The global crises of resource scarcity, energy shortages, and environmental degradation demand innovative solutions for sustainable development. Solar-driven interfacial evaporation (SIE) has emerged as a transformative technology for recovering resource/energy from seawater or wastewater. Despite SIE's high evaporation efficiency at the gas–liquid interface, significant challenges persist, including volatile organic compound (VOC) enrichment, selective separation limitations, and energy trade-offs in multifunctional systems. Accordingly, this work provides a comprehensive overview of recent SIE systems for resource/energy recovery while establishing novel dynamics and thermodynamics frameworks to guide their design and application. By shifting the paradigm from “water purification” to a “resource/energy factory”, SIE systems can offer a promising pathway toward carbon neutrality.
{"title":"Advanced solar-driven interfacial evaporation technology for resource and energy recovery","authors":"Xiaoqiang Cui, Shicheng Dong, Ningning Cao, Xuchen Zhang, Junxia Wang, Haiguang Fu, Beibei Yan, Zhen Yu, Miao Yu and Guanyi Chen","doi":"10.1039/D5EE05041C","DOIUrl":"10.1039/D5EE05041C","url":null,"abstract":"<p >The global crises of resource scarcity, energy shortages, and environmental degradation demand innovative solutions for sustainable development. Solar-driven interfacial evaporation (SIE) has emerged as a transformative technology for recovering resource/energy from seawater or wastewater. Despite SIE's high evaporation efficiency at the gas–liquid interface, significant challenges persist, including volatile organic compound (VOC) enrichment, selective separation limitations, and energy trade-offs in multifunctional systems. Accordingly, this work provides a comprehensive overview of recent SIE systems for resource/energy recovery while establishing novel dynamics and thermodynamics frameworks to guide their design and application. By shifting the paradigm from “water purification” to a “resource/energy factory”, SIE systems can offer a promising pathway toward carbon neutrality.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 446-459"},"PeriodicalIF":30.8,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760232","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}
Namrata Sharma, Louis Godeffroy, Peer Bärmann, Faidra Amargianou, Andreas Weisser, Zoé Dessoliers, Mailis Lounasvuori, Markus Weigand and Tristan Petit
Pseudocapacitive materials store electrochemical energy through fast and reversible surface charge transfer reactions. Titanium carbide MXenes are two-dimensional materials which have shown redox or intercalation pseudocapacitive properties depending on the electrolyte. Nevertheless, the intrinsic pseudocapacitive charging mechanism in individual MXene flakes remains unresolved. Here, we employ in situ scanning transmission X-ray microscopy (STXM) to map the local chemical changes in individual Ti3C2Tx MXene flakes during spontaneous and electrochemical intercalation of protons and lithium ions in aqueous electrolytes. Our investigations reveal that proton and lithium-ion intercalation induces a reduction and an oxidation, respectively, of the titanium atoms in the MXene. This difference reveals a profoundly different chemical origin between redox and intercalation pseudocapacitive processes. By elucidating the interplay between ion hydration, MXene surface chemistry and flake morphology, our study highlights the relevance of chemical imaging in single entities for the fundamental understanding of electrochemical charge storage mechanisms.
{"title":"Nanoscale chemical imaging of pseudocapacitive charge storage in MXenes","authors":"Namrata Sharma, Louis Godeffroy, Peer Bärmann, Faidra Amargianou, Andreas Weisser, Zoé Dessoliers, Mailis Lounasvuori, Markus Weigand and Tristan Petit","doi":"10.1039/D5EE05809K","DOIUrl":"10.1039/D5EE05809K","url":null,"abstract":"<p >Pseudocapacitive materials store electrochemical energy through fast and reversible surface charge transfer reactions. Titanium carbide MXenes are two-dimensional materials which have shown redox or intercalation pseudocapacitive properties depending on the electrolyte. Nevertheless, the intrinsic pseudocapacitive charging mechanism in individual MXene flakes remains unresolved. Here, we employ <em>in situ</em> scanning transmission X-ray microscopy (STXM) to map the local chemical changes in individual Ti<small><sub>3</sub></small>C<small><sub>2</sub></small>T<small><sub>x</sub></small> MXene flakes during spontaneous and electrochemical intercalation of protons and lithium ions in aqueous electrolytes. Our investigations reveal that proton and lithium-ion intercalation induces a reduction and an oxidation, respectively, of the titanium atoms in the MXene. This difference reveals a profoundly different chemical origin between redox and intercalation pseudocapacitive processes. By elucidating the interplay between ion hydration, MXene surface chemistry and flake morphology, our study highlights the relevance of chemical imaging in single entities for the fundamental understanding of electrochemical charge storage mechanisms.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 680-690"},"PeriodicalIF":30.8,"publicationDate":"2025-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ee/d5ee05809k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760234","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}
Proton exchange kinetics plays an important role in governing the performance of intermediate-temperature protonic ceramic electrolysis cells (PCECs) for hydrogen production. Our understanding of the nature of the surface hydration reaction at the single-cell level, however, remains very limited, hampering further efficiency improvements. Here, we developed a custom operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) platform that operates under high temperature and steam conditions with applied bias. Quantitative investigations of surface H2O/D2O isotope exchange in a BaZr0.1Ce0.7Y0.1Yb0.1O3−δ (BZCYYb1711) protonic electrolyte-based single cell were conducted under different applied voltages using this DRIFTS platform, to gain molecular-level insight into hydration kinetics. The findings show that the application of an external voltage significantly enhances the surface proton exchange rate, decreasing the apparent activation energy from 29.1 kJ mol−1 at open-circuit voltage (OCV) to 6.8 kJ mol−1 at 1.3 V. In addition, distinct voltage-induced spectral shifts in O–D vibrations point to dynamic changes in surface hydration. These findings demonstrate a sensitive spectroscopic platform for probing interfacial proton processes and reveal strong electrochemical control over surface proton kinetics, offering new opportunities for probing electrolyte hydration behavior in PCECs.
{"title":"Probing the proton exchange kinetics of BaZr0.1Ce0.7Y0.1Yb0.1O3−δ ceramic electrolyte by operando diffuse reflectance infrared Fourier transform spectroscopy","authors":"Yuqing Meng, Fan Liu, Meng Li, Zixian Wang, Hao Deng, Qian Zhang, Haixia Li, Wanhua Wang, Quanwen Sun, Joshua Gomez, Zeyu Zhao, Haiyan Zhao and Dong Ding","doi":"10.1039/D5EE05957G","DOIUrl":"10.1039/D5EE05957G","url":null,"abstract":"<p >Proton exchange kinetics plays an important role in governing the performance of intermediate-temperature protonic ceramic electrolysis cells (PCECs) for hydrogen production. Our understanding of the nature of the surface hydration reaction at the single-cell level, however, remains very limited, hampering further efficiency improvements. Here, we developed a custom <em>operando</em> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) platform that operates under high temperature and steam conditions with applied bias. Quantitative investigations of surface H<small><sub>2</sub></small>O/D<small><sub>2</sub></small>O isotope exchange in a BaZr<small><sub>0.1</sub></small>Ce<small><sub>0.7</sub></small>Y<small><sub>0.1</sub></small>Yb<small><sub>0.1</sub></small>O<small><sub>3−<em>δ</em></sub></small> (BZCYYb1711) protonic electrolyte-based single cell were conducted under different applied voltages using this DRIFTS platform, to gain molecular-level insight into hydration kinetics. The findings show that the application of an external voltage significantly enhances the surface proton exchange rate, decreasing the apparent activation energy from 29.1 kJ mol<small><sup>−1</sup></small> at open-circuit voltage (OCV) to 6.8 kJ mol<small><sup>−1</sup></small> at 1.3 V. In addition, distinct voltage-induced spectral shifts in O–D vibrations point to dynamic changes in surface hydration. These findings demonstrate a sensitive spectroscopic platform for probing interfacial proton processes and reveal strong electrochemical control over surface proton kinetics, offering new opportunities for probing electrolyte hydration behavior in PCECs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 3","pages":" 828-835"},"PeriodicalIF":30.8,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760235","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}
Li Liu, Hongju Zhu, Jin-Yun Wang, Di Wang, Dongdong Cai, Jianbin Wang, Qisheng Tu, Yunlong Ma and Qingdong Zheng
Dimerized M-series small-molecule acceptors feature highly planar conjugated backbones, enabling ordered stacking and enhanced morphological stability. However, rotatable bonds introduced during dimerization often induce conformational disorder, undermining efficient charge generation and transport. Here, we report two rationally designed M-series dimers, DM-TF and DMF-T, which both incorporate strategic intramolecular fluorine⋯hydrogen interactions to enhance conformational rigidity. DM-TF, which features fluorinated thiophene π-bridges interacting with hydrogen atoms on the central end groups, exhibits superior conformational rigidity, reduced energetic disorder, improved crystallinity, and enhanced charge transport properties compared to DMF-T. Consequently, DM-TF-based organic solar cells (OSCs) deliver a power conversion efficiency of 18.40%, surpassing the DMF-T-based devices (17.77%). Additionally, they demonstrate exceptional thermal stability, exhibiting negligible performance loss after being heated at 80 °C for 2000 hours. Furthermore, incorporating DM-TF as a third component into PM6:M36 blends boosts the efficiency of the resulting devices to 19.16%, which is the highest reported value among all non-Y-series acceptors. These results underscore the effectiveness of engineering intramolecular non-covalent interactions in the molecular design of acceptor materials and highlight the great potential of dimerized M-series acceptors for high-efficiency and stable OSCs.
{"title":"Conformational locking through intramolecular F⋯H interactions in dimerized M-series acceptors boosts efficiency and stability of organic solar cells","authors":"Li Liu, Hongju Zhu, Jin-Yun Wang, Di Wang, Dongdong Cai, Jianbin Wang, Qisheng Tu, Yunlong Ma and Qingdong Zheng","doi":"10.1039/D5EE06043E","DOIUrl":"10.1039/D5EE06043E","url":null,"abstract":"<p >Dimerized M-series small-molecule acceptors feature highly planar conjugated backbones, enabling ordered stacking and enhanced morphological stability. However, rotatable bonds introduced during dimerization often induce conformational disorder, undermining efficient charge generation and transport. Here, we report two rationally designed M-series dimers, DM-TF and DMF-T, which both incorporate strategic intramolecular fluorine⋯hydrogen interactions to enhance conformational rigidity. DM-TF, which features fluorinated thiophene π-bridges interacting with hydrogen atoms on the central end groups, exhibits superior conformational rigidity, reduced energetic disorder, improved crystallinity, and enhanced charge transport properties compared to DMF-T. Consequently, DM-TF-based organic solar cells (OSCs) deliver a power conversion efficiency of 18.40%, surpassing the DMF-T-based devices (17.77%). Additionally, they demonstrate exceptional thermal stability, exhibiting negligible performance loss after being heated at 80 °C for 2000 hours. Furthermore, incorporating DM-TF as a third component into PM6:M36 blends boosts the efficiency of the resulting devices to 19.16%, which is the highest reported value among all non-Y-series acceptors. These results underscore the effectiveness of engineering intramolecular non-covalent interactions in the molecular design of acceptor materials and highlight the great potential of dimerized M-series acceptors for high-efficiency and stable OSCs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 551-560"},"PeriodicalIF":30.8,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718067","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}
Lei Zhang, Qiaoling Xu, Mengshan Chen, Yongcai Zhang, Yingtang Zhou, Guangzhi Hu and Hermenegildo Garcia
Efficient metal-free catalysts are crucial for advancing aluminum–air batteries (AABs), yet their development has been hindered by poor electronic structure optimization and sluggish mass transport. In this study, we developed a hierarchically porous N/S co-doped carbon nanoreactor via an etching-doping pyrolysis strategy, achieving an ultrahigh surface area of 2630 m2 g−1 and a well-organized pore network. The resulting catalyst demonstrated outstanding oxygen reduction reaction (ORR) activity, with half-wave potentials of 0.952 V (vs. RHE; RHE stands for reversible hydrogen electrode) in alkaline and 0.754 V (vs. RHE) in acidic media. When assembled into AABs, it delivered a peak power density of 265 mW cm−2 and an energy density of 4152 Wh kg−1, along with excellent cycling stability. Finite element simulations showed that the hierarchical porosity promoted oxygen diffusion and enhanced reaction kinetics. Furthermore, in situ characterization and theoretical calculations revealed that S–C–N configurations dynamically transformed into Opre–S–C–N groups under working conditions, which modulated the electronic structure of adjacent carbon sites, facilitated *O-to-*OH conversion, and reduced energy barriers. This study provided a dynamic site-regulation strategy for improving ORR kinetics in metal-free catalysts and offered a new pathway for designing high-performance energy materials operating under realistic conditions.
{"title":"Self-optimizing metal-free porous reactors with dynamic active sites unlock record oxygen reduction activity","authors":"Lei Zhang, Qiaoling Xu, Mengshan Chen, Yongcai Zhang, Yingtang Zhou, Guangzhi Hu and Hermenegildo Garcia","doi":"10.1039/D5EE03645C","DOIUrl":"10.1039/D5EE03645C","url":null,"abstract":"<p >Efficient metal-free catalysts are crucial for advancing aluminum–air batteries (AABs), yet their development has been hindered by poor electronic structure optimization and sluggish mass transport. In this study, we developed a hierarchically porous N/S co-doped carbon nanoreactor <em>via</em> an etching-doping pyrolysis strategy, achieving an ultrahigh surface area of 2630 m<small><sup>2</sup></small> g<small><sup>−1</sup></small> and a well-organized pore network. The resulting catalyst demonstrated outstanding oxygen reduction reaction (ORR) activity, with half-wave potentials of 0.952 V (<em>vs.</em> RHE; RHE stands for reversible hydrogen electrode) in alkaline and 0.754 V (<em>vs.</em> RHE) in acidic media. When assembled into AABs, it delivered a peak power density of 265 mW cm<small><sup>−2</sup></small> and an energy density of 4152 Wh kg<small><sup>−1</sup></small>, along with excellent cycling stability. Finite element simulations showed that the hierarchical porosity promoted oxygen diffusion and enhanced reaction kinetics. Furthermore, <em>in situ</em> characterization and theoretical calculations revealed that S–C–N configurations dynamically transformed into O<small><sub>pre</sub></small>–S–C–N groups under working conditions, which modulated the electronic structure of adjacent carbon sites, facilitated *O-to-*OH conversion, and reduced energy barriers. This study provided a dynamic site-regulation strategy for improving ORR kinetics in metal-free catalysts and offered a new pathway for designing high-performance energy materials operating under realistic conditions.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 702-717"},"PeriodicalIF":30.8,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711353","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}
In aqueous zinc (Zn) metal secondary batteries, some interfacial side reactions, such as the hydrogen evolution reaction (HER), anode corrosion and dendrite growth, often lead to short circuit and cycling performance deterioration. Here we select four kinds of amino acid monomers (i.e., lysine, glutamate, cysteine and phenylalanine) with different polarity side chain groups to tailor pentapeptides, successfully constructing a thermodynamically stable colloid dispersion electrolyte system with the Tyndall effect for Zn metal secondary batteries. The proposed electrolyte system composed of the tailored lysine pentapeptide (LP) effectively suppresses Zn dendrite growth through regulating the (002) crystalline plane orientation. Furthermore, the LP has strong attraction towards H2O molecules, thereby achieving desolvation of Zn2+ ions and reducing anode corrosion as well as the HER. In this LP-based colloid dispersion electrolyte, the Zn//Zn symmetric cell demonstrated an unprecedented ultralong cycling time beyond 10 000 hours (416 days) at 2 mA cm−2. The developed Zn-ion pouch cells with a high cathode mass loading of ∼ 28.7 mg cm−2 displayed a capacity retention of ∼83.7% after 1000 cycles at 0.5 A g−1, which is superior to most recently reported zinc-ion pouch cells. The proposed thermodynamically stable colloid dispersion electrolyte is a new aqueous electrolyte system for economical, safe and long-lifespan Zn metal secondary batteries.
在含水锌(Zn)金属二次电池中,析氢反应(HER)、阳极腐蚀和枝晶生长等界面副反应往往会导致电池短路和循环性能下降。本文通过筛选具有不同极性侧链基团的4种氨基酸单体(赖氨酸、谷氨酸、半胱氨酸和苯丙氨酸)来定制五肽,成功构建了具有Tyndall效应的锌金属二次电池热稳定胶体分散电解质体系。由定制赖氨酸五肽(LP)组成的电解质体系通过调节(002)晶面取向,有效抑制Zn枝晶生长。此外,LP对H2O分子有很强的吸引力,从而实现Zn2+离子的脱溶,减少阳极腐蚀和HER。在这种基于lp的胶体分散电解质中,锌/锌对称电池在2 mA cm-2下的超长循环时间超过了10000小时(416天)。在0.5 a g-1条件下,经过1000次循环后,锌离子袋电池的容量保持率为83.7%,其阴极质量负载高达~ 28.7 mg cm-2,优于最近报道的锌离子袋电池。本文提出的热稳定胶体分散电解质是一种经济、安全、长寿命锌金属二次电池的新型水电解质体系。
{"title":"Thermodynamically stable colloid dispersion electrolytes with the Tyndall effect for practical zinc-ion pouch cells","authors":"Yu Liu, Jiaxin Meng, Mohan Yue, Changmei Jiao, Zhiyuan Zhao, Yuzhen Sun, Yingna Chang, Huayu Wu, Xiaoli Yan, Kefan Song, Jindi Wang, Weizhai Bao, Guozhen Zhang, Rong Xing, Jingfa Li, Feng Yu, Faxing Wang and Yuping Wu","doi":"10.1039/D5EE05434F","DOIUrl":"10.1039/D5EE05434F","url":null,"abstract":"<p >In aqueous zinc (Zn) metal secondary batteries, some interfacial side reactions, such as the hydrogen evolution reaction (HER), anode corrosion and dendrite growth, often lead to short circuit and cycling performance deterioration. Here we select four kinds of amino acid monomers (<em>i.e.</em>, lysine, glutamate, cysteine and phenylalanine) with different polarity side chain groups to tailor pentapeptides, successfully constructing a thermodynamically stable colloid dispersion electrolyte system with the Tyndall effect for Zn metal secondary batteries. The proposed electrolyte system composed of the tailored lysine pentapeptide (LP) effectively suppresses Zn dendrite growth through regulating the (002) crystalline plane orientation. Furthermore, the LP has strong attraction towards H<small><sub>2</sub></small>O molecules, thereby achieving desolvation of Zn<small><sup>2+</sup></small> ions and reducing anode corrosion as well as the HER. In this LP-based colloid dispersion electrolyte, the Zn//Zn symmetric cell demonstrated an unprecedented ultralong cycling time beyond 10 000 hours (416 days) at 2 mA cm<small><sup>−2</sup></small>. The developed Zn-ion pouch cells with a high cathode mass loading of ∼ 28.7 mg cm<small><sup>−2</sup></small> displayed a capacity retention of ∼83.7% after 1000 cycles at 0.5 A g<small><sup>−1</sup></small>, which is superior to most recently reported zinc-ion pouch cells. The proposed thermodynamically stable colloid dispersion electrolyte is a new aqueous electrolyte system for economical, safe and long-lifespan Zn metal secondary batteries.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 589-604"},"PeriodicalIF":30.8,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The synergistic regulation of steam utilization and proton transport at the oxygen electrode is crucial for proton ceramic electrolysis cells (PCECs). Ruddlesden–Popper (RP) perovskites leverage interlayer water intercalation features to achieve rapid proton uptake even under low-steam conditions. Herein, an RP-type oxygen electrode capable of reversible phase transitions and hydrated oxyhydroxide formation under high-temperature steam was constructed, successfully transcending the hydration limits of single perovskites. By integrating the structural analysis employing microcrystal electron diffraction (MicroED) and density functional theory (DFT) calculations, it is revealed that the interlayer proton-trapping sites significantly boost the steam adsorption/hydration and lower the energy barrier for proton migration across layers. The Sr3(Co0.8Fe0.1Nb0.1)2O7−δ (SCFN-RP) electrode demonstrates excellent catalytic activity, reaching 1.01 A cm−2@1.3 V at 550 °C. This work emphasizes the crucial role of reversible hydrated oxyhydroxides in RP perovskites and offers a novel conception for the design of high-performance oxygen electrodes for PCECs.
蒸汽利用和质子在氧电极上传输的协同调节对质子陶瓷电解电池(PCECs)至关重要。Ruddlesden-Popper (RP)钙钛矿利用层间水嵌入特性,即使在低蒸汽条件下也能快速吸收质子。本文构建了一种rp型氧电极,能够在高温蒸汽下实现可逆相变和水合氢氧化物的生成,成功地超越了单一钙钛矿的水化极限。通过结合微晶电子衍射(MicroED)和密度泛函理论(DFT)计算的结构分析,揭示了层间质子捕获位点显著提高了蒸汽吸附/水合作用,降低了质子跨层迁移的能垒。Sr3(Co0.8Fe0.1Nb0.1)2O7−δ (SCFN-RP)电极表现出优异的催化活性,在550℃时达到1.01 A cm−2@1.3 V。本研究强调了可逆水合氢氧化物在RP钙钛矿中的重要作用,并为pcec高性能氧电极的设计提供了新的思路。
{"title":"The interlayer proton capture and transport mechanism in oxygen electrodes boosts proton ceramic electrolysis","authors":"Meijuan Fei, Zhaohui Cai, Peng Chen, Dongliang Liu, Cheng Huang, Jianqiu Zhu, Linjuan Zhang, Wei Wang, Chuan Zhou, Wei Zhou and Zongping Shao","doi":"10.1039/D5EE05802C","DOIUrl":"10.1039/D5EE05802C","url":null,"abstract":"<p >The synergistic regulation of steam utilization and proton transport at the oxygen electrode is crucial for proton ceramic electrolysis cells (PCECs). Ruddlesden–Popper (RP) perovskites leverage interlayer water intercalation features to achieve rapid proton uptake even under low-steam conditions. Herein, an RP-type oxygen electrode capable of reversible phase transitions and hydrated oxyhydroxide formation under high-temperature steam was constructed, successfully transcending the hydration limits of single perovskites. By integrating the structural analysis employing microcrystal electron diffraction (MicroED) and density functional theory (DFT) calculations, it is revealed that the interlayer proton-trapping sites significantly boost the steam adsorption/hydration and lower the energy barrier for proton migration across layers. The Sr<small><sub>3</sub></small>(Co<small><sub>0.8</sub></small>Fe<small><sub>0.1</sub></small>Nb<small><sub>0.1</sub></small>)<small><sub>2</sub></small>O<small><sub>7−<em>δ</em></sub></small> (SCFN-RP) electrode demonstrates excellent catalytic activity, reaching 1.01 A cm<small><sup>−2</sup></small>@1.3 V at 550 °C. This work emphasizes the crucial role of reversible hydrated oxyhydroxides in RP perovskites and offers a novel conception for the design of high-performance oxygen electrodes for PCECs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 1","pages":" 349-358"},"PeriodicalIF":30.8,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711352","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}
Deng Hu, Hang Luo, Guanghu He, Xi Chen, Yuting Wan, Fan Wang, Xiaona Li, Huan Wang, Haoran Xie and Dou Zhang
Film capacitors are indispensable in electrical engineering; however, balancing the insulation and thermal stability of polymer dielectrics remains a key challenge for high-temperature energy storage. Aromatic polyimide (PI) exhibits a high glass transition temperature (Tg, >300 °C), facilitating the formation of charge transfer complexes (CTCs). Semi-aromatic PIs mitigate this order, but insufficient thermal stability leads to poor performance above 200 °C. To resolve this contradiction, we incorporated a sp3-centered monomer, tris(4-aminophenyl)methane (TAPM), into a semi-aromatic PI (MPD-PI), constructing a spatially disordered architecture that suppresses short-range π–π stacking and CTCs, enhancing dielectric insulation and thermal stability. The resulting copolymer specifically achieves a discharged energy density of 7.13 J cm−3 at 200 °C with 90% efficiency and 5.18 J cm−3 at 250 °C, representing 341% and 280% improvements compared to those of MPD-PI, respectively. The improved thermal stability also imparts excellent cycling stability (3 × 105 cycles at 200 °C and 300 MV m−1) and a state-of-the-art breakdown strength of 596.2 MV m−1 at 250 °C. The conformational-engineering strategy of this work provides a versatile route for high-temperature polymer dielectrics.
薄膜电容器在电气工程中是不可缺少的;然而,平衡聚合物电介质的绝缘性和热稳定性仍然是高温储能的关键挑战。芳香族聚酰亚胺(PI)具有较高的玻璃化转变温度(Tg, >300℃),有利于电荷转移配合物(ctc)的形成。半芳香族pi减轻了这一顺序,但热稳定性不足导致200°C以上性能不佳。为了解决这一矛盾,我们将sp3为中心的单体三(4-氨基苯基)甲烷(TAPM)加入到半芳香PI (MPD-PI)中,构建了一种空间无序结构,抑制了短程π -π堆叠和ctc,提高了介电绝缘性和热稳定性。该共聚物在200°C时的放电能量密度为7.13 J cm−3,效率为90%;在250°C时的放电能量密度为5.18 J cm−3,与MPD-PI相比,分别提高了341%和280%。改进的热稳定性也赋予了优异的循环稳定性(在200°C和300 MV m - 1下循环3 × 105次)和250°C下596.2 MV m - 1的最先进击穿强度。这项工作的构象工程策略为高温聚合物电介质提供了一条通用的途径。
{"title":"Disruption of short-range π–π stacking via a disordered spatial architecture for energy storage at 250 °C","authors":"Deng Hu, Hang Luo, Guanghu He, Xi Chen, Yuting Wan, Fan Wang, Xiaona Li, Huan Wang, Haoran Xie and Dou Zhang","doi":"10.1039/D5EE05932A","DOIUrl":"10.1039/D5EE05932A","url":null,"abstract":"<p >Film capacitors are indispensable in electrical engineering; however, balancing the insulation and thermal stability of polymer dielectrics remains a key challenge for high-temperature energy storage. Aromatic polyimide (PI) exhibits a high glass transition temperature (<em>T</em><small><sub>g</sub></small>, >300 °C), facilitating the formation of charge transfer complexes (CTCs). Semi-aromatic PIs mitigate this order, but insufficient thermal stability leads to poor performance above 200 °C. To resolve this contradiction, we incorporated a sp<small><sup>3</sup></small>-centered monomer, tris(4-aminophenyl)methane (TAPM), into a semi-aromatic PI (MPD-PI), constructing a spatially disordered architecture that suppresses short-range π–π stacking and CTCs, enhancing dielectric insulation and thermal stability. The resulting copolymer specifically achieves a discharged energy density of 7.13 J cm<small><sup>−3</sup></small> at 200 °C with 90% efficiency and 5.18 J cm<small><sup>−3</sup></small> at 250 °C, representing 341% and 280% improvements compared to those of MPD-PI, respectively. The improved thermal stability also imparts excellent cycling stability (3 × 10<small><sup>5</sup></small> cycles at 200 °C and 300 MV m<small><sup>−1</sup></small>) and a state-of-the-art breakdown strength of 596.2 MV m<small><sup>−1</sup></small> at 250 °C. The conformational-engineering strategy of this work provides a versatile route for high-temperature polymer dielectrics.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 1","pages":" 327-337"},"PeriodicalIF":30.8,"publicationDate":"2025-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145704751","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}
Ziqi Liu, Yiming Zhang, Shanshan Pan, Yong Chen, Keer Yang, Shanxi Wu, Musong Liu, Lei Hu, Shuaicheng Jiang, Xiaopeng Wang, Guoxiu Wang and Meng Yao
The rapid growth of electric vehicles (EVs) is driving an urgent demand for lithium-ion batteries (LIBs) with higher specific energy, longer life, and uncompromised safety. Ni-rich layered oxides (LiNixCoyMn(1−x−y)O2, x ≥ 0.8) have emerged as leading cathode materials for next-generation LIBs, owing to their high capacity and energy density. Further increasing Ni content is essential for improved performance and cost reduction. However, it also introduces new obstacles, necessitating thoughtful design of cathode composition, morphology, and microstructure, as well as the development of electrolyte formulations. In this review, we discuss the multiple failure mechanisms of Ni-rich cathodes in terms of two major aspects: structural degradation and gas release. We elucidate the key factors contributing to chemical, crystallographic, and microstructural degradation in Ni-rich cathodes, and summarize the various origins of gas evolution associated with these materials. Another key theme of this review is the modification of Ni-rich cathodes to address the practical hurdles that limit their use in long-range and high-safety EVs. Accordingly, we present a comprehensive overview of the latest Ni-rich cathode modification strategies for next-generation EV platforms.
{"title":"Addressing the fundamental issues in Ni-rich cathodes: degradation mechanisms and mitigation strategies","authors":"Ziqi Liu, Yiming Zhang, Shanshan Pan, Yong Chen, Keer Yang, Shanxi Wu, Musong Liu, Lei Hu, Shuaicheng Jiang, Xiaopeng Wang, Guoxiu Wang and Meng Yao","doi":"10.1039/D5EE04213E","DOIUrl":"10.1039/D5EE04213E","url":null,"abstract":"<p >The rapid growth of electric vehicles (EVs) is driving an urgent demand for lithium-ion batteries (LIBs) with higher specific energy, longer life, and uncompromised safety. Ni-rich layered oxides (LiNi<small><sub><em>x</em></sub></small>C<small><sub>o<em>y</em></sub></small>Mn<small><sub>(1−<em>x</em>−<em>y</em>)</sub></small>O<small><sub>2</sub></small>, <em>x</em> ≥ 0.8) have emerged as leading cathode materials for next-generation LIBs, owing to their high capacity and energy density. Further increasing Ni content is essential for improved performance and cost reduction. However, it also introduces new obstacles, necessitating thoughtful design of cathode composition, morphology, and microstructure, as well as the development of electrolyte formulations. In this review, we discuss the multiple failure mechanisms of Ni-rich cathodes in terms of two major aspects: structural degradation and gas release. We elucidate the key factors contributing to chemical, crystallographic, and microstructural degradation in Ni-rich cathodes, and summarize the various origins of gas evolution associated with these materials. Another key theme of this review is the modification of Ni-rich cathodes to address the practical hurdles that limit their use in long-range and high-safety EVs. Accordingly, we present a comprehensive overview of the latest Ni-rich cathode modification strategies for next-generation EV platforms.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 1","pages":" 84-125"},"PeriodicalIF":30.8,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145704846","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}
Ting Wang, Yuqi Zhou, Jiaqi Huang, Fangzhou Zhao, Wanglai Cen, Lanlu Lu, Yifei Dang, Kecheng Cao, Yan Meng, Yongzhi Zhang and Dan Xiao
Correction for ‘Ion exchange-induced LixMgyBOz coating synergized with reinforced bulk doping enables fast-charging long-cycling high-voltage LiCoO2’ by Ting Wang et al., Energy Environ. Sci., 2025, 18, 10444–10459, https://doi.org/10.1039/d5ee04240b.