Clara Schare, Giorgi Titvinidze, Christian Piesold, Edgar Cruz Ortiz, Nodar Dumbadze, Michael Schuster, Klaus‐Dieter Kreuer, Carolin Klose, Andreas Münchinger
Hydrocarbon (HC) membranes have the potential to significantly enhance the efficiency of water electrolyzers. However, their low mechanical integrity under electrolysis conditions, due to severe swelling, poses a challenge for industrial‐scale applications. Here, we present a 12 µm‐thick sulfonated poly(phenylene sulfone) (sPPS) membrane reinforced with a porous polyethylene (PE) substrate. The PE substrate reduces in‐plane swelling by a factor of 7 (10% vs 69%) and improves mechanical stability (440 MPa vs 50 MPa) in water at 60°C. Under electrolysis conditions, a 24 µm thick sandwich of two reinforced membranes shows stable operation over more than 2000 h in a constant current hold at 1 A cm −2 conducted at 60°C (first 1000 h) and 80°C (remaining 1000 h) with only 6 µV h −1 of voltage deviation within the last 500 h. With a potential of 1.67 V and a hydrogen in oxygen content of 1 vol% at 3 A cm −2 , the PFAS‐free membrane clearly outperforms a state‐of‐the‐art reference (Nafion‐N211: 1.73 V and 1.5 vol% at 3 A cm −2 ).
碳氢化合物（HC）膜具有显著提高水电解槽效率的潜力。然而，在电解条件下，由于严重的膨胀，它们的机械完整性很低，这对工业规模的应用提出了挑战。在这里，我们提出了一个12微米厚的磺化聚（苯基砜）（sPPS）膜，用多孔聚乙烯（PE）衬底增强。PE衬底可将平面内膨胀降低7倍（10% vs 69%），并在60°C的水中提高机械稳定性（440 MPa vs 50 MPa）。电解条件下,24µm厚三明治的两个钢筋膜显示稳定运行超过2000 h在恒定电流维持在1厘米−2进行了60°C(前1000 h)和80°C(剩余1000 h)只有6 Vµh−1的电压偏差在过去500 h。1.67 V的潜力和氢气在氧气含量在3厘米−1卷% 2,pfa检测自由膜明显优于高艺术自参考国家优先车道(全氟磺酸N211应承担:1.73 V和1.5 vol % 3厘米−2)。
{"title":"Thin Reinforced Sulfonated Poly(phenylene sulfone) Membranes for Durable Water Electrolysis: Suppressed Swelling and Enhanced Stability Over 2000 Hours","authors":"Clara Schare, Giorgi Titvinidze, Christian Piesold, Edgar Cruz Ortiz, Nodar Dumbadze, Michael Schuster, Klaus‐Dieter Kreuer, Carolin Klose, Andreas Münchinger","doi":"10.1002/aenm.202505888","DOIUrl":"https://doi.org/10.1002/aenm.202505888","url":null,"abstract":"Hydrocarbon (HC) membranes have the potential to significantly enhance the efficiency of water electrolyzers. However, their low mechanical integrity under electrolysis conditions, due to severe swelling, poses a challenge for industrial‐scale applications. Here, we present a 12 µm‐thick sulfonated poly(phenylene sulfone) (sPPS) membrane reinforced with a porous polyethylene (PE) substrate. The PE substrate reduces in‐plane swelling by a factor of 7 (10% vs 69%) and improves mechanical stability (440 MPa vs 50 MPa) in water at 60°C. Under electrolysis conditions, a 24 µm thick sandwich of two reinforced membranes shows stable operation over more than 2000 h in a constant current hold at 1 A cm <jats:sup>−2</jats:sup> conducted at 60°C (first 1000 h) and 80°C (remaining 1000 h) with only 6 µV h <jats:sup>−1</jats:sup> of voltage deviation within the last 500 h. With a potential of 1.67 V and a hydrogen in oxygen content of 1 vol% at 3 A cm <jats:sup>−2</jats:sup> , the PFAS‐free membrane clearly outperforms a state‐of‐the‐art reference (Nafion‐N211: 1.73 V and 1.5 vol% at 3 A cm <jats:sup>−2</jats:sup> ).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146014602","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 aluminum-ion batteries are promising for grid-scale energy storage due to their safety, low-cost, and high theoretical specific capacity. However, the development is hindered by the hydrogen evolution reaction from water splitting and corrosion, causing poor reversibility in aluminum plating/stripping. Utilizing strong anti-polyelectrolyte effect from aluminum cations and perchlorate anions, and the outstanding hydration strength from 2-methacryloyloxyethyl phosphorylcholine (MPC), this study introduces a novel polyzwitterionic hydrogel electrolyte (PZHE) for AAIBs with MPC monomer and aluminum perchlorate electrolyte. PZHE binds water molecules under lean-water conditions, greatly reducing free water activity and expanding the electrochemical stability window into 2.5 V. Despite limited water activity, ion migration channels created by zwitterionic phosphorylcholine groups enable high ionic conductivity of 4.22 mS cm−1 at 25°C. Consequently, the PZHE symmetrical cell achieves 600 h of reversible aluminum plating/stripping at a low overpotential of less than 0.2 V. With a potassium nickel hexacyanoferrate (KNHCF) cathode, the coin cell exhibits an initial discharge capacity of 66 mAh g−1 with a 1.2 V voltage plateau and retains 71% capacity after 400 cycles. Additionally, it demonstrates excellent capacity stability in the rest-cycling test (6 months) and pouch cell setup (200 cycles), highlighting its potential for grid-scale energy storage.
水铝离子电池因其安全、低成本和较高的理论比容量而在电网规模的储能中具有广阔的应用前景。但由于水裂解和腐蚀引起的析氢反应阻碍了其发展，导致镀铝/汽提的可逆性较差。利用铝阳离子和高氯酸盐阴离子具有较强的抗聚电解质作用，以及2-甲基丙烯酰氧乙基磷酸胆碱（MPC）具有较强的水合强度，研究了一种以MPC单体和高氯酸铝为电解质的aaib用聚两性离子水凝胶电解质（PZHE）。PZHE在稀水条件下结合水分子，大大降低了自由水活性，并将电化学稳定窗口扩大到2.5 V。尽管水活度有限，但两性磷胆碱基团产生的离子迁移通道在25°C时可实现4.22 mS cm−1的高离子电导率。因此，PZHE对称电池在低于0.2 V的低过电位下实现了600 h的可逆镀铝/剥离。采用六氰镍酸钾（KNHCF）阴极，硬币电池在1.2 V电压平台下的初始放电容量为66 mAh g−1，在400次循环后容量保持71%。此外，它在休息循环测试（6个月）和袋式电池设置（200个循环）中表现出出色的容量稳定性，突出了其在电网规模储能方面的潜力。
{"title":"Mitigating Hydrogen Evolution Reaction with Polyzwitterionic Hydrogel Electrolyte in Aqueous Aluminum-ion Batteries","authors":"Jin-Jie Liew, Bei-Er Jia, Dan-Yang Wang, Ziyue Wen, Hong-Han Choo, Jinxuan Song, Qiang Zhu, Man-Fai Ng, Qingyu Yan","doi":"10.1002/aenm.70677","DOIUrl":"https://doi.org/10.1002/aenm.70677","url":null,"abstract":"Aqueous aluminum-ion batteries are promising for grid-scale energy storage due to their safety, low-cost, and high theoretical specific capacity. However, the development is hindered by the hydrogen evolution reaction from water splitting and corrosion, causing poor reversibility in aluminum plating/stripping. Utilizing strong anti-polyelectrolyte effect from aluminum cations and perchlorate anions, and the outstanding hydration strength from 2-methacryloyloxyethyl phosphorylcholine (MPC), this study introduces a novel polyzwitterionic hydrogel electrolyte (PZHE) for AAIBs with MPC monomer and aluminum perchlorate electrolyte. PZHE binds water molecules under lean-water conditions, greatly reducing free water activity and expanding the electrochemical stability window into 2.5 V. Despite limited water activity, ion migration channels created by zwitterionic phosphorylcholine groups enable high ionic conductivity of 4.22 mS cm<sup>−1</sup> at 25°C. Consequently, the PZHE symmetrical cell achieves 600 h of reversible aluminum plating/stripping at a low overpotential of less than 0.2 V. With a potassium nickel hexacyanoferrate (KNHCF) cathode, the coin cell exhibits an initial discharge capacity of 66 mAh g<sup>−1</sup> with a 1.2 V voltage plateau and retains 71% capacity after 400 cycles. Additionally, it demonstrates excellent capacity stability in the rest-cycling test (6 months) and pouch cell setup (200 cycles), highlighting its potential for grid-scale energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022027","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}
Xabier Rodríguez-Martínez, Hongzheng Chen, Vida Turkovic, Feng Gao
Advances in Organic Photovoltaics
The cover highlights the five core topics of the Special Issue “Advances in Organic Photovoltaics”: (i) (photo)physics, device modelling, and machine-learning-driven studies in organic solar cells; (ii) design and synthesis of novel light-harvesting materials; (iii) sustainable, scalable processing of photoactive layers; (iv) enhanced thermal and mechanical device stability; and (v) building-integrated semi-transparent devices (e.g., smart windows). More in the Guest Editorial (e05958), Xabier Rodríguez-Martínez and co-authors.
该封面突出了特刊“有机光伏进展”的五个核心主题：(i)有机太阳能电池的（照片）物理，器件建模和机器学习驱动的研究；（ii）设计和合成新型光收集材料；（iii）可持续的、可扩展的光活性层处理；（iv）增强热和机械设备的稳定性；（五）建筑一体化半透明设备（如智能窗户）。更多信息请见客座编辑（e05958）， Xabier Rodríguez-Martínez和合著者。
{"title":"Advancing Organic Photovoltaics (Adv. Energy Mater. 3/2026)","authors":"Xabier Rodríguez-Martínez, Hongzheng Chen, Vida Turkovic, Feng Gao","doi":"10.1002/aenm.70569","DOIUrl":"10.1002/aenm.70569","url":null,"abstract":"<p><b>Advances in Organic Photovoltaics</b></p><p>The cover highlights the five core topics of the Special Issue “<i>Advances in Organic Photovoltaics</i>”: (i) (photo)physics, device modelling, and machine-learning-driven studies in organic solar cells; (ii) design and synthesis of novel light-harvesting materials; (iii) sustainable, scalable processing of photoactive layers; (iv) enhanced thermal and mechanical device stability; and (v) building-integrated semi-transparent devices (e.g., smart windows). More in the Guest Editorial (e05958), Xabier Rodríguez-Martínez and co-authors.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"16 3","pages":""},"PeriodicalIF":26.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://advanced.onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.70569","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146014612","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}
Chuanjun Wang, Hang Wang, Guifeng Zhou, Shilei Zhang, Min Zhang, Yang Wang, Xun Zhu, Qian Fu
Electrochemical CO2 reduction to multicarbon (C2+) products with high selectivity at industrial current densities using a membrane electrode assembly (MEA) electrolyzer in neutral electrolytes holds a great promise for carbon neutrality. However, the complex reaction pathways and low selectivity for C2+ products have hindered further development. Herein, an oxygen vacancy-engineered CuO nanoflower catalyst was designed to construct stable Cu0/Cu+ active interfaces and induce a localized alkaline microenvironment, effectively suppressing the competing hydrogen evolution reaction (HER) while enhancing ethylene (C2H4) selectivity. In situ spectroscopic characterization confirmed the stability of the Cu0/Cu+ active sites and their high *CO surface coverage. Multiphysics simulations combined with density functional theory (DFT) calculations revealed that the stable Cu0/Cu+ interface coupled with the localized alkaline microenvironment reduces the energy barrier for asymmetric C─C coupling, thereby boosting C2H4 selectivity. The optimized catalyst achieved remarkable C2H4 Faradaic efficiencies of 66.8% in alkaline and 66.1% in neutral electrolyte at a current density of 200 mA cm–2. This strategy of stabilizing Cu0/Cu+ interfaces coupled with microenvironment modulation offers novel insights for enabling highly selective CO2-to-C2H4 electrosynthesis at high current densities.
在工业电流密度下，使用膜电极组件（MEA）电解槽在中性电解质中电解CO2还原成具有高选择性的多碳（C2+）产品，具有很大的碳中性前景。然而，复杂的反应途径和低选择性的C2+产物阻碍了进一步的发展。本文设计了一种氧空位工程CuO纳米花催化剂，构建稳定的Cu0/Cu+活性界面，诱导局部碱性微环境，有效抑制竞争性析氢反应（HER），同时提高乙烯（C2H4）的选择性。原位光谱表征证实了Cu0/Cu+活性位点的稳定性及其高*CO表面覆盖率。多物理场模拟结合密度泛函理论（DFT）计算表明，稳定的Cu0/Cu+界面与局部碱性微环境的耦合降低了不对称C─C耦合的能量势垒，从而提高了C2H4的选择性。优化后的催化剂在200 mA cm-2电流密度下，C2H4在碱性电解质中的法拉第效率为66.8%，在中性电解质中的法拉第效率为66.1%。这种稳定Cu0/Cu+界面的策略与微环境调制相结合，为在高电流密度下实现高选择性CO2-to-C2H4电合成提供了新的见解。
{"title":"Highly Selective CO2 Electroreduction to Ethylene on Stable Cu0/Cu+ Interfaces by Local Microenvironment Modulation","authors":"Chuanjun Wang, Hang Wang, Guifeng Zhou, Shilei Zhang, Min Zhang, Yang Wang, Xun Zhu, Qian Fu","doi":"10.1002/aenm.202504744","DOIUrl":"https://doi.org/10.1002/aenm.202504744","url":null,"abstract":"Electrochemical CO<sub>2</sub> reduction to multicarbon (C<sub>2+</sub>) products with high selectivity at industrial current densities using a membrane electrode assembly (MEA) electrolyzer in neutral electrolytes holds a great promise for carbon neutrality. However, the complex reaction pathways and low selectivity for C<sub>2+</sub> products have hindered further development. Herein, an oxygen vacancy-engineered CuO nanoflower catalyst was designed to construct stable Cu<sup>0</sup>/Cu<sup>+</sup> active interfaces and induce a localized alkaline microenvironment, effectively suppressing the competing hydrogen evolution reaction (HER) while enhancing ethylene (C<sub>2</sub>H<sub>4</sub>) selectivity. In situ spectroscopic characterization confirmed the stability of the Cu<sup>0</sup>/Cu<sup>+</sup> active sites and their high *CO surface coverage. Multiphysics simulations combined with density functional theory (DFT) calculations revealed that the stable Cu<sup>0</sup>/Cu<sup>+</sup> interface coupled with the localized alkaline microenvironment reduces the energy barrier for asymmetric C─C coupling, thereby boosting C<sub>2</sub>H<sub>4</sub> selectivity. The optimized catalyst achieved remarkable C<sub>2</sub>H<sub>4</sub> Faradaic efficiencies of 66.8% in alkaline and 66.1% in neutral electrolyte at a current density of 200 mA cm<sup>–</sup><sup>2</sup>. This strategy of stabilizing Cu<sup>0</sup>/Cu<sup>+</sup> interfaces coupled with microenvironment modulation offers novel insights for enabling highly selective CO<sub>2</sub>-to-C<sub>2</sub>H<sub>4</sub> electrosynthesis at high current densities.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"142 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022029","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}
Hyeon Jun Jeong, Bora Kim, Ryosuke Nishikubo, Canjie Wang, Jongyoung Song, Yongjae In, Seokhun Han, Aedan Gibson, Urasawadee Amornkitbamrung, Atsushi Wakamiya, Akinori Saeki, Jooyoung Sung, Hyunjung Shin
Organic–inorganic halide perovskites have emerged as promising materials for next‐generation optoelectronic devices due to their exceptional photophysical properties. Among them, α‐formamidinium lead tri‐iodide (α‐FAPbI 3 ) with a cubic symmetry (space group of ) has garnered attention as a potential absorber in solar cells for its narrow bandgap and superior stability. The fundamental mechanisms governing its high performance have yet to be fully elucidated. In this study, we demonstrate that centrosymmetry breaking in [001] preferentially oriented α‐FAPbI 3 thin films (POF) arises from inevitable anisotropic strain during film formation. Using circular polarization‐dependent pump‐probe transient absorption spectroscopy, we observe Rashba‐type band splitting exclusively in POF, indicating symmetry breaking. Angle‐dependent X‐ray diffraction and photoluminescence (PL) reveal significant residual stress in POF compared to randomly oriented films (ROF), confirming strain‐induced lattice distortion. Furthermore, time‐resolved PL and microwave conductivity measurements reveal top‐back inhomogeneous carrier dynamics and anisotropic charge carrier mobility, supporting the presence of the anisotropic strain‐induced symmetry breaking. Our findings provide direct experimental evidence that inevitable strain in POF induces static Rashba effects, offering new insights into strain engineering for high‐performance perovskite optoelectronics and potential quantum applications.
{"title":"Anisotropic Strain‐Induced Centrosymmetry Breaking in Cubic Formamidinium Lead Iodide (α‐FAPbI 3 ) Thin Films","authors":"Hyeon Jun Jeong, Bora Kim, Ryosuke Nishikubo, Canjie Wang, Jongyoung Song, Yongjae In, Seokhun Han, Aedan Gibson, Urasawadee Amornkitbamrung, Atsushi Wakamiya, Akinori Saeki, Jooyoung Sung, Hyunjung Shin","doi":"10.1002/aenm.202506280","DOIUrl":"https://doi.org/10.1002/aenm.202506280","url":null,"abstract":"Organic–inorganic halide perovskites have emerged as promising materials for next‐generation optoelectronic devices due to their exceptional photophysical properties. Among them, α‐formamidinium lead tri‐iodide (α‐FAPbI <jats:sub>3</jats:sub> ) with a cubic symmetry (space group of ) has garnered attention as a potential absorber in solar cells for its narrow bandgap and superior stability. The fundamental mechanisms governing its high performance have yet to be fully elucidated. In this study, we demonstrate that centrosymmetry breaking in [001] preferentially oriented α‐FAPbI <jats:sub>3</jats:sub> thin films (POF) arises from inevitable anisotropic strain during film formation. Using circular polarization‐dependent pump‐probe transient absorption spectroscopy, we observe Rashba‐type band splitting exclusively in POF, indicating symmetry breaking. Angle‐dependent X‐ray diffraction and photoluminescence (PL) reveal significant residual stress in POF compared to randomly oriented films (ROF), confirming strain‐induced lattice distortion. Furthermore, time‐resolved PL and microwave conductivity measurements reveal top‐back inhomogeneous carrier dynamics and anisotropic charge carrier mobility, supporting the presence of the anisotropic strain‐induced symmetry breaking. Our findings provide direct experimental evidence that inevitable strain in POF induces static Rashba effects, offering new insights into strain engineering for high‐performance perovskite optoelectronics and potential quantum applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"57 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005807","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}
Neha Garg, Viorica-Alina Oltean, Daniel Brandell, Annukka Santasalo Aarnio
The rapid increase in electric vehicle (EV) adoption has significantly boosted the demand for lithium-ion batteries (LIBs), creating an urgent need for sustainable recycling strategies. Discharging end-of-life LIBs is a critical preprocessing step before recycling. Electrical discharge via cables is the current industrial state of the art for large battery packs, whereas electrochemical discharge (discharging batteries in solutions) offers a reliable alternative for smaller and mixed waste streams. This study compares electrical and electrochemical discharge methods and examines their effects on the morphology and composition of electrode materials from spent LIBs. Additionally, it evaluates the potential of electrochemical discharge to enable a closed-loop direct recycling process by recovering high-quality active materials from spent LIBs. Characterization results reveal that the lithium content is higher on negative electrode sheets after electrical discharge than after electrochemical discharge. Unreacted lithium on Ni-rich layered oxides can form residual lithium compounds, such as lithium carbonate (Li2CO3) and lithium hydroxide (LiOH), which can trigger undesirable side reactions. PXRD analysis indicates that positive electrode materials subjected to electrochemical discharge retain their layered structure with minimal cation mixing, unlike those subjected to electrical discharge. Overall, the findings demonstrate that electrochemical discharge is more effective in preserving the chemical composition and structural integrity of active materials than conventional electrical discharge methods.
{"title":"Impact of Discharging Methods on Electrode Integrity in Recycling of Lithium-Ion Batteries","authors":"Neha Garg, Viorica-Alina Oltean, Daniel Brandell, Annukka Santasalo Aarnio","doi":"10.1002/aenm.202505938","DOIUrl":"https://doi.org/10.1002/aenm.202505938","url":null,"abstract":"The rapid increase in electric vehicle (EV) adoption has significantly boosted the demand for lithium-ion batteries (LIBs), creating an urgent need for sustainable recycling strategies. Discharging end-of-life LIBs is a critical preprocessing step before recycling. Electrical discharge via cables is the current industrial state of the art for large battery packs, whereas electrochemical discharge (discharging batteries in solutions) offers a reliable alternative for smaller and mixed waste streams. This study compares electrical and electrochemical discharge methods and examines their effects on the morphology and composition of electrode materials from spent LIBs. Additionally, it evaluates the potential of electrochemical discharge to enable a closed-loop direct recycling process by recovering high-quality active materials from spent LIBs. Characterization results reveal that the lithium content is higher on negative electrode sheets after electrical discharge than after electrochemical discharge. Unreacted lithium on Ni-rich layered oxides can form residual lithium compounds, such as lithium carbonate (Li<sub>2</sub>CO<sub>3</sub>) and lithium hydroxide (LiOH), which can trigger undesirable side reactions. PXRD analysis indicates that positive electrode materials subjected to electrochemical discharge retain their layered structure with minimal cation mixing, unlike those subjected to electrical discharge. Overall, the findings demonstrate that electrochemical discharge is more effective in preserving the chemical composition and structural integrity of active materials than conventional electrical discharge methods.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"2 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005691","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}
Jonas Lindner, Ulrich Ross, Tobias Meyer, Sung Sakong, Axel Gross, Michael Seibt, Christian Jooss
Imaging atomic structure and electric fields of the electric double layer at electrode‐water interfaces is essential for understanding electrochemical reactions. The wave properties of electrons in an environmental transmission electron microscope were used to reconstruct the atomic scale electric potentials of a platinum (111) interface in water by phase shifting electron holography. This progress allowed the observation of ordered water layers at the dynamic state of the platinum (111) surface and the water reorganization under applied electric potentials. The obtained projected electric potential of the Pt‐water interface is quantitatively compared to ab‐initio molecular dynamics simulations, revealing an extended ordered water region. We conclude that the potential drop at the Pt ‐H 2 O interface is mainly carried by the polarization field of the ordered water structure. The impact of different surface Pt configurations and the presence of adsorbates on the ordered structure are discussed.
{"title":"Atomic Scale Ordering of Liquid Water at a Dynamic Pt(111) Interface Under Electrochemical Conditions Imaged by Electron Holography","authors":"Jonas Lindner, Ulrich Ross, Tobias Meyer, Sung Sakong, Axel Gross, Michael Seibt, Christian Jooss","doi":"10.1002/aenm.202505756","DOIUrl":"https://doi.org/10.1002/aenm.202505756","url":null,"abstract":"Imaging atomic structure and electric fields of the electric double layer at electrode‐water interfaces is essential for understanding electrochemical reactions. The wave properties of electrons in an environmental transmission electron microscope were used to reconstruct the atomic scale electric potentials of a platinum (111) interface in water by phase shifting electron holography. This progress allowed the observation of ordered water layers at the dynamic state of the platinum (111) surface and the water reorganization under applied electric potentials. The obtained projected electric potential of the Pt‐water interface is quantitatively compared to ab‐initio molecular dynamics simulations, revealing an extended ordered water region. We conclude that the potential drop at the Pt ‐H <jats:sub>2</jats:sub> O interface is mainly carried by the polarization field of the ordered water structure. The impact of different surface Pt configurations and the presence of adsorbates on the ordered structure are discussed.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"32 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006093","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}
Lithium plating on graphite anodes is a critical degradation pathway in lithium-ion batteries (LIBs), yet quantitative decoupling of its contribution from normal anode aging remains challenging. Here, we designed controlled Li plating tests using negative-to-positive (N/P) ratio < 1 LiFePO4/graphite cells and then compared them with practical fast-charging cells (N/P > 1), quantifying the decomposition of each electrolyte component (solvent, salt, additives) using nuclear magnetic resonance (NMR), mass spectrometry titration (MST), and gas chromatography-mass spectrometry (GC-MS). Controlled Li plating occurs after full graphite lithiation, and it leads to rapid vinylene carbonate (VC) depletion, time-dependent non-Faradaic consumption of hexafluorophosphate (PF6−)/ethyl methyl carbonate (EMC)/ethylene carbonate (EC), and more organic solid-electrolyte interphase (SEI) formation at higher rates. In routine fast-charging aging, Li plating occurs before graphite saturation, and we find pronounced EMC consumption under high-rate conditions compared with low - rate. Our comparative analysis indicates that VC consumption during fast charging originates not only from plating but also significantly from baseline graphite aging. Li plating likely induces SEI rupture, leading to direct contact with electrolyte, thus more organic SEI formation. This quantitative study enables decoupling of Li plating-induced side reactions from general aging without plating, informing battery design and predictive aging models.
{"title":"Decoupling Electrolyte Degradation Pathways With Diverse Li Plating Processes on Graphite Electrodes","authors":"Ke Zhang, Yonggang Hu, Shijun Tang, Wenxuan Hu, Jianrong Lin, Huiyan Zhang, Yufan Peng, Yuanzhe Tao, Yiqing Liao, Ying Lin, Lixuan Pan, Meifang Ding, Jinding Liang, Yimin Wei, Lufeng Yang, Jie Chen, Zhengliang Gong, Yanting Jin, Yong Yang","doi":"10.1002/aenm.202505230","DOIUrl":"https://doi.org/10.1002/aenm.202505230","url":null,"abstract":"Lithium plating on graphite anodes is a critical degradation pathway in lithium-ion batteries (LIBs), yet quantitative decoupling of its contribution from normal anode aging remains challenging. Here, we designed controlled Li plating tests using negative-to-positive (<i>N/P</i>) ratio < 1 LiFePO<sub>4</sub>/graphite cells and then compared them with practical fast-charging cells (<i>N/P</i> > 1), quantifying the decomposition of each electrolyte component (solvent, salt, additives) using nuclear magnetic resonance (NMR), mass spectrometry titration (MST), and gas chromatography-mass spectrometry (GC-MS). Controlled Li plating occurs after full graphite lithiation, and it leads to rapid vinylene carbonate (VC) depletion, time-dependent non-Faradaic consumption of hexafluorophosphate (PF<sub>6</sub><sup>−</sup>)/ethyl methyl carbonate (EMC)/ethylene carbonate (EC), and more organic solid-electrolyte interphase (SEI) formation at higher rates. In routine fast-charging aging, Li plating occurs before graphite saturation, and we find pronounced EMC consumption under high-rate conditions compared with low - rate. Our comparative analysis indicates that VC consumption during fast charging originates not only from plating but also significantly from baseline graphite aging. Li plating likely induces SEI rupture, leading to direct contact with electrolyte, thus more organic SEI formation. This quantitative study enables decoupling of Li plating-induced side reactions from general aging without plating, informing battery design and predictive aging models.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005707","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}
Jianchao Gao, Sisi Zhang, Chuang Jiang, Fangming Bai, Jiawei Yan, Wei Liu, Chenxiao Lin, Mingkai Liu
Zinc-ion batteries (ZIBs) have gained considerable attention as sustainable energy storage systems, offering advantages in capacity, safety, and cost. However, issues such as dendrite growth and side reactions hinder their practical adoption. Cellulose-based gel electrolytes (CGEs) have recently emerged as promising materials to mitigate these challenges. By inhibiting zinc dendrite formation and enhancing interfacial stability, CGEs improve cycling longevity and safety in ZIBs. This review begins by classifying gel electrolytes and outlining the distinctive benefits of CGEs prepared via crosslinking and non-crosslinking strategies. It then systematically examines recent developments in CGEs for use with various cathode materials and in multifunctional ZIBs configurations. Finally, the environmental merits and compelling electrochemical properties of CGEs are highlighted, together with a forward-looking discussion on their role in next-generation ZIBs and related future research directions. This work provides a timely and comprehensive resource that integrates materials design with electrochemical insights, offering valuable guidance for the rational development of CGEs.
{"title":"Rational Design of Cellulose-Based Gel Electrolytes for Next-Generation Zinc-Ion Batteries: Mechanisms, Advances, and Perspectives","authors":"Jianchao Gao, Sisi Zhang, Chuang Jiang, Fangming Bai, Jiawei Yan, Wei Liu, Chenxiao Lin, Mingkai Liu","doi":"10.1002/aenm.202506462","DOIUrl":"https://doi.org/10.1002/aenm.202506462","url":null,"abstract":"Zinc-ion batteries (ZIBs) have gained considerable attention as sustainable energy storage systems, offering advantages in capacity, safety, and cost. However, issues such as dendrite growth and side reactions hinder their practical adoption. Cellulose-based gel electrolytes (CGEs) have recently emerged as promising materials to mitigate these challenges. By inhibiting zinc dendrite formation and enhancing interfacial stability, CGEs improve cycling longevity and safety in ZIBs. This review begins by classifying gel electrolytes and outlining the distinctive benefits of CGEs prepared via crosslinking and non-crosslinking strategies. It then systematically examines recent developments in CGEs for use with various cathode materials and in multifunctional ZIBs configurations. Finally, the environmental merits and compelling electrochemical properties of CGEs are highlighted, together with a forward-looking discussion on their role in next-generation ZIBs and related future research directions. This work provides a timely and comprehensive resource that integrates materials design with electrochemical insights, offering valuable guidance for the rational development of CGEs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"47 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001559","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}
Lithium‐ion batteries (LIBs) are the most widely used commercial rechargeable batteries, but the stable supply of key raw materials such as lithium, nickel, and cobalt faces challenges. Sodium‐ion batteries (SIBs) are considered as potential alternatives and complements to LIBs due to similar working principles and the abundance of sodium resources. Layered oxide cathode materials (LOCMs) are recognized as one of the most promising practical cathodes for SIBs because of mature synthesis technology and satisfactory energy density. However, the use of nickel in LOCMs for SIBs has raised concerns about environmental pollution during nickel production and the risk of price volatility stemming from the widespread application of high‐nickel LOCMs for LIBs. Therefore, developing low‐cost nickel‐free LOCMs is crucial for enhancing the environmental friendliness and cost advantages of SIBs. For low‐cost LOCMs, this review discusses the feasibility of replacing Ni 2+ /Ni 4+ with Fe 3+ /Fe 4+ and Mn 3+ /Mn 4+ for charge compensation in SIBs, and summarizes the resulting critical scientific challenges (Fe migration, Mn dissolution, Jahn‐Teller effect, Na deficiency, and thermal instability). Economic efficiency assessment based on cost and electrochemical properties indicates that low‐cost LOCMs exhibit the highest cost‐performance ratio. Finally, to accelerate the commercialization of cost‐effective SIBs technologies, this review outlines promising development pathways of low‐cost LOCMs.
{"title":"Low‐Cost Layered Cathodes Toward Practical Sodium‐Ion Batteries: Scientific Challenges, Resolution Strategies, and Economic Efficiency","authors":"Xu Zhu, Shuai Sun, Mengting Liu, Peng‐Fei Wang","doi":"10.1002/aenm.202506411","DOIUrl":"https://doi.org/10.1002/aenm.202506411","url":null,"abstract":"Lithium‐ion batteries (LIBs) are the most widely used commercial rechargeable batteries, but the stable supply of key raw materials such as lithium, nickel, and cobalt faces challenges. Sodium‐ion batteries (SIBs) are considered as potential alternatives and complements to LIBs due to similar working principles and the abundance of sodium resources. Layered oxide cathode materials (LOCMs) are recognized as one of the most promising practical cathodes for SIBs because of mature synthesis technology and satisfactory energy density. However, the use of nickel in LOCMs for SIBs has raised concerns about environmental pollution during nickel production and the risk of price volatility stemming from the widespread application of high‐nickel LOCMs for LIBs. Therefore, developing low‐cost nickel‐free LOCMs is crucial for enhancing the environmental friendliness and cost advantages of SIBs. For low‐cost LOCMs, this review discusses the feasibility of replacing Ni <jats:sup>2+</jats:sup> /Ni <jats:sup>4+</jats:sup> with Fe <jats:sup>3+</jats:sup> /Fe <jats:sup>4+</jats:sup> and Mn <jats:sup>3+</jats:sup> /Mn <jats:sup>4+</jats:sup> for charge compensation in SIBs, and summarizes the resulting critical scientific challenges (Fe migration, Mn dissolution, Jahn‐Teller effect, Na deficiency, and thermal instability). Economic efficiency assessment based on cost and electrochemical properties indicates that low‐cost LOCMs exhibit the highest cost‐performance ratio. Finally, to accelerate the commercialization of cost‐effective SIBs technologies, this review outlines promising development pathways of low‐cost LOCMs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"183 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001578","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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