Solar-powered water electrolysis holds significant promise for the mass production of green hydrogen. However, the substantial water consumption associated with electrolysis not only increases the cost of green hydrogen but also raises critical concerns about accelerating water scarcity. Although seawater can be an infinite water supply for green hydrogen production, its complex composition poses substantial challenges to efficient and reliable electrolysis. Here, we demonstrate a high-efficiency solar-powered green hydrogen production from seawater. Our approach takes advantage of the full-spectrum utilization of solar energy. Photovoltaic electricity is used to drive the electrolysis whereas the waste heat from solar cells is harnessed to produce clean water through the seawater distillation. With natural sunlight and real seawater as the sole inputs, we experimentally demonstrate 12.6% solar-to-hydrogen efficiency and 35.9 L/m2/h production rate of green hydrogen under one-sun illumination, where additional 1.2 L/m2/h clean water is obtained as a byproduct. By reducing reliance on clean water and electricity supplies, this work provides a fully sustainable strategy to access green hydrogen with favorable energy efficiency and technoeconomic feasibility.
{"title":"Over 12% efficiency solar-powered green hydrogen production from seawater","authors":"Xuanjie Wang, Jintong Gao, Yipu Wang, Yayuan Liu, Xinyue Liu, Lenan Zhang","doi":"10.1039/d4ee06203e","DOIUrl":"https://doi.org/10.1039/d4ee06203e","url":null,"abstract":"Solar-powered water electrolysis holds significant promise for the mass production of green hydrogen. However, the substantial water consumption associated with electrolysis not only increases the cost of green hydrogen but also raises critical concerns about accelerating water scarcity. Although seawater can be an infinite water supply for green hydrogen production, its complex composition poses substantial challenges to efficient and reliable electrolysis. Here, we demonstrate a high-efficiency solar-powered green hydrogen production from seawater. Our approach takes advantage of the full-spectrum utilization of solar energy. Photovoltaic electricity is used to drive the electrolysis whereas the waste heat from solar cells is harnessed to produce clean water through the seawater distillation. With natural sunlight and real seawater as the sole inputs, we experimentally demonstrate 12.6% solar-to-hydrogen efficiency and 35.9 L/m2/h production rate of green hydrogen under one-sun illumination, where additional 1.2 L/m2/h clean water is obtained as a byproduct. By reducing reliance on clean water and electricity supplies, this work provides a fully sustainable strategy to access green hydrogen with favorable energy efficiency and technoeconomic feasibility.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"93 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703316","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}
Qinrui Ye, Wei Song, Yong Bai, Zhenyu Chen, Pengfei Ding, Jinfeng Ge, Yuanyuan Meng, Bin Han, Xin Zhou, Ziyi Ge
Achieving a balance between power conversion efficiency (PCE) and mechanical robustness in flexible organic solar cells (OSCs) remains a significant challenge for small molecule acceptors (SMA) and polymer acceptors. Here, we developed a series of flexible linker giant-molecule acceptors (GMAs), DSY-C4 to DSY-C10, by incorporating flexible linkers of varying lengths at side chain sites. The optimized DSY-C10-based device demonstrated both high efficiency (PCE=18.89%) and exceptional mechanical resilience (crack-onset strain (COS)=9.95%) in binary OSCs, representing a new benchmark for highly ductile acceptors. The linkage at side chain sites makes the molecules exhibit butterfly-like conformation and the flexible linker reduces spatial site resistance, significantly improving GMA crystallinity and aggregation. As a result, PM6:DSY-C10-based device exhibits superior short-circuit current density (JSC=27.51 mA cm-2) and fill factor (FF=0.785) over PM6:DSY-C4-based device (JSC=26.65 mA cm-2 and FF=0.728). Additionally, the longer flexible linker enhanced donor-acceptor interactions, leading to a 65% higher COS forPM6:DSY-C10 blend film compared to PM6:DSY-C4 (COS=6.04%), approaching the performance of polymer acceptor (PT-IY). In addition, the incorporation of DSY-C10 in the PM6:BTP-eC9 binary blend achieved a efficiency of 19.91% (certified 19.39%), underscoring the potential of flexible linker GMAs for high-efficiency flexible OSCs.. These results demonstrate that flexible linker GMAs provide an unprecedented balance of PCE and mechanical robustness in binary OSCs, paving the way for durable flexible OSCs.
{"title":"Butterfly-effect of Flexible Linker in Giant-molecule Acceptor: Optimized Crystallization and Aggregation for Enhancing Mechanical Durability and Approaching 19% Efficiency in Binary Organic Solar Cells","authors":"Qinrui Ye, Wei Song, Yong Bai, Zhenyu Chen, Pengfei Ding, Jinfeng Ge, Yuanyuan Meng, Bin Han, Xin Zhou, Ziyi Ge","doi":"10.1039/d4ee05456c","DOIUrl":"https://doi.org/10.1039/d4ee05456c","url":null,"abstract":"Achieving a balance between power conversion efficiency (PCE) and mechanical robustness in flexible organic solar cells (OSCs) remains a significant challenge for small molecule acceptors (SMA) and polymer acceptors. Here, we developed a series of flexible linker giant-molecule acceptors (GMAs), DSY-C4 to DSY-C10, by incorporating flexible linkers of varying lengths at side chain sites. The optimized DSY-C10-based device demonstrated both high efficiency (PCE=18.89%) and exceptional mechanical resilience (crack-onset strain (COS)=9.95%) in binary OSCs, representing a new benchmark for highly ductile acceptors. The linkage at side chain sites makes the molecules exhibit butterfly-like conformation and the flexible linker reduces spatial site resistance, significantly improving GMA crystallinity and aggregation. As a result, PM6:DSY-C10-based device exhibits superior short-circuit current density (JSC=27.51 mA cm-2) and fill factor (FF=0.785) over PM6:DSY-C4-based device (JSC=26.65 mA cm-2 and FF=0.728). Additionally, the longer flexible linker enhanced donor-acceptor interactions, leading to a 65% higher COS forPM6:DSY-C10 blend film compared to PM6:DSY-C4 (COS=6.04%), approaching the performance of polymer acceptor (PT-IY). In addition, the incorporation of DSY-C10 in the PM6:BTP-eC9 binary blend achieved a efficiency of 19.91% (certified 19.39%), underscoring the potential of flexible linker GMAs for high-efficiency flexible OSCs.. These results demonstrate that flexible linker GMAs provide an unprecedented balance of PCE and mechanical robustness in binary OSCs, paving the way for durable flexible OSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"9 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695831","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}
Zewei Zhu, Bingcan Ke, Kexuan Sun, Chengkai Jing, Zhenhua Song, Ruixuan Jiang, Jing Li, Song Kong, Chang Liu, Sai Bai, Sisi He, Ziyi Ge, Fuzhi Huang, Yi-Bing Cheng, Tongle Bu
The passivation of undesirable defects in the perovskite light-absorption layer is an essential and effective strategy for improving the performance of perovskite solar cells (PSCs). Herein, a novel additive, 5-Aminothiazole hydrochloride (5ATCl) possessing both electron-accepting (NH3+) and electron-donating (C=N) functional groups, is introduced into the perovskite precursor ink, enabling holistic improvements of perovskite thin-film quality and photovoltaic performance. Comprehensive theoretical calculations and experimental characterizations reveal strong hydrogen bonds and intermolecular coordination between 5ATCl with the perovskite components. Consequently, the perovskite films demonstrate increased grain size and improved film quality, along with a released residual stress and a reduced defect density. Furthermore, the 5ATCl contributes to a favorable energy level alignment, thus promoting charge transfer and minimizing open-circuit voltage loss of the resulting devices. Notably, the champion power conversion efficiencies (PCEs) of rigid and flexible PSCs with the incorporation of 5ATCl reach 26.38% (certified 25.87%) and 24.54%, respectively. The stability of devices is also enhanced, demonstrating a T90 lifetime of 850 hours under continuous light illumination at maximum power point tracking. Additionally, centimeter-sized PSCs and 5 cm × 5 cm solar mini-modules also demonstrate impressive PCEs of 24.86% and 21.72% respectively, indicating the great feasibility of our strategy in up-scaling device fabrication.
{"title":"High-performance inverted perovskite solar cells and modules via aminothiazole passivation","authors":"Zewei Zhu, Bingcan Ke, Kexuan Sun, Chengkai Jing, Zhenhua Song, Ruixuan Jiang, Jing Li, Song Kong, Chang Liu, Sai Bai, Sisi He, Ziyi Ge, Fuzhi Huang, Yi-Bing Cheng, Tongle Bu","doi":"10.1039/d5ee01083g","DOIUrl":"https://doi.org/10.1039/d5ee01083g","url":null,"abstract":"The passivation of undesirable defects in the perovskite light-absorption layer is an essential and effective strategy for improving the performance of perovskite solar cells (PSCs). Herein, a novel additive, 5-Aminothiazole hydrochloride (5ATCl) possessing both electron-accepting (NH3+) and electron-donating (C=N) functional groups, is introduced into the perovskite precursor ink, enabling holistic improvements of perovskite thin-film quality and photovoltaic performance. Comprehensive theoretical calculations and experimental characterizations reveal strong hydrogen bonds and intermolecular coordination between 5ATCl with the perovskite components. Consequently, the perovskite films demonstrate increased grain size and improved film quality, along with a released residual stress and a reduced defect density. Furthermore, the 5ATCl contributes to a favorable energy level alignment, thus promoting charge transfer and minimizing open-circuit voltage loss of the resulting devices. Notably, the champion power conversion efficiencies (PCEs) of rigid and flexible PSCs with the incorporation of 5ATCl reach 26.38% (certified 25.87%) and 24.54%, respectively. The stability of devices is also enhanced, demonstrating a T90 lifetime of 850 hours under continuous light illumination at maximum power point tracking. Additionally, centimeter-sized PSCs and 5 cm × 5 cm solar mini-modules also demonstrate impressive PCEs of 24.86% and 21.72% respectively, indicating the great feasibility of our strategy in up-scaling device fabrication.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"71 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695832","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}
Zhengyan Lun, Alice Jane Merryweather, Amoghavarsha Mahadevegowda, Shrinidhi S. Pandurangi, Chao Xu, Simon M Fairclough, V. S. Deshpande, Norman Fleck, Caterina Ducati, Christoph Schnedermann, Akshay Rao, Clare P. Grey
Extensive worldwide efforts have been made to understand the degradation behavior of layered Ni-rich LiNixMnyCo(1−x−y)O2 (NMC) cathodes. The majority of studies carried out to date have focused on thermodynamic perspectives and are conducted ex situ; operando investigations on aged materials, especially those that can resolve dynamic information in a single-particle level remain sparse, preventing the development of long-term stable NMCs. Here, we directly visualize the real-time Li-ion transport kinetics of aged Ni-rich single-crystal NMC under operando conditions and at single-particle level using a recently developed optical microscopy technique. For both fresh and aged particles, we identify Li-ion concentration gradients developing during the early stages of delithiation – resulting in a Li-rich core and Li-poor surface – as observed previously and attributed to low Li-ion diffusivity at high Li-occupancies. Critically, in contrast to fresh particles, the Li-ion gradients in aged particles become markedly asymmetric, with the Li-rich core shifted away from the center of mass of the particle. Using ex situ transmission electron microscopy, we show that cell aging produces an uneven build-up of a surface rocksalt layer. Supported by finite-element modelling, we attribute the asymmetric delithiation behavior of the aged particles to this uneven rocksalt layer, which impedes the Li-ion flux heterogeneously at the particle surface. Our results demonstrate a new mechanism that contributes to the capacity and rate degradation of Ni-rich cathodes, highlighting the importance of controlling the build-up of detrimental interfacial layers in cathodes and providing a rational for improving the long-term stability and rate capabilities of Ni-rich NMC cathodes.
{"title":"Operando single-particle imaging reveals that asymmetric ion flux contributes to capacity degradation in aged Ni-rich layered cathodes","authors":"Zhengyan Lun, Alice Jane Merryweather, Amoghavarsha Mahadevegowda, Shrinidhi S. Pandurangi, Chao Xu, Simon M Fairclough, V. S. Deshpande, Norman Fleck, Caterina Ducati, Christoph Schnedermann, Akshay Rao, Clare P. Grey","doi":"10.1039/d5ee00267b","DOIUrl":"https://doi.org/10.1039/d5ee00267b","url":null,"abstract":"Extensive worldwide efforts have been made to understand the degradation behavior of layered Ni-rich LiNixMnyCo(1−x−y)O2 (NMC) cathodes. The majority of studies carried out to date have focused on thermodynamic perspectives and are conducted ex situ; operando investigations on aged materials, especially those that can resolve dynamic information in a single-particle level remain sparse, preventing the development of long-term stable NMCs. Here, we directly visualize the real-time Li-ion transport kinetics of aged Ni-rich single-crystal NMC under operando conditions and at single-particle level using a recently developed optical microscopy technique. For both fresh and aged particles, we identify Li-ion concentration gradients developing during the early stages of delithiation – resulting in a Li-rich core and Li-poor surface – as observed previously and attributed to low Li-ion diffusivity at high Li-occupancies. Critically, in contrast to fresh particles, the Li-ion gradients in aged particles become markedly asymmetric, with the Li-rich core shifted away from the center of mass of the particle. Using ex situ transmission electron microscopy, we show that cell aging produces an uneven build-up of a surface rocksalt layer. Supported by finite-element modelling, we attribute the asymmetric delithiation behavior of the aged particles to this uneven rocksalt layer, which impedes the Li-ion flux heterogeneously at the particle surface. Our results demonstrate a new mechanism that contributes to the capacity and rate degradation of Ni-rich cathodes, highlighting the importance of controlling the build-up of detrimental interfacial layers in cathodes and providing a rational for improving the long-term stability and rate capabilities of Ni-rich NMC cathodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"10 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677601","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}
Shengyao Luo, Mengqi Wu, Said Amzil, Tonghui Xu, Qing Ming, Lei Zhang, Jie Gao, Shuang Tian, Yisen Qian, Donghai Wang, Yajun Cheng, Yonggao Xia
The combination of high-nickel cathodes with lithium metal anodes is widely considered a promising solution to alleviate range anxiety. Alternatively, challenges such as limited fast-charging capacity and rapid degradation persist when using carbonate-based electrolytes. While many researchers predominantly focus on solvation structures, we have strategically tailored the electrolyte formulation by employing isopropyl acetate as the primary solvent, informed by interfacial interactions. Compared to n-propyl acetate, isopropyl acetate reduced the interaction with the electrode surface, promoted tighter adsorption of the electrolyte ion network within the inner Helmholtz layer, and ultimately enhanced the dynamic stability of the lithium metal interface. In Li||NCM811 cells, this electrolyte demonstrates a 4.5 V cutoff and sustains 88.6% capacity retention over 200 cycles at a high rate of 15 C. Additionally, this electrolyte demonstrates stable cycling performance at elevated rates of 1 C and 5 C at temperatures of 60 °C and -20 °C respectively, while maintaining stability even at a rate of 10 C under poor electrolyte conditions with thin lithium layers-indicating significant application potential. These studies reveal that the electrolyte distribution at the electrode interface affects the electrochemical process and the formation of the electrode-electrolyte interphase significantly, offering new ideas for future electrolyte research and design.
{"title":"Small modification, Striking Improvement: Super-Fast Charging Over a Wide Temperature Range by Simply Replacing n-propyl Acetate with Isopropyl Acetate","authors":"Shengyao Luo, Mengqi Wu, Said Amzil, Tonghui Xu, Qing Ming, Lei Zhang, Jie Gao, Shuang Tian, Yisen Qian, Donghai Wang, Yajun Cheng, Yonggao Xia","doi":"10.1039/d4ee05789a","DOIUrl":"https://doi.org/10.1039/d4ee05789a","url":null,"abstract":"The combination of high-nickel cathodes with lithium metal anodes is widely considered a promising solution to alleviate range anxiety. Alternatively, challenges such as limited fast-charging capacity and rapid degradation persist when using carbonate-based electrolytes. While many researchers predominantly focus on solvation structures, we have strategically tailored the electrolyte formulation by employing isopropyl acetate as the primary solvent, informed by interfacial interactions. Compared to n-propyl acetate, isopropyl acetate reduced the interaction with the electrode surface, promoted tighter adsorption of the electrolyte ion network within the inner Helmholtz layer, and ultimately enhanced the dynamic stability of the lithium metal interface. In Li||NCM811 cells, this electrolyte demonstrates a 4.5 V cutoff and sustains 88.6% capacity retention over 200 cycles at a high rate of 15 C. Additionally, this electrolyte demonstrates stable cycling performance at elevated rates of 1 C and 5 C at temperatures of 60 °C and -20 °C respectively, while maintaining stability even at a rate of 10 C under poor electrolyte conditions with thin lithium layers-indicating significant application potential. These studies reveal that the electrolyte distribution at the electrode interface affects the electrochemical process and the formation of the electrode-electrolyte interphase significantly, offering new ideas for future electrolyte research and design.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"24 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677889","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}
Polythiophenes are the most promising electron donors for organic solar cells (OSCs) in large-scale manufacturing due to their simple chemical structures and low production cost. However, the efficiency of polythiophene solar cells is largely limited by the difficulty in morphology optimization. Herein, we report the construction of refined fibril network structure in polythiophene:non-fullerene acceptor blends based on Classical Nucleation Theory. By screening solvents for polythiophene to obtain appropriate nucleation driving force while ensuring that the non-fullerene acceptor does not over-crystallize, a refined crystalline fibril network morphology in the blend consisting of a structurally simple polythiophene P5TCN-HD and non-fullerene acceptor was obtained. This optimal morphology improves exciton dissociation and charge transport, thereby endowed the solar cells with an unprecedented power conversion efficiency of 18.12% and a fill factor of 79.17%, marking new breakthroughs for polythiophene-based OSCs. Importantly, these successes were achieved from toluene, a common non-halogenated and environmental benign solvent. Moreover, we revealed the crucial impact of solvent quality on the formation of fibril network structure, offering valuable insights for optimizing the morphology of polythiophene systems. This underscores the promising prospect of polythiophenes in developing high-efficiency yet low-cost OSCs via environmental benign processing, which will drive the industrialization of OSCs.
{"title":"Nucleation driving force-controlled fibril network formation enables polythiophene solar cells with exceeding 18% efficiency from non-halogenated solvent","authors":"Jianglong Li, Dongsheng Xie, Xiyue Yuan, Youle Li, Wenkui Wei, Yue Zhang, Haozhe Feng, Xiang Luo, Jiayuan Zhu, Zhao Qin, Jianbin Zhong, lifu zhang, Hongxiang Li, Wei Zhang, Yong Zhang, Fei Huang, Yong Cao, Chunhui Duan","doi":"10.1039/d4ee06158f","DOIUrl":"https://doi.org/10.1039/d4ee06158f","url":null,"abstract":"Polythiophenes are the most promising electron donors for organic solar cells (OSCs) in large-scale manufacturing due to their simple chemical structures and low production cost. However, the efficiency of polythiophene solar cells is largely limited by the difficulty in morphology optimization. Herein, we report the construction of refined fibril network structure in polythiophene:non-fullerene acceptor blends based on Classical Nucleation Theory. By screening solvents for polythiophene to obtain appropriate nucleation driving force while ensuring that the non-fullerene acceptor does not over-crystallize, a refined crystalline fibril network morphology in the blend consisting of a structurally simple polythiophene P5TCN-HD and non-fullerene acceptor was obtained. This optimal morphology improves exciton dissociation and charge transport, thereby endowed the solar cells with an unprecedented power conversion efficiency of 18.12% and a fill factor of 79.17%, marking new breakthroughs for polythiophene-based OSCs. Importantly, these successes were achieved from toluene, a common non-halogenated and environmental benign solvent. Moreover, we revealed the crucial impact of solvent quality on the formation of fibril network structure, offering valuable insights for optimizing the morphology of polythiophene systems. This underscores the promising prospect of polythiophenes in developing high-efficiency yet low-cost OSCs via environmental benign processing, which will drive the industrialization of OSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"26 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677888","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}
Inverted inorganic perovskite solar cells (PSCs) are ideal top cells for tandem configurations due to their ideal bandgap and excellent thermal stability. However, water-induced rapid crystallization during inorganic perovskite film processing in ambient air is difficult to control. Here, we report a crystallization retardation method to prepare inorganic perovskite film by incorporating acrylonitrile-methyl acrylate copolymer (AMAC) in perovskite precursor solution. Firstly, the strong interaction between AMAC and the precursor solution yields increased colloidal size, delays dimethyl sulfoxide (DMSO) volatilization during annealing and postpones the phase transition. Secondly, the interaction between AMAC and dimethylamine (DMA+) slows down the ion exchange with Cs+. These interactions retard perovskite crystallization, increase pack-crystal grain size and reduce residual stress. Combined with the functional groups in AMAC, the incorporation of AMAC reduces defects in perovskite films, modulates interfacial energy levels, prolongs charge lifetimes, and inhibiting the migration of iodide ions. Ultimately, the power conversion efficiency (PCE) of the AMAC-incorporated inverted (p-i-n) and conventional (n-i-p) PSCs reach 21.7% and 21.8%, respectively, while the unencapsulated devices show only 8% degradation over 2500 h of maximum power point tracking and continuous operation.
{"title":"Comprehensive crystallization retardation of inorganic perovskite for high performance inverted solar cells","authors":"Zezhang Wang, Tianfei Xu, Nan Li, Zhen Chang, Jing Shan, Yong Wang, Minfang Wu, Fengwei Xiao, Shengzhong Frank Liu, Wanchun Xiang","doi":"10.1039/d5ee00149h","DOIUrl":"https://doi.org/10.1039/d5ee00149h","url":null,"abstract":"Inverted inorganic perovskite solar cells (PSCs) are ideal top cells for tandem configurations due to their ideal bandgap and excellent thermal stability. However, water-induced rapid crystallization during inorganic perovskite film processing in ambient air is difficult to control. Here, we report a crystallization retardation method to prepare inorganic perovskite film by incorporating acrylonitrile-methyl acrylate copolymer (AMAC) in perovskite precursor solution. Firstly, the strong interaction between AMAC and the precursor solution yields increased colloidal size, delays dimethyl sulfoxide (DMSO) volatilization during annealing and postpones the phase transition. Secondly, the interaction between AMAC and dimethylamine (DMA+) slows down the ion exchange with Cs+. These interactions retard perovskite crystallization, increase pack-crystal grain size and reduce residual stress. Combined with the functional groups in AMAC, the incorporation of AMAC reduces defects in perovskite films, modulates interfacial energy levels, prolongs charge lifetimes, and inhibiting the migration of iodide ions. Ultimately, the power conversion efficiency (PCE) of the AMAC-incorporated inverted (p-i-n) and conventional (n-i-p) PSCs reach 21.7% and 21.8%, respectively, while the unencapsulated devices show only 8% degradation over 2500 h of maximum power point tracking and continuous operation.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"183 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666611","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}
Junpeng Sun, Jialong Shen, Huadong Qi, Mei Sun, Yuhang Lou, Yu Yao, Xianhong Rui, Yu Shao, Xiaojun Wu, Hai Yang, Yan Yu
Lithium-rich manganese-based oxides (LRMO) are a promising next-generation candidate cathode material, offering a high discharge capacity exceeding 300 mAh g−1. This exceptional capacity is attributed to the synergistic redox activity of transition metals and lattice oxygen. Nevertheless, the over-oxidation of lattice oxygen in LRMO leads to capacity fading, severe lattice strain, and sluggish oxygen redox reaction kinetics. Herein, we introduce a lithium-deficient layer and a RuO2-promoted interface-confined catalysis network on the surface of LRMO (Ru-1). The lithium-deficient layer effectively passivates the surface lattice oxygen by reducing the Li-O-Li configurations at the atomic level. The RuO2-promoted interface-confined catalysis network successfully captures trace amounts of lost lattice oxygen and catalyzes the reversible reduction of activated O species. This configuration yields a specific discharge capacity of 307 mAh g−1 at 0.1 C, with an impressive capacity retention rate of 97% after 300 cycles at 1 C. The Ru-1||graphite pouch cell exhibits a superior capacity retention rate of 85% after 450 cycles at C/3 and the Ru-1||Li pouch cell exhibits a high energy density of 513 Wh kg−1. Our strategies involving the lithium-deficient layer and interface-confined catalysis offer novel insights into protecting the surface and enhancing oxygen reusability within the LRMO.
{"title":"Incorporating Lithium-Deficient Layer and Interfacial-Confined Catalysis Enables the Reversible Redox of Surface Oxygen Species in Lithium-Rich Manganese-based Oxides","authors":"Junpeng Sun, Jialong Shen, Huadong Qi, Mei Sun, Yuhang Lou, Yu Yao, Xianhong Rui, Yu Shao, Xiaojun Wu, Hai Yang, Yan Yu","doi":"10.1039/d5ee00430f","DOIUrl":"https://doi.org/10.1039/d5ee00430f","url":null,"abstract":"Lithium-rich manganese-based oxides (LRMO) are a promising next-generation candidate cathode material, offering a high discharge capacity exceeding 300 mAh g−1. This exceptional capacity is attributed to the synergistic redox activity of transition metals and lattice oxygen. Nevertheless, the over-oxidation of lattice oxygen in LRMO leads to capacity fading, severe lattice strain, and sluggish oxygen redox reaction kinetics. Herein, we introduce a lithium-deficient layer and a RuO2-promoted interface-confined catalysis network on the surface of LRMO (Ru-1). The lithium-deficient layer effectively passivates the surface lattice oxygen by reducing the Li-O-Li configurations at the atomic level. The RuO2-promoted interface-confined catalysis network successfully captures trace amounts of lost lattice oxygen and catalyzes the reversible reduction of activated O species. This configuration yields a specific discharge capacity of 307 mAh g−1 at 0.1 C, with an impressive capacity retention rate of 97% after 300 cycles at 1 C. The Ru-1||graphite pouch cell exhibits a superior capacity retention rate of 85% after 450 cycles at C/3 and the Ru-1||Li pouch cell exhibits a high energy density of 513 Wh kg−1. Our strategies involving the lithium-deficient layer and interface-confined catalysis offer novel insights into protecting the surface and enhancing oxygen reusability within the LRMO.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"40 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666612","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}
Songyang Chang, Wentao Hou, Angelica Del Valle-Perez, Irfan Ullah, Xiaoyu Du, Lisandro Cunci, Gerardo Morell, Xianyong Wu
Aqueous multivalent metal batteries represent an attractive option for energy storage. Currently, various metals have been attempted for aqueous battery operation, ranging from divalent metals (zinc, iron, nickel, manganese) to trivalent ones (antimony, indium). However, the fundamental cobalt plating chemistry remains largely neglected and poorly understood, despite its appealing merits in capacity, redox potential, and morphology. Herein, we bridge this knowledge gap by revealing highly reversible Co2+/Co plating reaction in a near-neutral 1 M CoCl2 aqueous electrolyte. Remarkably, cobalt demonstrates exceptional performance, characterized by modest polarization (48 mV), ultrahigh plating efficiency (~99.9%), long lifespan (4,000 hours, 5.5 months), and strong resistance to harsh conditions, including ultrahigh capacities (up to 30 mAh cm-2), ultralow currents (down to 0.05 mA cm-2), and extended storage periods (24-168 hours). The superb performance primarily stems from its closely packed, spherical, and dendrite-free morphology with a minimal surface area. Moreover, cobalt is fully compatible with various cathode materials, enabling high-energy (240 Wh kg-1), high-rate (80 A g-1), and long-cycling (20,000 cycles) batteries. These properties were achieved without delicate optimization of experimental parameters, highlighting the inherent merits of cobalt over other metal candidates. This work unlocks the potential of cobalt for constructing advanced aqueous multivalent batteries.
{"title":"Cobalt Metal Enables Ultrahigh-Efficiency, Long-Life, and Dendrite-Free Aqueous Multivalent Batteries","authors":"Songyang Chang, Wentao Hou, Angelica Del Valle-Perez, Irfan Ullah, Xiaoyu Du, Lisandro Cunci, Gerardo Morell, Xianyong Wu","doi":"10.1039/d4ee06091a","DOIUrl":"https://doi.org/10.1039/d4ee06091a","url":null,"abstract":"Aqueous multivalent metal batteries represent an attractive option for energy storage. Currently, various metals have been attempted for aqueous battery operation, ranging from divalent metals (zinc, iron, nickel, manganese) to trivalent ones (antimony, indium). However, the fundamental cobalt plating chemistry remains largely neglected and poorly understood, despite its appealing merits in capacity, redox potential, and morphology. Herein, we bridge this knowledge gap by revealing highly reversible Co2+/Co plating reaction in a near-neutral 1 M CoCl2 aqueous electrolyte. Remarkably, cobalt demonstrates exceptional performance, characterized by modest polarization (48 mV), ultrahigh plating efficiency (~99.9%), long lifespan (4,000 hours, 5.5 months), and strong resistance to harsh conditions, including ultrahigh capacities (up to 30 mAh cm-2), ultralow currents (down to 0.05 mA cm-2), and extended storage periods (24-168 hours). The superb performance primarily stems from its closely packed, spherical, and dendrite-free morphology with a minimal surface area. Moreover, cobalt is fully compatible with various cathode materials, enabling high-energy (240 Wh kg-1), high-rate (80 A g-1), and long-cycling (20,000 cycles) batteries. These properties were achieved without delicate optimization of experimental parameters, highlighting the inherent merits of cobalt over other metal candidates. This work unlocks the potential of cobalt for constructing advanced aqueous multivalent batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"3 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666613","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}
Minkang Wang, Han Su, Yu Zhong, Chuming Zhou, Guoli Chen, Xiuli Wang, Jiangping Tu
All-solid-state lithium-sulfur batteries (ASSLSBs) are emerging as next-generation energy storage systems, offering enhanced energy density, safety, and cost-effectiveness. However, the breakdown of the ion-conducting network within sulfur cathode limits their cycling life and poses challenges to practical application. Here, we design an innovative unitized encapsulation architecture to decouple and rebuild Li-ion transport pathways through interfacial spontaneous anion exchange behavior between Li5.5PS4.5Cl1.5 and Li3YBr6 electrolytes. In this design, the internal Li5.5PS4.5Cl1.5 enables durable intra-particle charge transfer trails, while the external halide Li3YBr6 framework establishes inter-particle Li-ion diffusion highways. This hierarchical ion-conducting mechanism facilitates efficient and durable Li-ion flow. Moreover, the core-shell configuration alleviates localized stress accumulation and catholyte irreversible decomposition during cycling, reinforcing robust ion-conducting pathways and persistent phase contact. The optimized sulfur cathode, S/LPSC@LYB-0.25, exhibits remarkable electrochemical performance, achieving 85% capacity retention over 1000 cycles under high sulfur loading of 8 mg cm−2 and a high current density of 6.7 mA cm−2. Developed pouch cells demonstrate unparalleled cycling stability under low stack pressure, retaining 76.9% capacity after 500 cycles. This work provides a practical and scalable strategy for tailored ion-conducing network architecture, advancing the industrial viability of ASSLSBs.
{"title":"A Unitized Encapsulation Architecture with Durable Epitaxial Ion-conductive Scaffolds for Ultrastable Solid-state Sulfur Cathode","authors":"Minkang Wang, Han Su, Yu Zhong, Chuming Zhou, Guoli Chen, Xiuli Wang, Jiangping Tu","doi":"10.1039/d4ee05668j","DOIUrl":"https://doi.org/10.1039/d4ee05668j","url":null,"abstract":"All-solid-state lithium-sulfur batteries (ASSLSBs) are emerging as next-generation energy storage systems, offering enhanced energy density, safety, and cost-effectiveness. However, the breakdown of the ion-conducting network within sulfur cathode limits their cycling life and poses challenges to practical application. Here, we design an innovative unitized encapsulation architecture to decouple and rebuild Li-ion transport pathways through interfacial spontaneous anion exchange behavior between Li5.5PS4.5Cl1.5 and Li3YBr6 electrolytes. In this design, the internal Li5.5PS4.5Cl1.5 enables durable intra-particle charge transfer trails, while the external halide Li3YBr6 framework establishes inter-particle Li-ion diffusion highways. This hierarchical ion-conducting mechanism facilitates efficient and durable Li-ion flow. Moreover, the core-shell configuration alleviates localized stress accumulation and catholyte irreversible decomposition during cycling, reinforcing robust ion-conducting pathways and persistent phase contact. The optimized sulfur cathode, S/LPSC@LYB-0.25, exhibits remarkable electrochemical performance, achieving 85% capacity retention over 1000 cycles under high sulfur loading of 8 mg cm−2 and a high current density of 6.7 mA cm−2. Developed pouch cells demonstrate unparalleled cycling stability under low stack pressure, retaining 76.9% capacity after 500 cycles. This work provides a practical and scalable strategy for tailored ion-conducing network architecture, advancing the industrial viability of ASSLSBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"61 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660892","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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