The incorporation of redox-active molecules into aqueous electrolytes addressed the challenges in the development of energy storage devices by enhancing energy density, expanding voltage windows, and improving cycling stability. Aqueous Zinc-ion hybrid capacitors (ZICs), which combine the characteristics of metal-ion batteries and supercapacitors, are emerging to meet high energy-power demands. Herein, we investigate the irreversible and reversible dynamics of azobenzene compounds in the development of redox electrolytes for ZIC applications. The results reveal that Sunset Yellow (SY) additives promote reversible Zn2+ stripping/plating at the Zn anode through ion-ligand coordination, while the redox behavior of the -N=N- group enhances the interfacial charge transfer. The passivation behavior of redox electrolytes, derived by SY molecules, was investigated using in-situ electrochemical atomic force microscopy. Morphology evolution, coupled with nanomechanical tests, shed light on the transformation of SY-containing electrolytes. The redox electrolytes improve the lifespan of Zn//Zn cells from 50 to 1700 cycles at 2 mA cm−2 and 1 mAh cm−2 by suppressing parasitic reactions and mitigating by-product formation. The redox-enhanced ZIC delivers an increased capacity of 113.3 mAh g−1 with improved cycling stability, compared to 75.2 mAh g−1 of ZnSO4 electrolytes without SY molecules at 0.6 mA g-1. A range of azobenzene-based compounds with varying structures were investigated to demonstrate the synergistic modulating effects. The results demonstrate the molecular engineering of redox electrolytes and provide fundamental insights into electrochemical interphase transformation.
{"title":"Unraveling the Dynamic Transformation of Azobenzene-driven Redox Electrolytes for Zn-ion Hybrid Capacitors","authors":"Ming Chen, Li Gong, Igor Zhitomirsky, Kaiyuan Shi","doi":"10.1039/d4ee05696e","DOIUrl":"https://doi.org/10.1039/d4ee05696e","url":null,"abstract":"The incorporation of redox-active molecules into aqueous electrolytes addressed the challenges in the development of energy storage devices by enhancing energy density, expanding voltage windows, and improving cycling stability. Aqueous Zinc-ion hybrid capacitors (ZICs), which combine the characteristics of metal-ion batteries and supercapacitors, are emerging to meet high energy-power demands. Herein, we investigate the irreversible and reversible dynamics of azobenzene compounds in the development of redox electrolytes for ZIC applications. The results reveal that Sunset Yellow (SY) additives promote reversible Zn2+ stripping/plating at the Zn anode through ion-ligand coordination, while the redox behavior of the -N=N- group enhances the interfacial charge transfer. The passivation behavior of redox electrolytes, derived by SY molecules, was investigated using in-situ electrochemical atomic force microscopy. Morphology evolution, coupled with nanomechanical tests, shed light on the transformation of SY-containing electrolytes. The redox electrolytes improve the lifespan of Zn//Zn cells from 50 to 1700 cycles at 2 mA cm−2 and 1 mAh cm−2 by suppressing parasitic reactions and mitigating by-product formation. The redox-enhanced ZIC delivers an increased capacity of 113.3 mAh g−1 with improved cycling stability, compared to 75.2 mAh g−1 of ZnSO4 electrolytes without SY molecules at 0.6 mA g-1. A range of azobenzene-based compounds with varying structures were investigated to demonstrate the synergistic modulating effects. The results demonstrate the molecular engineering of redox electrolytes and provide fundamental insights into electrochemical interphase transformation.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736661","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}
Hyo Jin, Dong Woog Lee, Jeonguk Hwang, Min Hoon Myung, Jee Ho Ha, Seungwoo Choi, Soon-Jae Jung, Seunghyun Lee, Jinwoo Park, Young-Ryul Kim, Nyung Joo Kong, Youngsik Kim, Hyun-Wook Lee, Hyunhyub Ko, Tae Joo Shin, Seok Ju Kang, Myung-Jin Baek
Common polymer binders are insulators, which significantly diminish the battery performance owing to their low electron mobility. For aqueous sodium-air batteries (SABs) to exhibit reliable performance as energy storage systems, polymer binders should possess high electrolyte wettability, strong underwater adhesion, high crystallinity, and conductivity to efficiently transport electrons to current collectors without degradation or dissolution over time. In this study, the electrochemical performance of SABs was significantly improved using a newly developed binder containing poly(ethylene glycol), catechol, and anthracene (At) functional groups. Versatile analysis of the polymer, including two-dimensional grazing incidence-wide-angle X-ray diffraction and polarized optical microscopy, showed that the enhanced SAB performance can be attributed to the At groups which have high crystallinity due to π–π stacking, thereby lowering the resistance and increasing the electrical conductivity. Because of the catechol and PEG groups, the binder also possessed reliable underwater adhesion, and electrolyte wettability, which are essential for aqueous SAB binders. Moreover, the binder effectively prevented carbon corrosion of the carbon current collector in the air electrode. We believe that the synthesized semi-crystalline polymer binder can be applied to various batteries to improve their electrochemical performance and stability.
{"title":"Semi-crystalline polymer binder with enhanced electrical conductivity and strong underwater adhesion in aqueous sodium-air batteries","authors":"Hyo Jin, Dong Woog Lee, Jeonguk Hwang, Min Hoon Myung, Jee Ho Ha, Seungwoo Choi, Soon-Jae Jung, Seunghyun Lee, Jinwoo Park, Young-Ryul Kim, Nyung Joo Kong, Youngsik Kim, Hyun-Wook Lee, Hyunhyub Ko, Tae Joo Shin, Seok Ju Kang, Myung-Jin Baek","doi":"10.1039/d5ee01350j","DOIUrl":"https://doi.org/10.1039/d5ee01350j","url":null,"abstract":"Common polymer binders are insulators, which significantly diminish the battery performance owing to their low electron mobility. For aqueous sodium-air batteries (SABs) to exhibit reliable performance as energy storage systems, polymer binders should possess high electrolyte wettability, strong underwater adhesion, high crystallinity, and conductivity to efficiently transport electrons to current collectors without degradation or dissolution over time. In this study, the electrochemical performance of SABs was significantly improved using a newly developed binder containing poly(ethylene glycol), catechol, and anthracene (At) functional groups. Versatile analysis of the polymer, including two-dimensional grazing incidence-wide-angle X-ray diffraction and polarized optical microscopy, showed that the enhanced SAB performance can be attributed to the At groups which have high crystallinity due to π–π stacking, thereby lowering the resistance and increasing the electrical conductivity. Because of the catechol and PEG groups, the binder also possessed reliable underwater adhesion, and electrolyte wettability, which are essential for aqueous SAB binders. Moreover, the binder effectively prevented carbon corrosion of the carbon current collector in the air electrode. We believe that the synthesized semi-crystalline polymer binder can be applied to various batteries to improve their electrochemical performance and stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"31 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736658","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}
Seán R. Kavanagh, Rasmus Svejstrup Nielsen, John Lundsgaard Hansen, Rasmus Schmidt Davidsen, Ole Hansen, Alp E Samli, Peter C K Vesborg, David O. Scanlon, Aron Walsh
Selenium has reemerged as a promising absorber material for tandem and indoor photovoltaic (PV) devices due to its elemental simplicity, unique structural features, and wide band gap. However, despite rapid recent improvements, record Se solar cells only reach a third of their achievable effi- ciencies at the radiative limit, primarily due to a low open-circuit voltage relative to the band gap. The origins of this voltage deficit, along with the high doping densities often reported for trigonal selenium (t-Se), remain unclear. Here, we explore the point defect chemistry of t-Se combining first-principles calculations with experimental studies of thin-films from state-of-the-art PV devices. Our findings reveal a remarkable ability of the helical t-Se chains to reconstruct and form low-energy amphoteric defects, particularly in the case of self-vacancies and hydrogen, pnictogen, and halogen impurities. While chalcogen impurities and self-interstitials also form low-energy defects, these are electrically neutral. We also find that both intrinsic and extrinsic point defects do not contribute significantly to doping, either due to electrical inactivity (chalcogens) or self-compensation (hydro- gen, halogens, pnictogens). Finally, we show that intrinsic point defects do not form detrimental non-radiative recombination centres and propose that PV performance is instead limited by other factors. These findings highlight the potential of Se as a defect-tolerant absorber, while optimising interfaces and extended structural imperfections is key to unlocking its full performance potential.
{"title":"Intrinsic point defect tolerance in selenium for indoor and tandem photovoltaics","authors":"Seán R. Kavanagh, Rasmus Svejstrup Nielsen, John Lundsgaard Hansen, Rasmus Schmidt Davidsen, Ole Hansen, Alp E Samli, Peter C K Vesborg, David O. Scanlon, Aron Walsh","doi":"10.1039/d4ee04647a","DOIUrl":"https://doi.org/10.1039/d4ee04647a","url":null,"abstract":"Selenium has reemerged as a promising absorber material for tandem and indoor photovoltaic (PV) devices due to its elemental simplicity, unique structural features, and wide band gap. However, despite rapid recent improvements, record Se solar cells only reach a third of their achievable effi- ciencies at the radiative limit, primarily due to a low open-circuit voltage relative to the band gap. The origins of this voltage deficit, along with the high doping densities often reported for trigonal selenium (t-Se), remain unclear. Here, we explore the point defect chemistry of t-Se combining first-principles calculations with experimental studies of thin-films from state-of-the-art PV devices. Our findings reveal a remarkable ability of the helical t-Se chains to reconstruct and form low-energy amphoteric defects, particularly in the case of self-vacancies and hydrogen, pnictogen, and halogen impurities. While chalcogen impurities and self-interstitials also form low-energy defects, these are electrically neutral. We also find that both intrinsic and extrinsic point defects do not contribute significantly to doping, either due to electrical inactivity (chalcogens) or self-compensation (hydro- gen, halogens, pnictogens). Finally, we show that intrinsic point defects do not form detrimental non-radiative recombination centres and propose that PV performance is instead limited by other factors. These findings highlight the potential of Se as a defect-tolerant absorber, while optimising interfaces and extended structural imperfections is key to unlocking its full performance potential.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"53 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736657","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}
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}
Benjamin K. Sovacool, Dylan Furszyfer Del Rio, Kyle Herman, Marfuga Iskandarova, Joao M. Uratani and 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 and Steve Griffiths","doi":"10.1039/D5EE90031J","DOIUrl":"10.1039/D5EE90031J","url":null,"abstract":"<p >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.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 8","pages":" 3869-3869"},"PeriodicalIF":32.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ee/d5ee90031j?page=search","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":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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}
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 (>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}
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}
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}
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.
{"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}
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