Jie Chen,Jialun Guo,Xinyu Wang,Longlong Duan,Weixing Chen,Jinmeng Zhu,Jiadong Li,Si Chen,Yifei Wang
The insufficient thermal stability and large conduction loss severely constrain the dielectric energy storage performance of ferroelectric polymer nanocomposites under elevated temperatures. Herein, a multi-scale architecture strategy employing thermally robust laminated ferroelectric polymer nanocomposites reinforced by calcium hydroxide@polydopamine nanoplates (Ca(OH)₂@PDA NPLs) was demonstrated exquisitely to realize ferroelectric polymer nanocomposites with excellent high-temperature capacitive energy storage. Synergistic deep traps formed in the designed nanocomposite effectively elevate breakdown strength and inhibit conduction loss under harsh thermal and electric field conditions, transcending the performance boundaries of conventional nanocomposites. Consequently, the impressive discharge energy density (Ue) of 5.86 J/cm³ was achieved in an optimized nanocomposite with a low loading of 0.12 wt% Ca(OH)₂@PDA NPLs (C-0.12-C) at 150 °C and 550 MV/m, representing a 410% enhancement over commercial BOPP (1.4 J/cm³ at 120°C). Specifically, C-0.12-C delivers a Ue of 3.03 J/cm³ with efficiency (η) >88.86% at 150 °C and 400 MV/m, exceeding the performance of state-of-the-art high-temperature ferroelectric polymer nanocomposites. Moreover, exceptional energy storage performance consistency and long-term durability have been demonstrated after distinct regions assessment and exposure (720 hours), the retention rates of Ue and η are 96.1%, 99.5% at 150°C, respectively. This contribution presents a viable strategy for boosting the high-temperature energy storage capacity and thermal stability of ferroelectric polymer nanocomposites, paving the way for advanced composite dielectrics in extreme environments.
{"title":"Boosting High-Temperature Capacitive Energy Storage in Laminated Ferroelectric Polymer Nanocomposites reinforced by Ca(OH)₂@PDA Nanoplates","authors":"Jie Chen,Jialun Guo,Xinyu Wang,Longlong Duan,Weixing Chen,Jinmeng Zhu,Jiadong Li,Si Chen,Yifei Wang","doi":"10.1039/d6ta07303d","DOIUrl":"https://doi.org/10.1039/d6ta07303d","url":null,"abstract":"The insufficient thermal stability and large conduction loss severely constrain the dielectric energy storage performance of ferroelectric polymer nanocomposites under elevated temperatures. Herein, a multi-scale architecture strategy employing thermally robust laminated ferroelectric polymer nanocomposites reinforced by calcium hydroxide@polydopamine nanoplates (Ca(OH)₂@PDA NPLs) was demonstrated exquisitely to realize ferroelectric polymer nanocomposites with excellent high-temperature capacitive energy storage. Synergistic deep traps formed in the designed nanocomposite effectively elevate breakdown strength and inhibit conduction loss under harsh thermal and electric field conditions, transcending the performance boundaries of conventional nanocomposites. Consequently, the impressive discharge energy density (Ue) of 5.86 J/cm³ was achieved in an optimized nanocomposite with a low loading of 0.12 wt% Ca(OH)₂@PDA NPLs (C-0.12-C) at 150 °C and 550 MV/m, representing a 410% enhancement over commercial BOPP (1.4 J/cm³ at 120°C). Specifically, C-0.12-C delivers a Ue of 3.03 J/cm³ with efficiency (η) >88.86% at 150 °C and 400 MV/m, exceeding the performance of state-of-the-art high-temperature ferroelectric polymer nanocomposites. Moreover, exceptional energy storage performance consistency and long-term durability have been demonstrated after distinct regions assessment and exposure (720 hours), the retention rates of Ue and η are 96.1%, 99.5% at 150°C, respectively. This contribution presents a viable strategy for boosting the high-temperature energy storage capacity and thermal stability of ferroelectric polymer nanocomposites, paving the way for advanced composite dielectrics in extreme environments.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281759","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Malaya Kumar Sahoo,Kismat Kumar Sahoo,Poonam Parkar,Deepak K Swain Abe,Brahmananda Chakraborty,Jogendra Nath Behera
Metal-organic frameworks (MOFs) have emerged as promising precatalysts for alkaline hydrogen evolution owing to their structural tunability; however, understanding their dynamic electrochemical reconstruction and the nature of the true catalytic phase remains a major challenge. Herein, we investigate the alkaline hydrogen evolution reaction (HER) performance of cobalt-imidazole-vanadate (CoVIm) and nickel-imidazole-vanadate (NiVIm) crystalline frameworks. The pristine CoVIm and NiVIm require overpotentials of 365 and 480 mV, respectively, to achieve a current density of 10 mA cm - 2 . During prolonged electrolysis, both frameworks undergo pronounced electrochemical self-activation, leading to significant enhancement of HER activity. In-situ Raman spectroscopy reveals that the activation process proceeds through a gradual bias-induced evolution of the local coordination environment rather than an instantaneous structural transformation.Complementary ex-situ PXRD, electron microscopy, and XPS analyses demonstrate that the reconstructed catalysts consist of Co(OH)2V(O)1.7(OH)0.3 and Ni(OH)2-Ni3(VO4)2 heterostructures, respectively. Consequently, the activated CoVIm exhibits an overpotential of only 185 mV at 10 mA cm -2 with a Tafel slope of 42 mV dec -1 , whereas activated NiVIm requires 380 mV with a Tafel slope of 54 mV dec -1 . Density functional theory calculations further reveal that the reconstructed Co(OH)2-V(O)1.7(OH)0.3 heterointerface provides more favourable hydrogen adsorption energetics than the individual components, accounting for the experimentally observed enhancement in HER activity. This work demonstrates that metal-imidazolevanadate frameworks function as self-reconstructing precatalysts and highlights the crucial role of electrochemical reconstruction in generating catalytically active heterointerfaces for efficient alkaline hydrogen evolution.
金属-有机骨架（mof）由于其结构的可调性而成为很有前途的碱氢析氢预催化剂；然而，了解它们的动态电化学重建和真正催化相的性质仍然是一个主要的挑战。本文研究了钴-咪唑-钒酸盐（CoVIm）和镍-咪唑-钒酸盐（NiVIm）晶体框架的碱性析氢反应（HER）性能。原始的CoVIm和NiVIm分别需要365和480 mV的过电位，以达到10 mA cm - 2的电流密度。在长时间的电解过程中，这两种框架都经历了明显的电化学自激活，导致HER活性显著增强。原位拉曼光谱显示，激活过程是通过局部配位环境的逐渐偏置演变而不是瞬间的结构转变进行的。互补的非原位PXRD、电镜和XPS分析表明，重构的催化剂分别由Co(OH)2V(O)1.7(OH)0.3和Ni(OH)2- ni3 (VO4)2异质结构组成。因此，激活后的CoVIm在10 mA cm -2下的过电位仅为185 mV， Tafel斜率为42 mV dec -1，而激活后的NiVIm需要380 mV， Tafel斜率为54 mV dec -1。密度泛函理论计算进一步表明，重构的Co(OH)2-V(O)1.7(OH)0.3异质界面比单个组分提供更有利的氢吸附能量，这是实验观察到的HER活性增强的原因。这项工作证明了金属-咪唑酸盐框架作为自重构预催化剂的功能，并强调了电化学重构在生成催化活性异质界面以实现高效碱氢析氢方面的关键作用。
{"title":"Bias-Induced Self-Reconstruction of Metal-Imidazole-Vanadate Frameworks for Enhanced Alkaline Hydrogen Evolution","authors":"Malaya Kumar Sahoo,Kismat Kumar Sahoo,Poonam Parkar,Deepak K Swain Abe,Brahmananda Chakraborty,Jogendra Nath Behera","doi":"10.1039/d6ta07416b","DOIUrl":"https://doi.org/10.1039/d6ta07416b","url":null,"abstract":"Metal-organic frameworks (MOFs) have emerged as promising precatalysts for alkaline hydrogen evolution owing to their structural tunability; however, understanding their dynamic electrochemical reconstruction and the nature of the true catalytic phase remains a major challenge. Herein, we investigate the alkaline hydrogen evolution reaction (HER) performance of cobalt-imidazole-vanadate (CoVIm) and nickel-imidazole-vanadate (NiVIm) crystalline frameworks. The pristine CoVIm and NiVIm require overpotentials of 365 and 480 mV, respectively, to achieve a current density of 10 mA cm - 2 . During prolonged electrolysis, both frameworks undergo pronounced electrochemical self-activation, leading to significant enhancement of HER activity. In-situ Raman spectroscopy reveals that the activation process proceeds through a gradual bias-induced evolution of the local coordination environment rather than an instantaneous structural transformation.Complementary ex-situ PXRD, electron microscopy, and XPS analyses demonstrate that the reconstructed catalysts consist of Co(OH)2V(O)1.7(OH)0.3 and Ni(OH)2-Ni3(VO4)2 heterostructures, respectively. Consequently, the activated CoVIm exhibits an overpotential of only 185 mV at 10 mA cm -2 with a Tafel slope of 42 mV dec -1 , whereas activated NiVIm requires 380 mV with a Tafel slope of 54 mV dec -1 . Density functional theory calculations further reveal that the reconstructed Co(OH)2-V(O)1.7(OH)0.3 heterointerface provides more favourable hydrogen adsorption energetics than the individual components, accounting for the experimentally observed enhancement in HER activity. This work demonstrates that metal-imidazolevanadate frameworks function as self-reconstructing precatalysts and highlights the crucial role of electrochemical reconstruction in generating catalytically active heterointerfaces for efficient alkaline hydrogen evolution.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281760","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
We developed a coordination polymer (CP)-derived, photostable, ion-conductive membrane electrolyte as a material platform for gas-fed photofuel cells. The CP precursor serves as a chemically transformable and mechanically processable medium, facilitating membrane and MEA fabrication prior to humidification-induced conversion into an ionicliquid/inorganic-filler hybrid membrane. The resulting membrane exhibited an H+ conductivity of 3.0 × 10-4 S cm-1 and supported stable power generation for 72 h at 25 °C/50% RH using water vapour and O2 feeds.
我们开发了一种配位聚合物（CP）衍生的、光稳定的、离子导电的膜电解质，作为气馈光燃料电池的材料平台。CP前体作为一种化学可转化和机械可加工的介质，在湿化诱导转化为离子液体/无机填料杂化膜之前，促进膜和MEA的制造。所得膜的H+电导率为3.0 × 10-4 S cm-1，在25°C/50% RH条件下使用水蒸气和O2可稳定发电72 H。
{"title":"Coordination polymer-derived ion-conductive electrolyte for a gas-fed photofuel cell","authors":"Yuji Namiki,Hiroyasu Tabe,Karnjana Atthawilai,Takeshi Watanabe,Kanokwan Kongpatpanich,Satoshi Horike","doi":"10.1039/d6ta05966j","DOIUrl":"https://doi.org/10.1039/d6ta05966j","url":null,"abstract":"We developed a coordination polymer (CP)-derived, photostable, ion-conductive membrane electrolyte as a material platform for gas-fed photofuel cells. The CP precursor serves as a chemically transformable and mechanically processable medium, facilitating membrane and MEA fabrication prior to humidification-induced conversion into an ionicliquid/inorganic-filler hybrid membrane. The resulting membrane exhibited an H+ conductivity of 3.0 × 10-4 S cm-1 and supported stable power generation for 72 h at 25 °C/50% RH using water vapour and O2 feeds.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Commercial NiOx nanoparticles are attractive hole-transport materials for inverted perovskite solar cells, but their uncontrolled surface redox chemistry and nonideal energy-level alignment often lead to interfacial recombination and poor stability. Here, we report a facile aqueous-ammonia (NH3·H2O) treatment to regulate the surface redox state and electronic structure of commercial NiOx. The treatment selectively reduces the vacancy-related Ni3+ species and modifies hydroxyl-related oxygen species, shifts the NiOx surface energy levels upward, and suppresses interfacial trap-assisted recombination at the buried contact. These surface modifications provide a more favorable hole-selective contact environment for subsequent perovskite deposition, leading to improved crystallinity, enhanced hole extraction, and reduced interfacial non-radiative recombination. As a result, the optimized inverted device achieves a champion power conversion efficiency of 23.24%, compared with 20.11% for the control device. The unencapsulated treated devices also show improved stability, retaining 92.02% of their initial PCE after 15 days at 60 °C in a nitrogen atmosphere and 85.56% after 15 days under ambient conditions. This work establishes aqueous ammonia treatment as a facile route to convert commercially available NiOx into a more favorable buried-contact platform for efficient and durable inverted perovskite solar cells.
{"title":"Surface redox regulation of commercial NiO by aqueous ammonia for durable inverted perovskite solar cells","authors":"Yu Jiang,Kuina Yuan,Xisheng Zhang,Fanyue Kong,Jiawei Wang,Jiaqi Du,Yongqi Yin,Yusuke Yamauchi","doi":"10.1039/d6ta05855h","DOIUrl":"https://doi.org/10.1039/d6ta05855h","url":null,"abstract":"Commercial NiOx nanoparticles are attractive hole-transport materials for inverted perovskite solar cells, but their uncontrolled surface redox chemistry and nonideal energy-level alignment often lead to interfacial recombination and poor stability. Here, we report a facile aqueous-ammonia (NH3·H2O) treatment to regulate the surface redox state and electronic structure of commercial NiOx. The treatment selectively reduces the vacancy-related Ni3+ species and modifies hydroxyl-related oxygen species, shifts the NiOx surface energy levels upward, and suppresses interfacial trap-assisted recombination at the buried contact. These surface modifications provide a more favorable hole-selective contact environment for subsequent perovskite deposition, leading to improved crystallinity, enhanced hole extraction, and reduced interfacial non-radiative recombination. As a result, the optimized inverted device achieves a champion power conversion efficiency of 23.24%, compared with 20.11% for the control device. The unencapsulated treated devices also show improved stability, retaining 92.02% of their initial PCE after 15 days at 60 °C in a nitrogen atmosphere and 85.56% after 15 days under ambient conditions. This work establishes aqueous ammonia treatment as a facile route to convert commercially available NiOx into a more favorable buried-contact platform for efficient and durable inverted perovskite solar cells.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nicole Abdou,Maria Enrica Di Pietro,Franca Castiglione,Lars Evenäs,Andrea Mele,Anna Martinelli
Ionic liquids incorporated into solid polymer matrices offer a promising approach for developing mechanically stable electrolytes while maintaining favorable ion-transport properties. Here, ion dynamics and molecular organization are investigated in biphasic solid electrolytes, composed of a methacrylate-based polymer phase and a liquid electrolyte phase that contains a protic ionic liquid and a lithium salt. Pulsed-field gradient spin-echo (PGSE) and heteronuclear Overhauser effect spectroscopy (HOESY) NMR were selected for this purpose. The materials were studied as a function of temperature and polymer-to-liquid electrolyte ratio. Upon increasing polymer content, the cations mobility decreases, whilst the self-diffusion of the anions remains relatively insensitive to changes in composition and temperature. HOESY measurements showed decreasing 1H-19F cross-relaxation rates with increasing polymer content, indicating weaker cation-anion interactions and suggesting preferential interactions between the cationic species and the polymer matrix. These results show that composition and interfacial interactions strongly influence ion organization and local transport, providing molecular-level insights for the optimization of lithium-ion-conducting solid electrolytes.
{"title":"Structure-Dynamics Correlations in Ionic Liquid-Based Solid Electrolytes Explored by NMR Spectroscopy","authors":"Nicole Abdou,Maria Enrica Di Pietro,Franca Castiglione,Lars Evenäs,Andrea Mele,Anna Martinelli","doi":"10.1039/d6ta07722f","DOIUrl":"https://doi.org/10.1039/d6ta07722f","url":null,"abstract":"Ionic liquids incorporated into solid polymer matrices offer a promising approach for developing mechanically stable electrolytes while maintaining favorable ion-transport properties. Here, ion dynamics and molecular organization are investigated in biphasic solid electrolytes, composed of a methacrylate-based polymer phase and a liquid electrolyte phase that contains a protic ionic liquid and a lithium salt. Pulsed-field gradient spin-echo (PGSE) and heteronuclear Overhauser effect spectroscopy (HOESY) NMR were selected for this purpose. The materials were studied as a function of temperature and polymer-to-liquid electrolyte ratio. Upon increasing polymer content, the cations mobility decreases, whilst the self-diffusion of the anions remains relatively insensitive to changes in composition and temperature. HOESY measurements showed decreasing 1H-19F cross-relaxation rates with increasing polymer content, indicating weaker cation-anion interactions and suggesting preferential interactions between the cationic species and the polymer matrix. These results show that composition and interfacial interactions strongly influence ion organization and local transport, providing molecular-level insights for the optimization of lithium-ion-conducting solid electrolytes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"43 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Residual strain and defects, inevitably induced during thin-film fabrication and device operation by internal and external factors such as lattice mismatch, thermal stress, and external stimuli, severely limit the performance enhancement of perovskite solar cells (Pero-SCs). In this study, sulfur/oxygen-containing small molecules methyl thiophene-2-carboxylate (MTC) and dimethyl 2,5-thiophenedicarboxylate (DTD), which possess defect-passivation capabilities, are introduced as additives into Pero-SCs. The investigation revealed that the carbonyl groups (C=O) within these molecules act as Lewis bases, directly passivating undercoordinated Pb 2+ defects. Crucially, the unique dual-carbonyl spacing of the DTD molecule (6.32 Å) exhibits a high degree of matching with the lattice Pb-Pb distance of perovskite crystals (6.37 Å). Such structural matching optimizes the crystal growth orientation of perovskite films and significantly mitigates lattice distortion and growth stress.Benefiting from DTD optimization, the modified Pero-SCs achieved a champion power conversion efficiency (PCE) of 25.32%. Furthermore, unencapsulated devices retained 93% of their initial PCE after 3600 hours of storage in a N2 glovebox, and maintained 88% of their initial PCE after 720 hours of storage under ambient conditions (room temperature, 30-40% relative humidity).
{"title":"Dual-Site Coordination Engineering: Synergistic Passivation and Strain Relaxation via Lattice-Matched Small Molecules","authors":"Xuemei Lai,Ruicheng Tao,Wenxi Ji,Pan Xu,Qiaoyun Chen,Yuanyuan Zeng,Ming Yin,Lijie Wang,Xiaoting Nie,Zelong Zhang,Ming-Ao Pan,Xiafei Cheng,Xinmiao Niu,Yi Zhou,Bo Song","doi":"10.1039/d6ta07749h","DOIUrl":"https://doi.org/10.1039/d6ta07749h","url":null,"abstract":"Residual strain and defects, inevitably induced during thin-film fabrication and device operation by internal and external factors such as lattice mismatch, thermal stress, and external stimuli, severely limit the performance enhancement of perovskite solar cells (Pero-SCs). In this study, sulfur/oxygen-containing small molecules methyl thiophene-2-carboxylate (MTC) and dimethyl 2,5-thiophenedicarboxylate (DTD), which possess defect-passivation capabilities, are introduced as additives into Pero-SCs. The investigation revealed that the carbonyl groups (C=O) within these molecules act as Lewis bases, directly passivating undercoordinated Pb 2+ defects. Crucially, the unique dual-carbonyl spacing of the DTD molecule (6.32 Å) exhibits a high degree of matching with the lattice Pb-Pb distance of perovskite crystals (6.37 Å). Such structural matching optimizes the crystal growth orientation of perovskite films and significantly mitigates lattice distortion and growth stress.Benefiting from DTD optimization, the modified Pero-SCs achieved a champion power conversion efficiency (PCE) of 25.32%. Furthermore, unencapsulated devices retained 93% of their initial PCE after 3600 hours of storage in a N2 glovebox, and maintained 88% of their initial PCE after 720 hours of storage under ambient conditions (room temperature, 30-40% relative humidity).","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"254 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149272060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Veronica F. Michel,Oliver Von Grünigen,Markus Niederberger
Gel polymer electrolytes (GPEs) derived from biodegradable materials offer a promising route towards sustainable battery technologies. In this work, we revalorize two abundant food waste streams, spent coffee grounds and shrimp shells, into bio-derived GPEs. Specifically, we extract the polysaccharide-rich fraction (PRF) from spent coffee grounds and combine it with commercial chitosan from shrimp shells. We systematically screen PRF:chitosan ratios between 50:50 and 100:0 and investigate their physicochemical, mechanical, and electrochemical properties. We find that the PRF forms a hierarchical porous network, while chitosan enhances the mechanical stability of the GPEs. Ionic conductivities peak around 20 mS/cm for 70-80% PRF, and all compositions exhibit electrochemical stability up to 2 V vs Zn2+/Zn. The GPE containing 80% PRF was incorporated into Zn-MnO2 pouch cells that showed an open circuit voltage of 1.38 V and initial capacity of 166.6 mAh/g. The pouch cells successfully powered an LED device and sustained 600 charge-discharge cycles, demonstrating the practical applicability of this waste-derived GPE in aqueous battery systems. Under simulated aerobic composting conditions, the GPE furthermore shows fast and complete disintegration. This study presents a pathway to repurpose food waste into functional battery components, advancing environmentally responsible and bio-circular energy-storage technologies.
从可生物降解材料中提取的凝胶聚合物电解质（GPEs）为可持续电池技术提供了一条有前途的途径。在这项工作中，我们重新评估了两种丰富的食物废物流，废咖啡渣和虾壳，转化为生物衍生的gpe。具体地说，我们从废咖啡渣中提取了富含多糖的部分（PRF），并将其与虾壳的商业壳聚糖结合。我们系统地筛选了PRF：壳聚糖在50:50和100:0之间的比例，并研究了它们的物理化学、机械和电化学性能。我们发现PRF形成了层次化的多孔网络，壳聚糖增强了gpe的力学稳定性。当PRF为70-80%时，离子电导率峰值约为20 mS/cm，所有成分的电化学稳定性高达2 V vs Zn2+/Zn。将含有80% PRF的GPE加入Zn-MnO2袋状电池中，其开路电压为1.38 V，初始容量为166.6 mAh/g。袋状电池成功地为LED设备供电，并维持了600次充放电循环，证明了这种废物衍生的GPE在水性电池系统中的实际适用性。在模拟好氧堆肥条件下，GPE进一步表现出快速和完全的分解。这项研究提出了一种将食物垃圾转化为功能性电池组件的途径，推进了对环境负责的生物循环储能技术。
{"title":"Toward bio-circular energy storage: Revalorization of food waste for gel polymer electrolytes in aqueous batteries","authors":"Veronica F. Michel,Oliver Von Grünigen,Markus Niederberger","doi":"10.1039/d6ta05208h","DOIUrl":"https://doi.org/10.1039/d6ta05208h","url":null,"abstract":"Gel polymer electrolytes (GPEs) derived from biodegradable materials offer a promising route towards sustainable battery technologies. In this work, we revalorize two abundant food waste streams, spent coffee grounds and shrimp shells, into bio-derived GPEs. Specifically, we extract the polysaccharide-rich fraction (PRF) from spent coffee grounds and combine it with commercial chitosan from shrimp shells. We systematically screen PRF:chitosan ratios between 50:50 and 100:0 and investigate their physicochemical, mechanical, and electrochemical properties. We find that the PRF forms a hierarchical porous network, while chitosan enhances the mechanical stability of the GPEs. Ionic conductivities peak around 20 mS/cm for 70-80% PRF, and all compositions exhibit electrochemical stability up to 2 V vs Zn2+/Zn. The GPE containing 80% PRF was incorporated into Zn-MnO2 pouch cells that showed an open circuit voltage of 1.38 V and initial capacity of 166.6 mAh/g. The pouch cells successfully powered an LED device and sustained 600 charge-discharge cycles, demonstrating the practical applicability of this waste-derived GPE in aqueous battery systems. Under simulated aerobic composting conditions, the GPE furthermore shows fast and complete disintegration. This study presents a pathway to repurpose food waste into functional battery components, advancing environmentally responsible and bio-circular energy-storage technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149272071","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anqi Li,Yuedan Wang,Yun Lin,Menglin Xu,Wenwen Wang,Qiongzhen Liu,Dong Wang
To overcome the limitations of single-function optical materials, a dual-response system integrating dynamic fluorescence and photochromism was developed based on the composite of lanthanide metal-organic framework (Ln-MOF) and tungsten oxide (WO3 ). The Ln-MOF@WO 3 composite was fabricated and characterized by SEM, XRD, and FT-IR etc. Under UV excitation, the system exhibits a dual-mode response. The fluorescence intensity gradually decreases within 30 s, while the material color changes from colorless to blue (color difference up to 36.4). The composite retains the photochromic reversibility of WO 3 (1 min coloration, 10 min bleaching) and displays long-lived luminescence (λ em =615 nm, τ ave =5.418 ms). The color and fluorescence are highly reversibly photoswitchable under alternating UV/visible light. Meanwhile, after 10 washing cycles and 30 days of ambient storage, this textile still maintained excellent color change and luminescence stability. The color-changing luminescence mechanism of the entire system and interface were explored. Based on this composite, light-activated luminescent hydrogels, photoswitchable electrospun nanofiber membranes, and light-switching inks were further fabricated. Performance tests demonstrate rapid dual-mode response and reversible switching capability, which are essential for time-resolved optical security applications. The Ln-MOF@WO3 composite represents a promising time-dependent, dual-mode dynamic responsive flexible material for advanced information encryption, dynamic anti-counterfeiting, and visual ion detection etc.
{"title":"Dynamic luminescent and photochromic Ln-MOF@WO3 flexible material for multi-level anti-counterfeiting encryption and visual detection","authors":"Anqi Li,Yuedan Wang,Yun Lin,Menglin Xu,Wenwen Wang,Qiongzhen Liu,Dong Wang","doi":"10.1039/d6ta07301h","DOIUrl":"https://doi.org/10.1039/d6ta07301h","url":null,"abstract":"To overcome the limitations of single-function optical materials, a dual-response system integrating dynamic fluorescence and photochromism was developed based on the composite of lanthanide metal-organic framework (Ln-MOF) and tungsten oxide (WO3 ). The Ln-MOF@WO 3 composite was fabricated and characterized by SEM, XRD, and FT-IR etc. Under UV excitation, the system exhibits a dual-mode response. The fluorescence intensity gradually decreases within 30 s, while the material color changes from colorless to blue (color difference up to 36.4). The composite retains the photochromic reversibility of WO 3 (1 min coloration, 10 min bleaching) and displays long-lived luminescence (λ em =615 nm, τ ave =5.418 ms). The color and fluorescence are highly reversibly photoswitchable under alternating UV/visible light. Meanwhile, after 10 washing cycles and 30 days of ambient storage, this textile still maintained excellent color change and luminescence stability. The color-changing luminescence mechanism of the entire system and interface were explored. Based on this composite, light-activated luminescent hydrogels, photoswitchable electrospun nanofiber membranes, and light-switching inks were further fabricated. Performance tests demonstrate rapid dual-mode response and reversible switching capability, which are essential for time-resolved optical security applications. The Ln-MOF@WO3 composite represents a promising time-dependent, dual-mode dynamic responsive flexible material for advanced information encryption, dynamic anti-counterfeiting, and visual ion detection etc.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"17 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149272064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A simple and scalable strategy has been developed for the in situ fabrication of a self-supported oxygen evolution reaction (OER) electrode consisting of a nanocomposite layer of metallic NiFe nanoparticles and NixFe3-xO4 (NPs/NFO). Anodizing electroplated Fe-Ni produces an oxyfluoride precursor film, which converts into the NPs/NFO composite via low-temperature post-annealing (673 K) in a nitrogen atmosphere without external reductants.During annealing, fluorine desorption and matrix reconstruction into NixFe3-xO4 accompany the exsolution of metallic NiFe nanoparticles. Solid-state two-terminal I-V measurements demonstrate higher through-plane electrical conductivity for the NPs/NFO film compared to the s-NFO film, resulting in an electrochemically active surface area (ECSA) 7.7 times larger. The optimized NPs/NFO electrode exhibits an overpotential of 0.324 V at 10 mA cm⁻² and a Tafel slope of 38.4 mV dec⁻¹. Ex situ X-ray photoelectron and Raman spectroscopies revealed that both the s-NFO and NPs/NFO films developed essentially the same surface chemical states and structural characteristics after OER, consistent with the formation of NiFe (oxy)hydroxide species through surface reconstruction while largely retaining the underlying spinel framework. Thus, the enhanced OER performance of NPs/NFO film is unlikely to originate from differences in surface active species, but is mainly attributed to its enlarged ECSA and enhanced electrical conductivity. This enhanced conductivity is suggested to promote a more uniform current distribution within the porous structure, which may contribute to the improved resistance of the NPs/NFO film to localized degradation and delamination during accelerated durability tests (ADTs) under accelerated shutdown conditions associated with intermittent alkaline water electrolysis.
本文提出了一种简单、可扩展的原位制备自支撑析氧反应（OER）电极的方法，该电极由金属NiFe纳米颗粒和NixFe3-xO4 （NPs/NFO）纳米复合层组成。电镀Fe-Ni阳极氧化制备氟氧前驱体膜，在无外部还原剂的氮气气氛下经低温后退火（673 K）转化为NPs/NFO复合材料。在退火过程中，氟的解吸和基体重构为NixFe3-xO4，并伴有金属NiFe纳米颗粒的析出。固态双端I-V测量表明，与s-NFO膜相比，NPs/NFO膜的通平面导电性更高，导致电化学活性表面积（ECSA）增加7.7倍。优化后的NPs/NFO电极在10 mA cm⁻²时的过电位为0.324 V， Tafel斜率为38.4 mV dec⁻¹。非原位x射线光电子和拉曼光谱显示，经过OER处理后，s-NFO和NPs/NFO薄膜的表面化学状态和结构特征基本相同，与通过表面重建形成的NiFe（氧）氢氧化物相一致，同时基本保留了底层尖晶石骨架。因此，NPs/NFO膜OER性能的增强不太可能源于表面活性物质的差异，而主要归因于其ECSA的扩大和导电性的增强。这种增强的电导率可以促进多孔结构内更均匀的电流分布，这可能有助于提高NPs/NFO膜在加速耐久性测试（ADTs）中在与间歇性碱性电解相关的加速关闭条件下的局部降解和分层的抵抗能力。
{"title":"Nanoporous NiFe/NiFeO nanocomposites as self-supported electrodes via low-temperature exsolution for efficient oxygen evolution and with enhanced durability","authors":"Yoshiki Konno,Takayo Yamamoto,Tomio Nagayama","doi":"10.1039/d6ta03458f","DOIUrl":"https://doi.org/10.1039/d6ta03458f","url":null,"abstract":"A simple and scalable strategy has been developed for the in situ fabrication of a self-supported oxygen evolution reaction (OER) electrode consisting of a nanocomposite layer of metallic NiFe nanoparticles and NixFe3-xO4 (NPs/NFO). Anodizing electroplated Fe-Ni produces an oxyfluoride precursor film, which converts into the NPs/NFO composite via low-temperature post-annealing (673 K) in a nitrogen atmosphere without external reductants.During annealing, fluorine desorption and matrix reconstruction into NixFe3-xO4 accompany the exsolution of metallic NiFe nanoparticles. Solid-state two-terminal I-V measurements demonstrate higher through-plane electrical conductivity for the NPs/NFO film compared to the s-NFO film, resulting in an electrochemically active surface area (ECSA) 7.7 times larger. The optimized NPs/NFO electrode exhibits an overpotential of 0.324 V at 10 mA cm⁻² and a Tafel slope of 38.4 mV dec⁻¹. Ex situ X-ray photoelectron and Raman spectroscopies revealed that both the s-NFO and NPs/NFO films developed essentially the same surface chemical states and structural characteristics after OER, consistent with the formation of NiFe (oxy)hydroxide species through surface reconstruction while largely retaining the underlying spinel framework. Thus, the enhanced OER performance of NPs/NFO film is unlikely to originate from differences in surface active species, but is mainly attributed to its enlarged ECSA and enhanced electrical conductivity. This enhanced conductivity is suggested to promote a more uniform current distribution within the porous structure, which may contribute to the improved resistance of the NPs/NFO film to localized degradation and delamination during accelerated durability tests (ADTs) under accelerated shutdown conditions associated with intermittent alkaline water electrolysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"43 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149272062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dongjun Lee,Doyeon Lee,Jaeyoung Hong,Seong-Hyeon Hong
A series of olivine-type lithium manganese iron phosphate (LiMnxFe1-xPO4, LMFP; x = 0.5, 0.6, 0.7, and 0.8) powders are synthesized via a solvothermal method and evaluated as cathode materials for lithium-ion batteries, focusing on composition-dependent electrochemical degradation. Comparable particle morphology and size minimize the extrinsic morphological differences. Cycling-induced degradation appears as capacity fading and voltage decay, with the latter becoming more pronounced as Mn content increases. Mn-rich compositions exhibit severe polarization growth, indicating increasing kinetic limitations in the high-voltage Mn-redox region. Partial recovery of the Mn-redox plateau following lower-rate cycling supports a kinetic contribution to this voltage depression. Ex-situ structural analyses reveal more pronounced structural disorder in Mn-rich LMFP, particularly in LMFP 82 (x=0.8) after a prolonged cycling, supporting a structural contribution to hindered Li ion transport and increased polarization. The Mn content recovered from the Li counter electrodes increases with Mn content, supporting the more pronounced Mn dissolution and deposition. Ex-situ XPS and ToF-SIMS analyses indicate the composition-dependent changes in interphase chemistry. These results indicate that Mn-rich LMFP degradation involves the coupled evolution of structural disorder, Mn dissolution, and interfacial changes. Among these factors, Mn content-dependent structural disorder is an important contributor to the kinetic limitations, alongside interfacial processes. These kinetic limitations contribute to greater losses of operating voltage and cathode-specific discharge energy despite relatively comparable capacity retention.
{"title":"Composition-dependent degradation of manganese-rich olivine cathodes","authors":"Dongjun Lee,Doyeon Lee,Jaeyoung Hong,Seong-Hyeon Hong","doi":"10.1039/d6ta06239c","DOIUrl":"https://doi.org/10.1039/d6ta06239c","url":null,"abstract":"A series of olivine-type lithium manganese iron phosphate (LiMnxFe1-xPO4, LMFP; x = 0.5, 0.6, 0.7, and 0.8) powders are synthesized via a solvothermal method and evaluated as cathode materials for lithium-ion batteries, focusing on composition-dependent electrochemical degradation. Comparable particle morphology and size minimize the extrinsic morphological differences. Cycling-induced degradation appears as capacity fading and voltage decay, with the latter becoming more pronounced as Mn content increases. Mn-rich compositions exhibit severe polarization growth, indicating increasing kinetic limitations in the high-voltage Mn-redox region. Partial recovery of the Mn-redox plateau following lower-rate cycling supports a kinetic contribution to this voltage depression. Ex-situ structural analyses reveal more pronounced structural disorder in Mn-rich LMFP, particularly in LMFP 82 (x=0.8) after a prolonged cycling, supporting a structural contribution to hindered Li ion transport and increased polarization. The Mn content recovered from the Li counter electrodes increases with Mn content, supporting the more pronounced Mn dissolution and deposition. Ex-situ XPS and ToF-SIMS analyses indicate the composition-dependent changes in interphase chemistry. These results indicate that Mn-rich LMFP degradation involves the coupled evolution of structural disorder, Mn dissolution, and interfacial changes. Among these factors, Mn content-dependent structural disorder is an important contributor to the kinetic limitations, alongside interfacial processes. These kinetic limitations contribute to greater losses of operating voltage and cathode-specific discharge energy despite relatively comparable capacity retention.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"58 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149251065","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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