high specific capacity of 1240 mAh g<small><sup>−1</sup></small> at 0.5 A g<small><sup>−1</sup></small>, an enhanced cyclability (72% capacity retention after 2000 cycles at 5 A g<small><sup>−1</sup></small>) and superior anti-self-discharge performance (98.91% coulombic efficiency after 48 h). The success of the ZSB study at high sulfur loading (4.5 mg cm<small><sup>−2</sup></small>) under lean electrolyte conditions (<em>E</em>/<em>S</em> = 10 μL mg<small><sub>s</sub></small><small><sup>−1</sup></small>) demonstrates the potential practicality. This work establishes fundamental insights into the synergistic catalytic mechanisms of Ch<small><sup>+</sup></small>/I<small><sup>−</sup></small> for high-performance ZSBs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 20","pages":" 9158-9170"},"PeriodicalIF":30.8,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144911129","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}