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An Electrochemically Paralleled Biomass Electrolyte Additive Facilitates the Integrated Modification of Multi-dimensional Zn Metal Batteries
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-29 DOI: 10.1039/d5ee00237k
Kefeng Ouyang, Sheng Chen, Lidong Yu, Hongyu Qin, Ao Liu, Youfa Liu, Quan Wu, Bingjie Ran, Shubing Wei, Fei Gao, Kun Zhang, Jin Hu, Yan Huang
A diverse array of Zn metal batteries (ZMBs) is swiftly emerging as a prominent force in the energy storage sector. The electrolyte modification is integral to improving ZMB performance by effectively optimizing the behavior of both the anode and cathode. However, most existing electrolytes are specifically tailored to individual battery systems, thereby limiting their broader applicability across different ZMB technologies. Herein, a universal electrolyte additive design strategy, termed "electrochemical parallelism", has been proposed to address this issue. By addressing critical challenges of poor reversibility of the Zn anode, severe pH fluctuation at the MnO2 electrode/electrolyte interface, solvent evaporation in open system, and corrosion induced by polyiodide ions, a multifunctional pyrrolidone carboxylate sodium (PCA-Na) additive is developed. Its integrated functionalities include Zn anode interfacial modification, Zn2+ solvation regulation, pH buffering, hydrogen bond network restructuring and polyiodide ions repulsion. As a result, it enables the Zn anode of symmetric pouch cell a cumulative plating capacity of 704 Ah, as well as Zn||MnO2 pouch cell with a discharge capacity exceeding 370 mAh, Zn-air battery with an electrolyte shelf life surpassing 1000 h, and 3.7 Ah-level Zn||I2 pouch cell with a capacity retention of 83% after 130 cycles. These advancements collectively realize the electrochemical parallel integration of ZMBs.
{"title":"An Electrochemically Paralleled Biomass Electrolyte Additive Facilitates the Integrated Modification of Multi-dimensional Zn Metal Batteries","authors":"Kefeng Ouyang, Sheng Chen, Lidong Yu, Hongyu Qin, Ao Liu, Youfa Liu, Quan Wu, Bingjie Ran, Shubing Wei, Fei Gao, Kun Zhang, Jin Hu, Yan Huang","doi":"10.1039/d5ee00237k","DOIUrl":"https://doi.org/10.1039/d5ee00237k","url":null,"abstract":"A diverse array of Zn metal batteries (ZMBs) is swiftly emerging as a prominent force in the energy storage sector. The electrolyte modification is integral to improving ZMB performance by effectively optimizing the behavior of both the anode and cathode. However, most existing electrolytes are specifically tailored to individual battery systems, thereby limiting their broader applicability across different ZMB technologies. Herein, a universal electrolyte additive design strategy, termed \"electrochemical parallelism\", has been proposed to address this issue. By addressing critical challenges of poor reversibility of the Zn anode, severe pH fluctuation at the MnO2 electrode/electrolyte interface, solvent evaporation in open system, and corrosion induced by polyiodide ions, a multifunctional pyrrolidone carboxylate sodium (PCA-Na) additive is developed. Its integrated functionalities include Zn anode interfacial modification, Zn2+ solvation regulation, pH buffering, hydrogen bond network restructuring and polyiodide ions repulsion. As a result, it enables the Zn anode of symmetric pouch cell a cumulative plating capacity of 704 Ah, as well as Zn||MnO2 pouch cell with a discharge capacity exceeding 370 mAh, Zn-air battery with an electrolyte shelf life surpassing 1000 h, and 3.7 Ah-level Zn||I2 pouch cell with a capacity retention of 83% after 130 cycles. These advancements collectively realize the electrochemical parallel integration of ZMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"72 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143733972","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}
引用次数: 0
Correction: Reconfiguring European industry for net-zero: a qualitative review of hydrogen and carbon capture utilization and storage benefits and implementation challenges
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-28 DOI: 10.1039/d5ee90031j
Benjamin K. Sovacool, Dylan Furszyfer Del Rio, Kyle Herman, Marfuga Iskandarova, Joao M. Uratani, Steve Griffiths
Correction for ‘Reconfiguring European industry for net-zero: a qualitative review of hydrogen and carbon capture utilization and storage benefits and implementation challenges’ by Benjamin K. Sovacool et al., Energy Environ. Sci., 2024, 17, 3523–3569, https://doi.org/10.1039/D3EE03270A.
{"title":"Correction: Reconfiguring European industry for net-zero: a qualitative review of hydrogen and carbon capture utilization and storage benefits and implementation challenges","authors":"Benjamin K. Sovacool, Dylan Furszyfer Del Rio, Kyle Herman, Marfuga Iskandarova, Joao M. Uratani, Steve Griffiths","doi":"10.1039/d5ee90031j","DOIUrl":"https://doi.org/10.1039/d5ee90031j","url":null,"abstract":"Correction for ‘Reconfiguring European industry for net-zero: a qualitative review of hydrogen and carbon capture utilization and storage benefits and implementation challenges’ by Benjamin K. Sovacool <em>et al.</em>, <em>Energy Environ. Sci.</em>, 2024, <strong>17</strong>, 3523–3569, https://doi.org/10.1039/D3EE03270A.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"57 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723183","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}
引用次数: 0
Strategies toward high-energy-density Co-free lithium nickel manganese oxide: From crystal structure to flexible configuration
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-28 DOI: 10.1039/d5ee00197h
Jiguo Tu, Yan Li, Bokun Zhang, Xiaoyun Wang, Ramachandran Vasant Kumar, Libo Chen, Shuqiang Jiao
High-voltage spinel lithium nickel manganese oxide (LNMO) stand out as a promising cobalt-free cathode material for lithium-ion batteries, due to its low cost, high voltage and energy density capabilities. However, the commercialization of LNMO is hindered by challenges such as structural instability, Mn dissolution, inadequate high-temperature performance, and relatively low tap density. This article presents a comprehensive framework that establishes the rational design principles for optimizing both active LNMO materials and overall battery performance. We summarize various modification strategies related to LNMO, encompassing crystal structure design, interfacial control, microscopic morphology regulation, as well as flexible configuration, all aimed at improving the reaction kinetics, energy density and high-temperature performance. Through the discussion of the current advancements and presentation of the perspectives on further development, it is expected to provide inspirations for further elevating the energy density and promoting the practical energy storage applications of LNMO-based batteries.
{"title":"Strategies toward high-energy-density Co-free lithium nickel manganese oxide: From crystal structure to flexible configuration","authors":"Jiguo Tu, Yan Li, Bokun Zhang, Xiaoyun Wang, Ramachandran Vasant Kumar, Libo Chen, Shuqiang Jiao","doi":"10.1039/d5ee00197h","DOIUrl":"https://doi.org/10.1039/d5ee00197h","url":null,"abstract":"High-voltage spinel lithium nickel manganese oxide (LNMO) stand out as a promising cobalt-free cathode material for lithium-ion batteries, due to its low cost, high voltage and energy density capabilities. However, the commercialization of LNMO is hindered by challenges such as structural instability, Mn dissolution, inadequate high-temperature performance, and relatively low tap density. This article presents a comprehensive framework that establishes the rational design principles for optimizing both active LNMO materials and overall battery performance. We summarize various modification strategies related to LNMO, encompassing crystal structure design, interfacial control, microscopic morphology regulation, as well as flexible configuration, all aimed at improving the reaction kinetics, energy density and high-temperature performance. Through the discussion of the current advancements and presentation of the perspectives on further development, it is expected to provide inspirations for further elevating the energy density and promoting the practical energy storage applications of LNMO-based batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"1 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723348","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}
引用次数: 0
Robust interphase derived from a dual-cation ionic liquid electrolyte enabling exceptional stability of high-nickel layered cathodes
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-28 DOI: 10.1039/d5ee00669d
Fanglin Wu, Haolin Tang, Jian Wang, Xilai Xue, Thomas Diemant, Shan Fang, Huihua Li, Ziyuan Lyu, Hao Li, En Xie, Hongzhen Lin, Jae-Kwang Kim, Guk Tae Kim, Stefano Passerini
Nickel-rich layered cathodes suffer from unstable interface and structural collapse, leading to poor cycling stability in conventional carbonate-based electrolytes. Ionic liquid electrolytes promise to enable high-safety and high-specific energy lithium metal batteries employing nickel-rich cathodes. However, the practical performance is limited by the low ionic conductivity and unsatisfying interphase formation, only allowing operation at relatively low current density. In this work, a dual-cation-IL-based electrolyte is employed, including NaPF6 as an additive tuning the solvation structure. This electrolyte, exhibiting high ionic conductivity (5.06 mS cm-1 at 20 oC), enables Li||LiNi0.83Co0.11Mn0.05B0.01O2 cells operating in the voltage range of 3.0-4.3 V with excellent capacity retention after 500 cycles at 1C (95.2%) and long 1500-cycle-lifespan (>80%). Even reducing the operative temperature down to 0 oC, the cells deliver high discharge capacity (above 150 mAh g-1) at 0.5C without capacity decay. Combining ex-situ X-ray photoelectron spectroscopy and time-of-flight secondary-ion mass spectrometry analysis, the electrode/electrolyte interphase derived from the NaPF6 additive is shown to be more robust and uniform, possibly granting the electrostatic shielding against Li dendrite growth. Meanwhile, the inorganics-dominated cathode/electrolyte interphase (CEI) greatly protects the cathode structure, inhibiting lattice distortion and microcracks as revealed by atom-level electronic microscopy and in-situ X-ray diffraction.
{"title":"Robust interphase derived from a dual-cation ionic liquid electrolyte enabling exceptional stability of high-nickel layered cathodes","authors":"Fanglin Wu, Haolin Tang, Jian Wang, Xilai Xue, Thomas Diemant, Shan Fang, Huihua Li, Ziyuan Lyu, Hao Li, En Xie, Hongzhen Lin, Jae-Kwang Kim, Guk Tae Kim, Stefano Passerini","doi":"10.1039/d5ee00669d","DOIUrl":"https://doi.org/10.1039/d5ee00669d","url":null,"abstract":"Nickel-rich layered cathodes suffer from unstable interface and structural collapse, leading to poor cycling stability in conventional carbonate-based electrolytes. Ionic liquid electrolytes promise to enable high-safety and high-specific energy lithium metal batteries employing nickel-rich cathodes. However, the practical performance is limited by the low ionic conductivity and unsatisfying interphase formation, only allowing operation at relatively low current density. In this work, a dual-cation-IL-based electrolyte is employed, including NaPF6 as an additive tuning the solvation structure. This electrolyte, exhibiting high ionic conductivity (5.06 mS cm-1 at 20 oC), enables Li||LiNi0.83Co0.11Mn0.05B0.01O2 cells operating in the voltage range of 3.0-4.3 V with excellent capacity retention after 500 cycles at 1C (95.2%) and long 1500-cycle-lifespan (&gt;80%). Even reducing the operative temperature down to 0 oC, the cells deliver high discharge capacity (above 150 mAh g-1) at 0.5C without capacity decay. Combining ex-situ X-ray photoelectron spectroscopy and time-of-flight secondary-ion mass spectrometry analysis, the electrode/electrolyte interphase derived from the NaPF6 additive is shown to be more robust and uniform, possibly granting the electrostatic shielding against Li dendrite growth. Meanwhile, the inorganics-dominated cathode/electrolyte interphase (CEI) greatly protects the cathode structure, inhibiting lattice distortion and microcracks as revealed by atom-level electronic microscopy and in-situ X-ray diffraction.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"10 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723347","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}
引用次数: 0
Aluminum Macrocycles Induced Superior High-temperature Capacitive Energy Storage for Polymer-based Dielectrics via Constructing Charge Trap Rings
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-27 DOI: 10.1039/d4ee05689b
Zhongbin Pan, Yu Cheng, Zhicheng Li, Pang Xi, Peng Wang, Xu Fan, Hanxi Chen, Jinjun Liu, Junfei Luo, Jinhong Yu, Minhao Yang, Jiwei Zhai, Weiping Li
Electrostatic capacitors are typically necessary to operate in harsh-temperature environments to fulfill the demanding requirements of renewable energy, electrified transportations, and advanced propulsion systems. However, achieving exceptional capacitive performance in polymer dielectrics at elevated temperatures and electric fields remains a formidable challenge owing to the exponential growth of conduction loss. Herein, we propose a new class of polymer dielectric composites comprising polyetherimide (PEI) incorporated with monodispersed aluminum macrocycle (AOC). The Al-O backbone of AOC creates a ring, where electron-rich O atoms own a strong charge scattering effect and electron-deficient Al atoms have a charge captured capability. Such a unique structure reduces both electron concentration and mobility, thereby effectively inhibiting charge transport within polymer dielectrics and significantly suppressing the high-temperature electrical conduction loss even at high electric fields. Consequently, the PEI-AOC composite exhibits the maximum discharged energy density with an efficiency above 90% of 6.57 J/cm3 and 4.4 J/cm3 at 150°C and 200 °C, which exceed those of the original dielectric by more than ten-fold under identical conditions. This work presents a groundbreaking approach to manipulate the high-temperature capacitive performance of polymer dielectrics in practical power apparatus and electronic devices.
{"title":"Aluminum Macrocycles Induced Superior High-temperature Capacitive Energy Storage for Polymer-based Dielectrics via Constructing Charge Trap Rings","authors":"Zhongbin Pan, Yu Cheng, Zhicheng Li, Pang Xi, Peng Wang, Xu Fan, Hanxi Chen, Jinjun Liu, Junfei Luo, Jinhong Yu, Minhao Yang, Jiwei Zhai, Weiping Li","doi":"10.1039/d4ee05689b","DOIUrl":"https://doi.org/10.1039/d4ee05689b","url":null,"abstract":"Electrostatic capacitors are typically necessary to operate in harsh-temperature environments to fulfill the demanding requirements of renewable energy, electrified transportations, and advanced propulsion systems. However, achieving exceptional capacitive performance in polymer dielectrics at elevated temperatures and electric fields remains a formidable challenge owing to the exponential growth of conduction loss. Herein, we propose a new class of polymer dielectric composites comprising polyetherimide (PEI) incorporated with monodispersed aluminum macrocycle (AOC). The Al-O backbone of AOC creates a ring, where electron-rich O atoms own a strong charge scattering effect and electron-deficient Al atoms have a charge captured capability. Such a unique structure reduces both electron concentration and mobility, thereby effectively inhibiting charge transport within polymer dielectrics and significantly suppressing the high-temperature electrical conduction loss even at high electric fields. Consequently, the PEI-AOC composite exhibits the maximum discharged energy density with an efficiency above 90% of 6.57 J/cm3 and 4.4 J/cm3 at 150°C and 200 °C, which exceed those of the original dielectric by more than ten-fold under identical conditions. This work presents a groundbreaking approach to manipulate the high-temperature capacitive performance of polymer dielectrics in practical power apparatus and electronic devices.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"15 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713433","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}
引用次数: 0
Single-atom mediated crystal facet engineering for the exceptional production of acetate in CO electrolysis 通过单原子介导的晶体面工程,在一氧化碳电解过程中实现醋酸盐的卓越生产
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-26 DOI: 10.1039/d4ee06192f
Jiacheng Liu, Yan Wen, Wei Yan, Zhongliang Huang, Xiaozhi Liu, Xuan Huang, Changhong Zhan, Yuqi Zhang, Wei-Hsiang Huang, Chih-Wen Pao, Zhiwei Hu, Dong Su, Shunji Xie, Ye Wang, Jiajia Han, Haifeng Xiong, Xiaoqing Huang, Nanjun Chen
The production of value-added liquid fuels via the electroreduction of CO has received widespread attention. Although copper (Cu) has demonstrated promising activity in producing multi-carbon products, the yield of a specific product like acetate remains limited, resulting in low resource utilization efficiency. Here, we present a Co single-atom mediated Cu(111) (CuCo1) triangular sheet, in which the Co single atom was specifically modified on the exposed Cu (111) crystal face. Importantly, CuCo1 sheets achieve an exceptional acetate Faradaic efficiency of 72% at a high current density of 600 mA cm-2, along with the topmost acetate formation rate of 1.11 μmol s-1 cm-2, surpassing most state-of-the-art Cu-type catalysts. Moreover, the CuCo1-based membrane electrode assembly (MEA) enables a stable production of acetate at 600 mA cm-2 for over 500 h, demonstrating the exceptional stability of CuCo1. In situ spectroscopic and computational investigations suggest that Co single atoms can significantly modulate the CO activation step to form *CO adsorption on both the top and bridge sites of Cu sheets, triggering the asymmetric C−C coupling to facilitate the *OCCOH intermediate. Furthermore, Co single atom reduces the energy barrier for the second hydrogenation step over Cu(111), thereby stabilizing ethenone production and enhancing acetate yield. This work provides an avenue to design highly efficient and stable Cu catalysts via the combination of crystal facet design and single atom promoter.
{"title":"Single-atom mediated crystal facet engineering for the exceptional production of acetate in CO electrolysis","authors":"Jiacheng Liu, Yan Wen, Wei Yan, Zhongliang Huang, Xiaozhi Liu, Xuan Huang, Changhong Zhan, Yuqi Zhang, Wei-Hsiang Huang, Chih-Wen Pao, Zhiwei Hu, Dong Su, Shunji Xie, Ye Wang, Jiajia Han, Haifeng Xiong, Xiaoqing Huang, Nanjun Chen","doi":"10.1039/d4ee06192f","DOIUrl":"https://doi.org/10.1039/d4ee06192f","url":null,"abstract":"The production of value-added liquid fuels via the electroreduction of CO has received widespread attention. Although copper (Cu) has demonstrated promising activity in producing multi-carbon products, the yield of a specific product like acetate remains limited, resulting in low resource utilization efficiency. Here, we present a Co single-atom mediated Cu(111) (CuCo1) triangular sheet, in which the Co single atom was specifically modified on the exposed Cu (111) crystal face. Importantly, CuCo1 sheets achieve an exceptional acetate Faradaic efficiency of 72% at a high current density of 600 mA cm<small><sup>-2</sup></small>, along with the topmost acetate formation rate of 1.11 μmol s<small><sup>-1</sup></small> cm<small><sup>-2</sup></small>, surpassing most state-of-the-art Cu-type catalysts. Moreover, the CuCo1-based membrane electrode assembly (MEA) enables a stable production of acetate at 600 mA cm<small><sup>-2</sup></small> for over 500 h, demonstrating the exceptional stability of CuCo1. In situ spectroscopic and computational investigations suggest that Co single atoms can significantly modulate the CO activation step to form *CO adsorption on both the top and bridge sites of Cu sheets, triggering the asymmetric C−C coupling to facilitate the *OCCOH intermediate. Furthermore, Co single atom reduces the energy barrier for the second hydrogenation step over Cu(111), thereby stabilizing ethenone production and enhancing acetate yield. This work provides an avenue to design highly efficient and stable Cu catalysts via the combination of crystal facet design and single atom promoter.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"61 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703265","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}
引用次数: 0
Porous Organic Materials-Based Atomically Dispersed Metal Electrocatalysts
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-26 DOI: 10.1039/d5ee00273g
Hao Zhang, Suwen Wang, Enmin Lv, menghui qi, Chengchao He, Xing-Long Dong, Jieshan Qiu, Yong Wang, Zhenhai Wen
The transition to renewable energy sources and the need for efficient energy conversion technologies have led to the development of various types of catalysts, among which atomically dispersed metal catalysts (ADMCs) supported by porous organic materials (POMs) have attracted attention for their high catalytic efficiency and stability. This review focuses on the development and application of ADMCs supported by POMs, such as MOFs, COFs, and HOFs, which offer catalytic performance due to their high atomic utilization, stability, and selectivity. The paper systematically explores various strategies for synthesizing ADMCs, including the use of organic linkers, metal nodes, and pore spaces within POMs to stabilize metal atoms and prevent aggregation. Key applications highlighted include energy conversion and storage technologies, such as fuel cells, water splitting, CO2 reduction and nitrogen reduction, where ADMCs demonstrate the potential to replace noble metals. Despite progress, challenges remain in achieving high metal loading, long-term stability, and cost-effective large-scale production. The study underscores the importance of advanced characterization techniques and computational models to deepen the understanding of ADMCs’ catalytic mechanisms and guide future material design, paving the way for their broader application in sustainable energy technologies.
向可再生能源的过渡以及对高效能源转换技术的需求促使人们开发了各种类型的催化剂,其中以多孔有机材料(POMs)为支撑的原子分散金属催化剂(ADMCs)因其高催化效率和稳定性而备受关注。本综述重点介绍了由多孔有机材料(如 MOFs、COFs 和 HOFs)支撑的 ADMCs 的开发和应用,这些 ADMCs 因其原子利用率高、稳定性和选择性强而具有良好的催化性能。本文系统地探讨了合成 ADMC 的各种策略,包括使用有机连接体、金属节点和 POM 内的孔隙来稳定金属原子并防止聚集。重点介绍的主要应用包括能量转换和储存技术,如燃料电池、水分离、二氧化碳还原和氮还原,在这些应用中,ADMC 展示了取代贵金属的潜力。尽管取得了进展,但在实现高金属负载、长期稳定性和具有成本效益的大规模生产方面仍存在挑战。这项研究强调了先进表征技术和计算模型的重要性,有助于加深对ADMC催化机理的理解,指导未来的材料设计,为其在可持续能源技术中的更广泛应用铺平道路。
{"title":"Porous Organic Materials-Based Atomically Dispersed Metal Electrocatalysts","authors":"Hao Zhang, Suwen Wang, Enmin Lv, menghui qi, Chengchao He, Xing-Long Dong, Jieshan Qiu, Yong Wang, Zhenhai Wen","doi":"10.1039/d5ee00273g","DOIUrl":"https://doi.org/10.1039/d5ee00273g","url":null,"abstract":"The transition to renewable energy sources and the need for efficient energy conversion technologies have led to the development of various types of catalysts, among which atomically dispersed metal catalysts (ADMCs) supported by porous organic materials (POMs) have attracted attention for their high catalytic efficiency and stability. This review focuses on the development and application of ADMCs supported by POMs, such as MOFs, COFs, and HOFs, which offer catalytic performance due to their high atomic utilization, stability, and selectivity. The paper systematically explores various strategies for synthesizing ADMCs, including the use of organic linkers, metal nodes, and pore spaces within POMs to stabilize metal atoms and prevent aggregation. Key applications highlighted include energy conversion and storage technologies, such as fuel cells, water splitting, CO2 reduction and nitrogen reduction, where ADMCs demonstrate the potential to replace noble metals. Despite progress, challenges remain in achieving high metal loading, long-term stability, and cost-effective large-scale production. The study underscores the importance of advanced characterization techniques and computational models to deepen the understanding of ADMCs’ catalytic mechanisms and guide future material design, paving the way for their broader application in sustainable energy technologies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"215 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703266","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}
引用次数: 0
Over 12% efficiency solar-powered green hydrogen production from seawater
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-25 DOI: 10.1039/d4ee06203e
Xuanjie Wang, Jintong Gao, Yipu Wang, Yayuan Liu, Xinyue Liu, Lenan Zhang
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.
太阳能驱动的水电解为大规模生产绿色氢气带来了巨大希望。然而,与电解相关的大量耗水不仅增加了绿色氢气的成本,还引发了对水资源短缺加速的严重关切。虽然海水可以作为绿色制氢的无限水源,但其复杂的成分给高效可靠的电解带来了巨大挑战。在这里,我们展示了一种利用海水进行高效太阳能绿色制氢的方法。我们的方法利用了太阳能的全光谱利用。光伏发电用于驱动电解,而太阳能电池产生的废热则用于通过海水蒸馏生产清洁水。以自然阳光和真实海水为唯一输入,我们在实验中证明了 12.6% 的太阳能制氢效率,以及在一个太阳光照下 35.9 升/平方米/小时的绿色氢气生产率,其中额外 1.2 升/平方米/小时的清洁水为副产品。通过减少对清洁水和电力供应的依赖,这项工作为获取绿色氢气提供了一种完全可持续的战略,具有良好的能源效率和技术经济可行性。
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引用次数: 0
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
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-25 DOI: 10.1039/d4ee05456c
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.
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引用次数: 0
High-performance inverted perovskite solar cells and modules via aminothiazole passivation
IF 32.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-03-25 DOI: 10.1039/d5ee01083g
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}
引用次数: 0
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Energy & Environmental Science
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