Alan R Bowman,Qimu Yuan,Joshua R. S. Lilly,Adam T Wood,Vincent Jae-Yeon Lim,Michael B Johnston,Nakita K. Noel,Laura M Herz
Reliable predictions of long-term stability are essential as halide perovskite solar cells approach widespread commercial deployment. However, extrapolation from aging tests requires knowledge of material degradation dynamics, which remain unclear for halide perovskites. Here, we reveal the structural and optoelectronic evolution of formamidinium-caesium lead-halide perovskite films under heat and/or light using in-situ X-ray diffraction and photoluminescence. Heat and light combined induce much faster degradation than either stressor alone, with 1-sun illumination degrading material 53 times faster at 85°C than room temperature. For all compositions investigated the degradation rate is highly nonlinear in time and follows a sigmoidal decay, suggestive of interface-driven dynamics. Degradation proceeds in three steps: halide segregation (for mixed-halide perovskites), A-site cation diffusion triggered by heterogeneity and strain, and finally iodine and formamidinium loss. Our findings provide a quantitative framework for lifetime predictions and highlight the necessity of combined heat and light ageing tests.
{"title":"Degradation dynamics of lead-halide perovskites under combined heat and light","authors":"Alan R Bowman,Qimu Yuan,Joshua R. S. Lilly,Adam T Wood,Vincent Jae-Yeon Lim,Michael B Johnston,Nakita K. Noel,Laura M Herz","doi":"10.1039/d6ee04175b","DOIUrl":"https://doi.org/10.1039/d6ee04175b","url":null,"abstract":"Reliable predictions of long-term stability are essential as halide perovskite solar cells approach widespread commercial deployment. However, extrapolation from aging tests requires knowledge of material degradation dynamics, which remain unclear for halide perovskites. Here, we reveal the structural and optoelectronic evolution of formamidinium-caesium lead-halide perovskite films under heat and/or light using in-situ X-ray diffraction and photoluminescence. Heat and light combined induce much faster degradation than either stressor alone, with 1-sun illumination degrading material 53 times faster at 85°C than room temperature. For all compositions investigated the degradation rate is highly nonlinear in time and follows a sigmoidal decay, suggestive of interface-driven dynamics. Degradation proceeds in three steps: halide segregation (for mixed-halide perovskites), A-site cation diffusion triggered by heterogeneity and strain, and finally iodine and formamidinium loss. Our findings provide a quantitative framework for lifetime predictions and highlight the necessity of combined heat and light ageing tests.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"269 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980707","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}
Radiative cooling has been developed for two largely separate functions: passive thermal management and atmospheric water harvesting (AWH). Combining them on a single surface under an imposed heat load is intrinsically difficult, as hotspot cooling raises the emitter temperature, whereas condensation requires sustained sub-dew-point regions. Here we establish, to our knowledge, a previously unreported geometry-driven co-functional regime in which a localized hotspot is coupled to an extended planar or pyramidal radiative emitter. Lateral heat spreading creates a warm, dry zone near the hotspot while preserving cooler peripheral regions for dew formation, allowing the same passive platform to reject heat and harvest water simultaneously. We combine angle-resolved optical characterization, raytracing, coupled heat and mass transfer modelling, and outdoor experiments. At a hotspot heat flux of 1021 W m-2, the largest planar emitter and 45° pyramidal emitter retain dew fluxes of 9.3 and 7.9 g m-2 h-1, respectively, while lowering the near-hotspot temperature by more than 45 °C relative to a non-concentrated control. At 1500 W m-2, the same architectures keep the hotspot below 20 °C, whereas the control approaches 85 °C. Finally, an experiment-calibrated global assessment further identifies where this regime is climatically accessible. These results provide a general framework for the passive co-management of localized heat and atmospheric water.
辐射冷却已经发展为两个主要独立的功能：被动热管理和大气集水（AWH）。在强加的热负荷下，将它们结合在一个表面上本质上是困难的，因为热点冷却会提高发射器的温度，而冷凝需要持续的亚露点区域。在这里，我们建立，据我们所知，一个以前未报道的几何驱动的共功能制度，其中一个局部热点是耦合到一个扩展的平面或金字塔形辐射发射器。横向热扩散在热点附近创造了一个温暖干燥的区域，同时为露水形成保留了较冷的外围区域，允许同一个被动平台同时拒绝热量和收集水。我们结合了角度分辨光学表征、光线追踪、耦合传热传质建模和室外实验。在热点热流密度为1021 W m-2时，最大的平面发射极和45°锥体发射极分别保持了9.3 g m-2 h-1和7.9 g m-2 h-1的露水通量，而相对于非集中控制，近热点温度降低了45°C以上。在1500 W m-2时，相同的架构将热点保持在20°C以下，而控制则接近85°C。最后，一项实验校准的全球评估进一步确定了在气候条件下实现这一机制的地方。这些结果为局部热和大气水的被动协同管理提供了一个总体框架。
{"title":"From Flat to Structured: Geometry-Driven Dual-Mode Radiative Emitters for Simultaneous Hotspot Cooling and Water Harvesting","authors":"Primož Poredoš,Gerardo Silva-Oelker,Inigo González de Arrieta,Gabriel Alejandro López,Dejan Josif Trajkovski,Higgins Wilson,Abdallah Ali,Jiaxing Xu,Chenxi Wang,Tej Žižak,Eva Zavrl,Ciril Arkar,Sašo Medved,Suzana Domjan,Juliana Fernandez,Ruzhu Wang","doi":"10.1039/d6ee04674f","DOIUrl":"https://doi.org/10.1039/d6ee04674f","url":null,"abstract":"Radiative cooling has been developed for two largely separate functions: passive thermal management and atmospheric water harvesting (AWH). Combining them on a single surface under an imposed heat load is intrinsically difficult, as hotspot cooling raises the emitter temperature, whereas condensation requires sustained sub-dew-point regions. Here we establish, to our knowledge, a previously unreported geometry-driven co-functional regime in which a localized hotspot is coupled to an extended planar or pyramidal radiative emitter. Lateral heat spreading creates a warm, dry zone near the hotspot while preserving cooler peripheral regions for dew formation, allowing the same passive platform to reject heat and harvest water simultaneously. We combine angle-resolved optical characterization, raytracing, coupled heat and mass transfer modelling, and outdoor experiments. At a hotspot heat flux of 1021 W m-2, the largest planar emitter and 45° pyramidal emitter retain dew fluxes of 9.3 and 7.9 g m-2 h-1, respectively, while lowering the near-hotspot temperature by more than 45 °C relative to a non-concentrated control. At 1500 W m-2, the same architectures keep the hotspot below 20 °C, whereas the control approaches 85 °C. Finally, an experiment-calibrated global assessment further identifies where this regime is climatically accessible. These results provide a general framework for the passive co-management of localized heat and atmospheric water.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"111 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980702","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}
Hoang-Long Du,Duong T Truong,Karolina Matuszek,Ngoc-Trung Ngoc Nguyen,Rebecca Hodgetts,Khang Dinh,Th Vu,Shohreh M Khah,Peter Strasser,Douglas R. MacFarlane,Alexandr N Simonov,Uli Hintermair
Electrolyte engineering is an effective means to enhance the performance of electrochemical systems, including the lithium redox-mediated nitrogen reduction reaction (Li-NRR) – a process that might support future sustainable ammonia production. The current best Li-NRR performance requires elevated N2 pressures (PN2) ≥10 bar in model three-electrode cells, though practical electrolysers would benefit from operation at close to ambient PN2. To enable this, we designed an electrolyte containing a high concentration of trihexyltetradecylphosphonium bis(trifluoromethylsulfonyl)imide, [P6,6,6,14][NTf2], and used it for the Li-NRR mediated by LiNTf2 under flowing N2 at 1-2 bar. Under these conditions, the 1.5 LiNTf2 + 0.65 M [P6,6,6,14][NTf2] + 0.1 M ethanol combination produced NH3 at a faradaic efficiency of 90 ± 5% (0.05 cm2 electrode) and 83 ± 9% (1.2 cm2 electrode), contrasting ca 36% for the conventional [P6,6,6,14][NTf2]-free electrolyte. Our data suggest that high-concentration [P6,6,6,14][NTf2] inhibits side reactions and thereby improves the Li-NRR performance. Moreover, the hydrophobic nature of [P6,6,6,14]+ enabled stable Li-NRR when the cell was assembled in air and in the presence of water. This opens a pathway for the future integration of the Li-NRR with a water oxidising anode for sustainable ammonia production.
{"title":"High-selectivity nitrogen electroreduction to ammonia at near-ambient pressure","authors":"Hoang-Long Du,Duong T Truong,Karolina Matuszek,Ngoc-Trung Ngoc Nguyen,Rebecca Hodgetts,Khang Dinh,Th Vu,Shohreh M Khah,Peter Strasser,Douglas R. MacFarlane,Alexandr N Simonov,Uli Hintermair","doi":"10.1039/d6ee03717h","DOIUrl":"https://doi.org/10.1039/d6ee03717h","url":null,"abstract":"Electrolyte engineering is an effective means to enhance the performance of electrochemical systems, including the lithium redox-mediated nitrogen reduction reaction (Li-NRR) – a process that might support future sustainable ammonia production. The current best Li-NRR performance requires elevated N2 pressures (PN2) ≥10 bar in model three-electrode cells, though practical electrolysers would benefit from operation at close to ambient PN2. To enable this, we designed an electrolyte containing a high concentration of trihexyltetradecylphosphonium bis(trifluoromethylsulfonyl)imide, [P6,6,6,14][NTf2], and used it for the Li-NRR mediated by LiNTf2 under flowing N2 at 1-2 bar. Under these conditions, the 1.5 LiNTf2 + 0.65 M [P6,6,6,14][NTf2] + 0.1 M ethanol combination produced NH3 at a faradaic efficiency of 90 ± 5% (0.05 cm2 electrode) and 83 ± 9% (1.2 cm2 electrode), contrasting ca 36% for the conventional [P6,6,6,14][NTf2]-free electrolyte. Our data suggest that high-concentration [P6,6,6,14][NTf2] inhibits side reactions and thereby improves the Li-NRR performance. Moreover, the hydrophobic nature of [P6,6,6,14]+ enabled stable Li-NRR when the cell was assembled in air and in the presence of water. This opens a pathway for the future integration of the Li-NRR with a water oxidising anode for sustainable ammonia production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"152 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980703","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}
Intrinsically stretchable perovskite solar cells (IS-PSCs) are promising autonomous power sources for wearable electronics and aerospace platforms; however, their practical implementation is hindered by rapid performance degradation under mechanical strain. This failure stems largely from a pronounced Young's modulus (E) mismatch across multilayer stacks, which intensifies stress localization and triggers catastrophic, electrically disruptive cracking. Here, we report an E-gradient shear-lag design that stabilizes IS-PSCs by strategically converging the E values of both the substrate and perovskite layer toward the intermediate E of the PH1000/NiOx electrode region (4.70 GPa). This is achieved by stiffening the thermoplastic polyurethane (TPU) substrate through increased hard-segment fraction, increasing E from 199 to 1560 MPa, while softening the perovskite film via TPU additive engineering, reducing E from 19.2 to 8.39 GPa. This mechanically graded architecture suppresses strain localization and redistributes tensile stress, thereby preserving the continuity of carrier transport even under significant deformation. Consequently, the optimized IS-PSC achieves a power conversion efficiency of 22.14% (certified: 21.52%) and retains 80% of its initial performance at 60% tensile strain, demonstrating the efficacy of E-gradient engineering in overcoming the inherent brittleness of perovskite photovoltaics.
{"title":"Modulus-gradient shear-lag design for robust, high-efficiency intrinsically stretchable perovskite solar cells","authors":"Min-Ho Lee,Seo-Joon Hong,Seungbok Lee,Min Seok Kim,Hajun Lee,Myoung Song,Dohun Kim,Dong-Ha Kim,Taek-Soo Kim,Jiyun Kim,Jangwon Seo,Jung-Yong Lee","doi":"10.1039/d6ee03077g","DOIUrl":"https://doi.org/10.1039/d6ee03077g","url":null,"abstract":"Intrinsically stretchable perovskite solar cells (IS-PSCs) are promising autonomous power sources for wearable electronics and aerospace platforms; however, their practical implementation is hindered by rapid performance degradation under mechanical strain. This failure stems largely from a pronounced Young's modulus (E) mismatch across multilayer stacks, which intensifies stress localization and triggers catastrophic, electrically disruptive cracking. Here, we report an E-gradient shear-lag design that stabilizes IS-PSCs by strategically converging the E values of both the substrate and perovskite layer toward the intermediate E of the PH1000/NiOx electrode region (4.70 GPa). This is achieved by stiffening the thermoplastic polyurethane (TPU) substrate through increased hard-segment fraction, increasing E from 199 to 1560 MPa, while softening the perovskite film via TPU additive engineering, reducing E from 19.2 to 8.39 GPa. This mechanically graded architecture suppresses strain localization and redistributes tensile stress, thereby preserving the continuity of carrier transport even under significant deformation. Consequently, the optimized IS-PSC achieves a power conversion efficiency of 22.14% (certified: 21.52%) and retains 80% of its initial performance at 60% tensile strain, demonstrating the efficacy of E-gradient engineering in overcoming the inherent brittleness of perovskite photovoltaics.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"59 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148980708","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}
Yehui Zhang,Ziyang Song,Qi Huang,Yaokang Lv,Lihua Gan,Mingxian Liu
Polymers featuring inherent structural insolubility and customizable redox-active sites are booming as promising cathode materials for propelling aqueous iron-organic batteries (IOBs). However, their rotating single-bond linkers (e.g., β-ketoenamine) often lead to structural distortion with high redox barriers, hindering full utilization of active sites and thus unsatisfactory capacity. Here we propose a β-ketoenamine-bond confinement strategy to construct near-planar quinone polymer cathodes through integrating 2,4,6-triformylphloroglucinol with different diaminoanthraquinone isomers. Shifting the amino groups on diaminoanthraquinone unit from ortho to para-position mitigates repulsive interactions between neighboring carbonyl groups and polymeric β-ketoenamine linkers, suppressing structural distortion to yield a near-planar quinone skeleton (2,6-DT) with a dihedral angle of 178.4° (vs. 134.1°/160.1° for ortho-/meta-substituted 1,2‑DT/1,5‑DT). This feature enables low-energy-barrier redox reaction (0.14 eV) to promise full utilization (96.8%) of multielectron carbonyl groups in 2,6-DT (vs. 0.25 eV/68.5% of 1,2-DT and 0.19 eV/84.9% of 1,5-DT). Furthermore, the extended near-planar structure of 2,6-DT promotes robust intramolecular π-π stacking (5.93 eV vs. 4.63/5.28 eV for 1,2-DT/1,5-DT), conferring exceptional structural anti-dissolution in aqueous electrolytes. Consequently, 2,6-DT cathode harvests state-of-the-art capacity (313 mAh g−1) and cycling lifetime (80,000 cycles), placing it among the leading reported IOBs. Our findings provide new insights for designing near-planar polymer structures via single-bond-confined engineering towards better IOBs.
聚合物具有固有的结构不溶性和可定制的氧化还原活性位点，作为推进水铁有机电池（IOBs）的有前途的正极材料而蓬勃发展。然而，它们的旋转单键连接体（如β-酮胺）往往导致结构扭曲，具有高氧化还原障碍，阻碍了活性位点的充分利用，因此不能令人满意的容量。本文提出了一种β-酮胺键约束策略，通过将2,4,6-三甲酰间苯三酚与不同的二氨基蒽醌异构体结合，构建近平面醌聚合物阴极。将二氨基蒽醌单元上的氨基从邻位转移到对位，减轻了相邻羰基与聚合物β-酮胺连接物之间的排斥相互作用，抑制了结构扭曲，从而产生了二面角为178.4°的近平面醌骨架（2,6-DT）（邻位/元取代的1,2 -DT /1,5 -DT为134.1°/160.1°）。这一特性使得低能垒氧化还原反应（0.14 eV）能够保证2,6- dt中多电子羰基的充分利用（96.8%）（1,2- dt为0.25 eV/68.5%, 1,5- dt为0.19 eV/84.9%）。此外，2,6- dt的扩展近平面结构促进了分子内π-π堆积（5.93 eV vs. 4.63/5.28 eV 1,2- dt /1,5- dt），赋予了特殊的结构抗溶解水性电解质。因此，2,6- dt阴极获得了最先进的容量（313 mAh g−1）和循环寿命（80,000次循环），使其成为报道中领先的IOBs。我们的发现为通过单键约束工程设计近平面聚合物结构以获得更好的IOBs提供了新的见解。
{"title":"β-Ketoenamine-bond confinement enables near-planar quinone polymer cathodes for high-capacity and ultrastable iron-organic batteries","authors":"Yehui Zhang,Ziyang Song,Qi Huang,Yaokang Lv,Lihua Gan,Mingxian Liu","doi":"10.1039/d6ee04914a","DOIUrl":"https://doi.org/10.1039/d6ee04914a","url":null,"abstract":"Polymers featuring inherent structural insolubility and customizable redox-active sites are booming as promising cathode materials for propelling aqueous iron-organic batteries (IOBs). However, their rotating single-bond linkers (e.g., β-ketoenamine) often lead to structural distortion with high redox barriers, hindering full utilization of active sites and thus unsatisfactory capacity. Here we propose a β-ketoenamine-bond confinement strategy to construct near-planar quinone polymer cathodes through integrating 2,4,6-triformylphloroglucinol with different diaminoanthraquinone isomers. Shifting the amino groups on diaminoanthraquinone unit from ortho to para-position mitigates repulsive interactions between neighboring carbonyl groups and polymeric β-ketoenamine linkers, suppressing structural distortion to yield a near-planar quinone skeleton (2,6-DT) with a dihedral angle of 178.4° (vs. 134.1°/160.1° for ortho-/meta-substituted 1,2‑DT/1,5‑DT). This feature enables low-energy-barrier redox reaction (0.14 eV) to promise full utilization (96.8%) of multielectron carbonyl groups in 2,6-DT (vs. 0.25 eV/68.5% of 1,2-DT and 0.19 eV/84.9% of 1,5-DT). Furthermore, the extended near-planar structure of 2,6-DT promotes robust intramolecular π-π stacking (5.93 eV vs. 4.63/5.28 eV for 1,2-DT/1,5-DT), conferring exceptional structural anti-dissolution in aqueous electrolytes. Consequently, 2,6-DT cathode harvests state-of-the-art capacity (313 mAh g−1) and cycling lifetime (80,000 cycles), placing it among the leading reported IOBs. Our findings provide new insights for designing near-planar polymer structures via single-bond-confined engineering towards better IOBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"76 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973565","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}
Low-voltage operation of manganese-based spinel cathodes can access additional capacity but is typically limited by cooperative Jahn–Teller distortion, cubic-to-tetragonal phase evolution and rapid capacity decay. Stabilization strategies have therefore largely aimed to suppress this low-voltage phase transition. Here, using phosphorus-integrated Li1.67Mn1.5P0.17O4 (LMPO) and phosphorus-free Li1.86Mn1.67O4 (LMO) as a matched model pair, we show that the key to low-voltage reversibility is not preventing tetragonal phase formation, but controlling how the tetragonal phase evolves during cycling. LMPO retains 78.0% of its capacity after 100 cycles, whereas LMO retains only 26.0%, despite both materials forming a discharged tetragonal phase. Combined electrochemical analysis, multiscale structural characterization and first-principles calculations reveal that phosphorus narrows the extended 8a-to-16c two-phase regime and suppresses irreversible tetragonal-phase accumulation. More importantly, phosphorus disrupts the cooperative ordering of Jahn–Teller axes, attenuates MnO6 distortion and reduces the lattice/volume mismatch between cubic and tetragonal phases. These results identify the cooperative character of Jahn–Teller distortion as a critical design target for stabilizing low-voltage cycling in Mn-based spinel cathodes.
{"title":"Phosphorus-enabled reversible Jahn–Teller phase evolution in manganese spinel cathodes","authors":"Hyoi Jo,Hyojun Kim,Cheolwoo Jo,Sungsoo Kim,Byunghoon Kim,Sung-Kyun Jung","doi":"10.1039/d6ee04410g","DOIUrl":"https://doi.org/10.1039/d6ee04410g","url":null,"abstract":"Low-voltage operation of manganese-based spinel cathodes can access additional capacity but is typically limited by cooperative Jahn–Teller distortion, cubic-to-tetragonal phase evolution and rapid capacity decay. Stabilization strategies have therefore largely aimed to suppress this low-voltage phase transition. Here, using phosphorus-integrated Li1.67Mn1.5P0.17O4 (LMPO) and phosphorus-free Li1.86Mn1.67O4 (LMO) as a matched model pair, we show that the key to low-voltage reversibility is not preventing tetragonal phase formation, but controlling how the tetragonal phase evolves during cycling. LMPO retains 78.0% of its capacity after 100 cycles, whereas LMO retains only 26.0%, despite both materials forming a discharged tetragonal phase. Combined electrochemical analysis, multiscale structural characterization and first-principles calculations reveal that phosphorus narrows the extended 8a-to-16c two-phase regime and suppresses irreversible tetragonal-phase accumulation. More importantly, phosphorus disrupts the cooperative ordering of Jahn–Teller axes, attenuates MnO6 distortion and reduces the lattice/volume mismatch between cubic and tetragonal phases. These results identify the cooperative character of Jahn–Teller distortion as a critical design target for stabilizing low-voltage cycling in Mn-based spinel cathodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"21 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973571","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}
Jie Shi,Jiayue Tang,Hongting Du,Danni Wang,Yiming Zhao,Yuze Wang,Xunsi Wang,Jiaqiang Huang,Biao Zhang
The anode-free configuration holds great promise in breaking the energy limits of current sodium batteries by pairing with a high-voltage cathode. While glyme electrolytes have enabled stable 3 V-class anode-free sodium batteries (AFSBs), fast degradation has been observed when high-voltage cathodes are used, despite the electrolytes being well suited to such cathodes in half cells. Here, we decipher that the anode poisoning arising from the crossovers of oxidative products, which are non-threatening to the cathodes alone, is the main culprit. This discovery contests the common belief that intrinsic interface instability solely dominates the lifespan of AFSBs. As a mechanistic intervention, introducing 1,3-dioxane (DX) as a co-solvent shifts the oxidation pathway from diglyme towards DX-oriented, which suppresses the accumulation and crossover of the attacking species. Consequently, the optimized electrolyte realizes 80% capacity retention of 4 V-class AFSBs after 500 cycles at −20 °C. These results demonstrate that solvation regulation can reshape electrolyte decomposition pathways and reduce the generation of detrimental crossover species, providing a useful design principle for mitigating crosstalk-induced degradation in high-voltage AFSBs.
{"title":"Unraveling anomalous capacity degradation and its alleviation in high-voltage anode-free sodium batteries","authors":"Jie Shi,Jiayue Tang,Hongting Du,Danni Wang,Yiming Zhao,Yuze Wang,Xunsi Wang,Jiaqiang Huang,Biao Zhang","doi":"10.1039/d6ee02194h","DOIUrl":"https://doi.org/10.1039/d6ee02194h","url":null,"abstract":"The anode-free configuration holds great promise in breaking the energy limits of current sodium batteries by pairing with a high-voltage cathode. While glyme electrolytes have enabled stable 3 V-class anode-free sodium batteries (AFSBs), fast degradation has been observed when high-voltage cathodes are used, despite the electrolytes being well suited to such cathodes in half cells. Here, we decipher that the anode poisoning arising from the crossovers of oxidative products, which are non-threatening to the cathodes alone, is the main culprit. This discovery contests the common belief that intrinsic interface instability solely dominates the lifespan of AFSBs. As a mechanistic intervention, introducing 1,3-dioxane (DX) as a co-solvent shifts the oxidation pathway from diglyme towards DX-oriented, which suppresses the accumulation and crossover of the attacking species. Consequently, the optimized electrolyte realizes 80% capacity retention of 4 V-class AFSBs after 500 cycles at −20 °C. These results demonstrate that solvation regulation can reshape electrolyte decomposition pathways and reduce the generation of detrimental crossover species, providing a useful design principle for mitigating crosstalk-induced degradation in high-voltage AFSBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"394 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973584","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}
Shang Wen,Weiyi Xia,Yichen Zheng,Yunxia Mao,Hanyang Chen,Hui Wang,Dan Liu,Wei Li,Tao Wang
Printing optoelectronics has long been challenged by the complex flow field during film drying, where erratic solute migration readily hampers the molecular packing and film uniformity, leading to compromised power conversion efficiency and operational stability. In this work, two rheology thickeners, polar ethyl cellulose (EC)-a non-ionic surfactant with amphiphilic characteristics, and non-polar polyisobutylene (PIB) are incorporated in the photovoltaic ink to tune the film formation quality and dynamics. Through a range of rheological and morphological measurements, we find that EC acts as a surface-active agent, reducing surface tension and reversing the Marangoni flow to partially suppress the coffee-ring defects, yet it disrupts the donor/acceptor interactions and introduces directional stripes. In contrast, PIB grants the ink shear-thinning ability to facilitate the spreading of solution to form uniform wet films, whilst it also increases the static viscosity of the ink to kinetically suppress both capillary and Marangoni flows after printing, without altering the molecular packing of donor and acceptor. Consequently, PIB yields excellent uniformity across largearea PM6:BTP-eC9 films and delivers power conversion efficiencies (PCEs) over 19.0% and 18.3% in 100 and 300 -nm thick devices respectively, whilst maintaining the PCE of 17.6% for 1 cm 2 device, which are among the highest values for blade-coated binary OSCs. This work demonstrates that ink tuning employing the rheology thickener with shear-thinning character is a facile approach to prepare scalable and efficient printed organic solar cells.
长期以来，印刷光电子技术一直受到薄膜干燥过程中复杂流场的挑战，其中不稳定的溶质迁移容易阻碍分子包装和薄膜均匀性，导致功率转换效率和操作稳定性下降。在这项工作中，两种流变增稠剂，极性乙基纤维素(EC)-一种具有两亲性特征的非离子表面活性剂，和非极性聚异丁烯（PIB）加入光伏油墨中，以调节薄膜的形成质量和动力学。通过一系列流变学和形态学测量，我们发现EC作为表面活性剂，降低表面张力，逆转马兰戈尼流，部分抑制咖啡环缺陷，但它破坏了供体/受体的相互作用，并引入了定向条纹。相比之下，PIB赋予油墨剪切变薄的能力，以促进溶液的扩散，形成均匀的湿膜，同时它也增加了油墨的静态粘度，在印刷后动态抑制毛细管和马兰戈尼流动，而不改变供体和受体的分子包装。因此，PIB在大面积PM6:BTP-eC9薄膜上产生出色的均匀性，并在100和300纳米厚的器件中分别提供超过19.0%和18.3%的功率转换效率（PCE），同时在1 cm 2器件中保持17.6%的PCE，这是叶片涂层二元osc的最高值之一。这项工作表明，采用具有剪切减薄特性的流变增稠剂进行油墨调整是制备可扩展和高效印刷有机太阳能电池的简便方法。
{"title":"Ink tuning with rheology thickener for efficient and printed organic solar cells","authors":"Shang Wen,Weiyi Xia,Yichen Zheng,Yunxia Mao,Hanyang Chen,Hui Wang,Dan Liu,Wei Li,Tao Wang","doi":"10.1039/d6ee04808k","DOIUrl":"https://doi.org/10.1039/d6ee04808k","url":null,"abstract":"Printing optoelectronics has long been challenged by the complex flow field during film drying, where erratic solute migration readily hampers the molecular packing and film uniformity, leading to compromised power conversion efficiency and operational stability. In this work, two rheology thickeners, polar ethyl cellulose (EC)-a non-ionic surfactant with amphiphilic characteristics, and non-polar polyisobutylene (PIB) are incorporated in the photovoltaic ink to tune the film formation quality and dynamics. Through a range of rheological and morphological measurements, we find that EC acts as a surface-active agent, reducing surface tension and reversing the Marangoni flow to partially suppress the coffee-ring defects, yet it disrupts the donor/acceptor interactions and introduces directional stripes. In contrast, PIB grants the ink shear-thinning ability to facilitate the spreading of solution to form uniform wet films, whilst it also increases the static viscosity of the ink to kinetically suppress both capillary and Marangoni flows after printing, without altering the molecular packing of donor and acceptor. Consequently, PIB yields excellent uniformity across largearea PM6:BTP-eC9 films and delivers power conversion efficiencies (PCEs) over 19.0% and 18.3% in 100 and 300 -nm thick devices respectively, whilst maintaining the PCE of 17.6% for 1 cm 2 device, which are among the highest values for blade-coated binary OSCs. This work demonstrates that ink tuning employing the rheology thickener with shear-thinning character is a facile approach to prepare scalable and efficient printed organic solar cells.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973566","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}
Perovskite solar cells (PSCs) have reached power conversion efficiencies (PCEs) of 28%, but their scalable manufacturing remains hindered by the use of hazardous solvents and inert-atmosphere processing. Green-solvent air-processing is a promising route towards sustainable perovskite photovoltaics, yet its efficiency remains limited by an unresolved chemical bottleneck. Here we report that air-processing disrupts solvent–lead coordination in the precursor state, leading to intermediate-phase heterogeneity, defect formation, and non-uniform crystallization in dimethyl sulfoxide (DMSO)-based systems. We resolve this challenge by introducing a coordination-reconfiguration strategy in a green DMSO/isopropanol (IPA) solvent system using iodo-binaphthyl-sulfonimide (IBS) as a coordination-reconfiguring agent. Ab initio calculations and experimental results indicate that IBS preferentially binds PbI2, weakens the DMSO–PbI2 interaction, and reconfigures the precursor coordination environment, thereby suppressing air-disrupted solvated intermediates and enabling homogeneous crystallization of phase-pure perovskite films. The p–i–n PSCs processed from this system achieve PCEs of 26.51% in N2 and 26.20% in air, outperforming air-processed DMF/DMSO controls, while 13.3 cm2 mini-modules deliver 23.20% PCE with strong operational and damp-heat stability.
{"title":"Reconfiguring solvent–lead coordination enables green-solvent air-processing of high-efficiency and scalable perovskite photovoltaics","authors":"Chunlei Zhang,Liangchen Qian,Qi Liu,Xintong Li,Ning Wang,Francesco Vanin,Zexin Yu,Yan Wang,Dong Zhang,Shuai Li,Jianqiu Gong,Danpeng Gao,Zhe Wang,Bo Li,Yen-Hung Lin,Chunyi Zhi,Martin Stolterfoht,Nan Li,Xiao Cheng Zeng,Zonglong Zhu","doi":"10.1039/d6ee04136a","DOIUrl":"https://doi.org/10.1039/d6ee04136a","url":null,"abstract":"Perovskite solar cells (PSCs) have reached power conversion efficiencies (PCEs) of 28%, but their scalable manufacturing remains hindered by the use of hazardous solvents and inert-atmosphere processing. Green-solvent air-processing is a promising route towards sustainable perovskite photovoltaics, yet its efficiency remains limited by an unresolved chemical bottleneck. Here we report that air-processing disrupts solvent–lead coordination in the precursor state, leading to intermediate-phase heterogeneity, defect formation, and non-uniform crystallization in dimethyl sulfoxide (DMSO)-based systems. We resolve this challenge by introducing a coordination-reconfiguration strategy in a green DMSO/isopropanol (IPA) solvent system using iodo-binaphthyl-sulfonimide (IBS) as a coordination-reconfiguring agent. Ab initio calculations and experimental results indicate that IBS preferentially binds PbI2, weakens the DMSO–PbI2 interaction, and reconfigures the precursor coordination environment, thereby suppressing air-disrupted solvated intermediates and enabling homogeneous crystallization of phase-pure perovskite films. The p–i–n PSCs processed from this system achieve PCEs of 26.51% in N2 and 26.20% in air, outperforming air-processed DMF/DMSO controls, while 13.3 cm2 mini-modules deliver 23.20% PCE with strong operational and damp-heat stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973567","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}
Early prediction of battery cycle life is essential for improving battery design, manufacturing and deployment. However, despite encouraging progress with machine learning, battery life prediction remains constrained by scarce data and pronounced heterogeneity across battery chemistries, specifications, formation protocols and operating conditions. Although transfer learning has been widely explored to alleviate these challenges, its effectiveness is limited by the absence of a foundation model that can integrate heterogeneous battery life data and provide broadly useful knowledge for target-scenario specialization. Here we introduce the pretrained battery transformer (PBT), an integrated foundation model comprising a general PBT and specialized PBT models for individual target scenarios. At its core, battery-knowledge-encoded mixture-of-experts layers enable the general PBT to consolidate shared cycling-pattern–lifetime relationships from 13 heterogeneous lithium-ion battery datasets while preserving specialization across distinct aging regimes. The resulting general PBT provides a shared knowledge and parameter foundation from which specialized PBT models are constructed using limited labelled data to capture target-specific degradation behavior. Across 15 downstream datasets covering 977 batteries and 532 aging conditions from lithium-ion, sodium-ion and zinc-ion batteries, the specialized PBT models achieve state-of-the-art performance, outperforming the strongest comparator by 24.8% on average and by up to 73.9%. This study establishes, to our knowledge, the first foundation model for battery life prediction and points towards a shift from isolated, scenario-specific modelling to a reusable knowledge foundation for data-efficient specialization, with broader implications for sustainable-energy prediction problems constrained by scarce and heterogeneous data.
{"title":"Pretrained battery transformer (PBT): A foundation model for battery life prediction","authors":"Ruifeng Tan,Weixiang Hong,Jia Li,Jiaqiang Huang,Tongyi Zhang","doi":"10.1039/d6ee03446b","DOIUrl":"https://doi.org/10.1039/d6ee03446b","url":null,"abstract":"Early prediction of battery cycle life is essential for improving battery design, manufacturing and deployment. However, despite encouraging progress with machine learning, battery life prediction remains constrained by scarce data and pronounced heterogeneity across battery chemistries, specifications, formation protocols and operating conditions. Although transfer learning has been widely explored to alleviate these challenges, its effectiveness is limited by the absence of a foundation model that can integrate heterogeneous battery life data and provide broadly useful knowledge for target-scenario specialization. Here we introduce the pretrained battery transformer (PBT), an integrated foundation model comprising a general PBT and specialized PBT models for individual target scenarios. At its core, battery-knowledge-encoded mixture-of-experts layers enable the general PBT to consolidate shared cycling-pattern–lifetime relationships from 13 heterogeneous lithium-ion battery datasets while preserving specialization across distinct aging regimes. The resulting general PBT provides a shared knowledge and parameter foundation from which specialized PBT models are constructed using limited labelled data to capture target-specific degradation behavior. Across 15 downstream datasets covering 977 batteries and 532 aging conditions from lithium-ion, sodium-ion and zinc-ion batteries, the specialized PBT models achieve state-of-the-art performance, outperforming the strongest comparator by 24.8% on average and by up to 73.9%. This study establishes, to our knowledge, the first foundation model for battery life prediction and points towards a shift from isolated, scenario-specific modelling to a reusable knowledge foundation for data-efficient specialization, with broader implications for sustainable-energy prediction problems constrained by scarce and heterogeneous data.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"5 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148964447","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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