Seawater electrolysis offers a potential avenue for the unlimited production of green hydrogen. However, developing low-cost and highly stable electrocatalysts remains a critical challenge. Herein, we developed a waste materialization strategy to directly construct a novel Pt/Pd@SOG electrocatalyst from the recycled automobile catalyst and graphite anode. The as-fabricated catalyst exhibited superior performance in alkaline seawater electrolysis, delivering a low overpotential of 195 mV and 333 mV at current densities of 10 mA cm⁻² and 100 mA cm⁻² for hydrogen evolution reaction (HER), respectively, outperforming the commercial Pt/C (228 mV and 372 mV). The state-of-the-art high turnover frequency (TOF) of 43.745 s⁻¹ has been delivered. Additionally, the catalyst demonstrated exceptional stability at a current density of 100 mA cm⁻² for over 192 hours. A comprehensive characterization and mechanism study reveals that the graphene-based material provides a fast electron transport pathway and guarantees excellent electron conductivity to the catalytic active center, while the d-d orbital coupling between Pt and Pd within the as-synthesized Pt/Pd@SOG significantly lowers the energy barrier for electron transfer during catalytic reaction and stabilizes the intermediate's adsorption at the Pt sites, thus promoting the HER reaction. This research demonstrates a rapid valorization pathway for synergistic materializing multiple city mine wastes for advanced seawater electrocatalyst, which synergistically addresses the critical element cycling challenge and paves the way for sustainable energy catalysis.
{"title":"Synergistic Upcycling Pt/Pd and Graphite from City Mines for Highly Efficient Seawater Hydrogen Evolution Catalysis","authors":"Wenhan Cheng, Shuichang Liu, Qingsong Jiang, Songhe Yang, Yangzi Shangguan, Jian Hu, Jiaxin Liang, Shengyao Jin, Weixu Zhong, Xiangyang Lou, Hong Chen","doi":"10.1039/d5ta00055f","DOIUrl":"https://doi.org/10.1039/d5ta00055f","url":null,"abstract":"Seawater electrolysis offers a potential avenue for the unlimited production of green hydrogen. However, developing low-cost and highly stable electrocatalysts remains a critical challenge. Herein, we developed a waste materialization strategy to directly construct a novel Pt/Pd@SOG electrocatalyst from the recycled automobile catalyst and graphite anode. The as-fabricated catalyst exhibited superior performance in alkaline seawater electrolysis, delivering a low overpotential of 195 mV and 333 mV at current densities of 10 mA cm⁻² and 100 mA cm⁻² for hydrogen evolution reaction (HER), respectively, outperforming the commercial Pt/C (228 mV and 372 mV). The state-of-the-art high turnover frequency (TOF) of 43.745 s⁻¹ has been delivered. Additionally, the catalyst demonstrated exceptional stability at a current density of 100 mA cm⁻² for over 192 hours. A comprehensive characterization and mechanism study reveals that the graphene-based material provides a fast electron transport pathway and guarantees excellent electron conductivity to the catalytic active center, while the d-d orbital coupling between Pt and Pd within the as-synthesized Pt/Pd@SOG significantly lowers the energy barrier for electron transfer during catalytic reaction and stabilizes the intermediate's adsorption at the Pt sites, thus promoting the HER reaction. This research demonstrates a rapid valorization pathway for synergistic materializing multiple city mine wastes for advanced seawater electrocatalyst, which synergistically addresses the critical element cycling challenge and paves the way for sustainable energy catalysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"7 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuqing Yue, Hongkai Zhang, Jie Fu, Changtan Qu, Yueyue Gao, Bin Wei, Yuchuan Shao, Yifan Zheng, Wei Shi
Perovskite solar cell (PSCs), with their high efficiency and low-cost potential, have emerged as a promising alternative in the photovoltaic industry. The attainment of rapid output in large-scale PSC modules requires addressing several critical challenges, with the optimization of the top electrode being of utmost importance. This comprehensive review elucidates recent developments in solution-processed top electrodes for PSCs, analyzing the impact of various electrode materials, architectures, and fabrication techniques on device performance. Through a meticulous examination of the existing reports, effective strategies for enhancing the efficiency of PSCs are delineated, addressing both immediate market demands and broader applications in renewable energy. The insights derived from this review provide invaluable guidance for optimizing top electrodes, which may catalyze significant improvements in the efficiency and stability of PSCs, thereby accelerating their commercialization trajectory. The implications of this study are far-reaching, with the potential to transform the renewable energy landscape through advancements in PSC technology.
{"title":"From lab to fab: solution-processed top electrodes for commercializing perovskite solar cells","authors":"Yuqing Yue, Hongkai Zhang, Jie Fu, Changtan Qu, Yueyue Gao, Bin Wei, Yuchuan Shao, Yifan Zheng, Wei Shi","doi":"10.1039/d4ta08802f","DOIUrl":"https://doi.org/10.1039/d4ta08802f","url":null,"abstract":"Perovskite solar cell (PSCs), with their high efficiency and low-cost potential, have emerged as a promising alternative in the photovoltaic industry. The attainment of rapid output in large-scale PSC modules requires addressing several critical challenges, with the optimization of the top electrode being of utmost importance. This comprehensive review elucidates recent developments in solution-processed top electrodes for PSCs, analyzing the impact of various electrode materials, architectures, and fabrication techniques on device performance. Through a meticulous examination of the existing reports, effective strategies for enhancing the efficiency of PSCs are delineated, addressing both immediate market demands and broader applications in renewable energy. The insights derived from this review provide invaluable guidance for optimizing top electrodes, which may catalyze significant improvements in the efficiency and stability of PSCs, thereby accelerating their commercialization trajectory. The implications of this study are far-reaching, with the potential to transform the renewable energy landscape through advancements in PSC technology.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Adjusting the interfacial interaction between metal and support in loaded electrocatalysts is critical for enhancing the performance of electrocatalytic hydrogen evolution in both acidic and basic media, yet it continues to pose a significant challenge. This study proposes a sulfur doping strategy aimed at enhancing the strong metal–support interaction (SMSI) of ultra-small platinum (Pt) nanoparticles (NPs) uniformly encapsulated within nitrogen–sulfur co-doped carbon materials (NSC). This approach modulates the coordination environment and electronic structure of the Pt material, leading to substantial charge redistribution at the closely interfaced Pt–carbon layer heterojunction, thereby facilitating a rapid hydrogen evolution reaction (HER). The Pt/NSC exhibits excellent intrinsic activity at 1.0 M KOH (η10 = 17.8 mV, 30.59 mV dec−1) and 0.5 M H2SO4 (η10 = 10.2 mV, 18.85 mV dec−1), demonstrating a lower overpotential and a reduced Tafel slope, significantly outperforming the commercial Pt/C catalyst. Furthermore, owing to the exceptional stability of NSC and the pronounced confinement effect at the interface, Pt/NSC exhibits robust resistance to both acid and alkaline corrosion. Experimental and theoretical investigations reveal that the strong interfacial coupling effect can facilitate spontaneous electron transfer from the support to the Pt NPs. The electron-rich Pt NPs significantly enhance the efficiency of charge transfer and optimize the chemisorption behavior of intermediates, thereby improving the kinetics of hydrogen production.
{"title":"Sulfur doping activated metal–support interaction drives Pt nanoparticles to achieve acid–base hydrogen evolution reaction","authors":"Yagang Li, Jiaqing Luo, Peilin Liu, Liangkun Zhang, Weiyu Song, Yuechang Wei, Zhen Zhao, Xiao Zhang, Jian Liu, Yuanqing Sun","doi":"10.1039/d4ta08499c","DOIUrl":"https://doi.org/10.1039/d4ta08499c","url":null,"abstract":"Adjusting the interfacial interaction between metal and support in loaded electrocatalysts is critical for enhancing the performance of electrocatalytic hydrogen evolution in both acidic and basic media, yet it continues to pose a significant challenge. This study proposes a sulfur doping strategy aimed at enhancing the strong metal–support interaction (SMSI) of ultra-small platinum (Pt) nanoparticles (NPs) uniformly encapsulated within nitrogen–sulfur co-doped carbon materials (NSC). This approach modulates the coordination environment and electronic structure of the Pt material, leading to substantial charge redistribution at the closely interfaced Pt–carbon layer heterojunction, thereby facilitating a rapid hydrogen evolution reaction (HER). The Pt/NSC exhibits excellent intrinsic activity at 1.0 M KOH (<em>η</em><small><sub>10</sub></small> = 17.8 mV, 30.59 mV dec<small><sup>−1</sup></small>) and 0.5 M H<small><sub>2</sub></small>SO<small><sub>4</sub></small> (<em>η</em><small><sub>10</sub></small> = 10.2 mV, 18.85 mV dec<small><sup>−1</sup></small>), demonstrating a lower overpotential and a reduced Tafel slope, significantly outperforming the commercial Pt/C catalyst. Furthermore, owing to the exceptional stability of NSC and the pronounced confinement effect at the interface, Pt/NSC exhibits robust resistance to both acid and alkaline corrosion. Experimental and theoretical investigations reveal that the strong interfacial coupling effect can facilitate spontaneous electron transfer from the support to the Pt NPs. The electron-rich Pt NPs significantly enhance the efficiency of charge transfer and optimize the chemisorption behavior of intermediates, thereby improving the kinetics of hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"88 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Arghanoon Moeini, Kassio Zanoni, Cristina Roldán Carmona, Henk J. Bolink
Perovskite photovoltaics have recently achieved significant breakthroughs in cell efficiency, while offering simple and low-cost processability. Vacuum-based techniques are gaining increased attention due to their scalability and material versatility. However, fully vacuum-deposited devices remain rare, partly due to the limited availability of charge transport materials compatible with vacuum-deposition. Additionally, sublimed organic contact materials often require high work function interlayers, like MoO3, or molecular oxidants, which complicate device stability. In this study we explore the use of simpler non-extended conjugated self-assemble monolayers (SAMs) as alternatives to these high work function interlayers, demonstrating improved hole extraction, higher fill factors, and enhanced long-term stability compared to state-of-the art vacuum-deposited architectures. As a proof of concept, devices incorporating SAMs/TaTm (N4,N4,N4″,N4″-tetra([1,1′-biphenyl]-4-yl)-[1,1′:4′,1″-terphenyl]-4,4″-diamine) interfaces and methylammonium lead iodide perovskite (MAPbI3) achieve power conversion efficiencies exceeding 19.5 %, approaching the highest reported values for fully evaporated stacks, along with remarkable thermal stability at 85 ºC.
{"title":"Engineering stable p-type contacts towards efficient fully vacuum deposited perovskite solar cells","authors":"Arghanoon Moeini, Kassio Zanoni, Cristina Roldán Carmona, Henk J. Bolink","doi":"10.1039/d5ta00429b","DOIUrl":"https://doi.org/10.1039/d5ta00429b","url":null,"abstract":"Perovskite photovoltaics have recently achieved significant breakthroughs in cell efficiency, while offering simple and low-cost processability. Vacuum-based techniques are gaining increased attention due to their scalability and material versatility. However, fully vacuum-deposited devices remain rare, partly due to the limited availability of charge transport materials compatible with vacuum-deposition. Additionally, sublimed organic contact materials often require high work function interlayers, like MoO3, or molecular oxidants, which complicate device stability. In this study we explore the use of simpler non-extended conjugated self-assemble monolayers (SAMs) as alternatives to these high work function interlayers, demonstrating improved hole extraction, higher fill factors, and enhanced long-term stability compared to state-of-the art vacuum-deposited architectures. As a proof of concept, devices incorporating SAMs/TaTm (N4,N4,N4″,N4″-tetra([1,1′-biphenyl]-4-yl)-[1,1′:4′,1″-terphenyl]-4,4″-diamine) interfaces and methylammonium lead iodide perovskite (MAPbI3) achieve power conversion efficiencies exceeding 19.5 %, approaching the highest reported values for fully evaporated stacks, along with remarkable thermal stability at 85 ºC.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677777","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jianghu Yu, Chong-yu Wang, Hao Liang, Yangwei Wang, Ze-Yuan Yang, yi xin Zhang, Jing Feng, Zhen-Hua Ge
Thermoelectric materials hold significant promise as they can directly convert thermal energy into electrical energy. Despite the discovery of numerous new thermoelectric materials in recent years, bismuth telluride(Bi2Te3)-based materials continue to be the most suitable for large-scale commercialization. Presently, there is scope for further improvement in the average ZT value and conversion efficiency of Bi2Te3-based materials. This study presents the successful synthesis of Bi0.42Sb1.58Te3(BST) alloys and ZIF-8 with high porosity and adjustable pore size using the solid-phase sintering method and spark plasma sintering(SPS). This method facilitates the doping of Bi sites and produces several atomic clusters in the BST matrix, significantly optimizing the electrical and thermal transport properties of BST thermoelectric materials. The Bi sites undergo low-valent cation doping, and additional hole carriers are introduced to optimize the electrical conductivity. Moreover, a large number of atomic clusters in the BST matrix act as effective phonon scattering centers, enhancing phonon scattering and reducing lattice thermal conductivity. Additionally, ZńBi,Sb defects are observed as defect clusters around the nanopores, which further reduce the lattice thermal conductivity. Notably, the ZT of Bi0.42Sb1.58Te3/0.3 wt% ZIF-8 sample reaches 1.42 at 348 K, and the average ZT is as high as 1.16 in the temperature range of 300–500 K due to the synergistic optimization of thermal and electrical transport properties. Furthermore, the thermoelectric conversion efficiency of the single-leg device reaches 5.03% at ΔT=250 K, and the mechanical properties of the sample are significantly improved. Due to the fine grain strengthening effect, the hardness of the 0.3 wt% doped sample is 1.2 GPa, and its Young's modulus is 43 GPa, exhibiting significant improvement compared to the pure sample. The findings of this study are expected to provide valuable insights for the optimization of other thermoelectric materials.
{"title":"Synergistic enhancement of thermoelectric and mechanical properties in Bi-Sb-Te alloys collaborated by Zn based metal organic framework (ZIF-8)","authors":"Jianghu Yu, Chong-yu Wang, Hao Liang, Yangwei Wang, Ze-Yuan Yang, yi xin Zhang, Jing Feng, Zhen-Hua Ge","doi":"10.1039/d5ta01631b","DOIUrl":"https://doi.org/10.1039/d5ta01631b","url":null,"abstract":"Thermoelectric materials hold significant promise as they can directly convert thermal energy into electrical energy. Despite the discovery of numerous new thermoelectric materials in recent years, bismuth telluride(Bi2Te3)-based materials continue to be the most suitable for large-scale commercialization. Presently, there is scope for further improvement in the average ZT value and conversion efficiency of Bi2Te3-based materials. This study presents the successful synthesis of Bi0.42Sb1.58Te3(BST) alloys and ZIF-8 with high porosity and adjustable pore size using the solid-phase sintering method and spark plasma sintering(SPS). This method facilitates the doping of Bi sites and produces several atomic clusters in the BST matrix, significantly optimizing the electrical and thermal transport properties of BST thermoelectric materials. The Bi sites undergo low-valent cation doping, and additional hole carriers are introduced to optimize the electrical conductivity. Moreover, a large number of atomic clusters in the BST matrix act as effective phonon scattering centers, enhancing phonon scattering and reducing lattice thermal conductivity. Additionally, ZńBi,Sb defects are observed as defect clusters around the nanopores, which further reduce the lattice thermal conductivity. Notably, the ZT of Bi0.42Sb1.58Te3/0.3 wt% ZIF-8 sample reaches 1.42 at 348 K, and the average ZT is as high as 1.16 in the temperature range of 300–500 K due to the synergistic optimization of thermal and electrical transport properties. Furthermore, the thermoelectric conversion efficiency of the single-leg device reaches 5.03% at ΔT=250 K, and the mechanical properties of the sample are significantly improved. Due to the fine grain strengthening effect, the hardness of the 0.3 wt% doped sample is 1.2 GPa, and its Young's modulus is 43 GPa, exhibiting significant improvement compared to the pure sample. The findings of this study are expected to provide valuable insights for the optimization of other thermoelectric materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"8 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sai Sundara Sandeep Ganti, Pintu Kumar Roy, Nayonay Wagh, Kona Naga Surya Siva Sai, Sushant Kumar
The role of ammonia would continue to be significant in the changing energy landscape with focus on mitigating carbon footprints per unit of ammonia production. Since ammonia is a zero-carbon molecule and increasingly considered as an important hydrogen energy carrier for future energy systems, its generation under mild conditions and subsequent industrial acceptance becomes critical. Therefore, the recent challenges are to design and engineer alternative but greener methods that can generate ammonia at low input energy that will facilitate inexpensive, localized, and renewable-coupled ammonia generation. This review underscores the recent development in design strategies of novel catalysts, specially emphasizing recent advances in different class of thermal, electrochemical, and non-thermal plasmacatalysis that can generate ammonia under mild conditions. Hence, this article can serve as a comprehensive work for engineering novel catalysts and methods which can contribute to generation of sustainable and cost-efficient solutions for expanding landscape of ammonia applications.
{"title":"Strategically Designed Catalysts for Ammonia Synthesis Under Mild Conditions: Recent Advances and Challenges","authors":"Sai Sundara Sandeep Ganti, Pintu Kumar Roy, Nayonay Wagh, Kona Naga Surya Siva Sai, Sushant Kumar","doi":"10.1039/d4ta08232j","DOIUrl":"https://doi.org/10.1039/d4ta08232j","url":null,"abstract":"The role of ammonia would continue to be significant in the changing energy landscape with focus on mitigating carbon footprints per unit of ammonia production. Since ammonia is a zero-carbon molecule and increasingly considered as an important hydrogen energy carrier for future energy systems, its generation under mild conditions and subsequent industrial acceptance becomes critical. Therefore, the recent challenges are to design and engineer alternative but greener methods that can generate ammonia at low input energy that will facilitate inexpensive, localized, and renewable-coupled ammonia generation. This review underscores the recent development in design strategies of novel catalysts, specially emphasizing recent advances in different class of thermal, electrochemical, and non-thermal plasmacatalysis that can generate ammonia under mild conditions. Hence, this article can serve as a comprehensive work for engineering novel catalysts and methods which can contribute to generation of sustainable and cost-efficient solutions for expanding landscape of ammonia applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"9 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672508","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Agricultural biomass is a kind of abundant renewable resources in nature, the effective conversion of agricultural biomass to chemical fuel is crucial for reducing dependence on fossil fuels, but it was limited by the absence of appropriate conversion strategies. Here, we report a simple photocatalytic system for rapid conversion of agricultural biomass to H2 by using few-layer MoS2 modified ultra-small TiO2 nanopaticles (MoS2@TiO2 NPs) as photocatalysts. In α-cellulose system, the H2 generation rate of optimized photocatalyst achieves 1653 under 300 W Xe lamp irradiation, and the apparent quantum yield at 380 nm reaches 5.62%. Meanwhile, comparable photocatalytic H2 generation activity was achieved from different agricultural biomass of rice straw, corn straw, wheat straw, rice husk, soybean straw and corncob sources, with a maximum H2 generation rate of 50 μmol·g-1·h-1 in corncob system. The high photocatalytic H2 production activity of MoS2@TiO2 NPs photocatalyst was contributed to the large specific surface area of TiO2 NPs and abundant active sites of MoS2, which respectively promotes biomass oxidation and H2 generation reaction. This study provides a green approach for agricultural biomass upgrading through photocatalysis strategy.
{"title":"Solar driven conversion of agricultural biomass to H2 over few-layer MoS2 modified ultra-small TiO2 nanopaticles photocatalysts","authors":"Yun-Hui Hu, Jia-Hao Wang, Yan Chen, Ji-Ping Tang, Zi-Yi Wang, Yong-Jun Yuan","doi":"10.1039/d5ta00763a","DOIUrl":"https://doi.org/10.1039/d5ta00763a","url":null,"abstract":"Agricultural biomass is a kind of abundant renewable resources in nature, the effective conversion of agricultural biomass to chemical fuel is crucial for reducing dependence on fossil fuels, but it was limited by the absence of appropriate conversion strategies. Here, we report a simple photocatalytic system for rapid conversion of agricultural biomass to H2 by using few-layer MoS2 modified ultra-small TiO2 nanopaticles (MoS2@TiO2 NPs) as photocatalysts. In α-cellulose system, the H2 generation rate of optimized photocatalyst achieves 1653 under 300 W Xe lamp irradiation, and the apparent quantum yield at 380 nm reaches 5.62%. Meanwhile, comparable photocatalytic H2 generation activity was achieved from different agricultural biomass of rice straw, corn straw, wheat straw, rice husk, soybean straw and corncob sources, with a maximum H2 generation rate of 50 μmol·g-1·h-1 in corncob system. The high photocatalytic H2 production activity of MoS2@TiO2 NPs photocatalyst was contributed to the large specific surface area of TiO2 NPs and abundant active sites of MoS2, which respectively promotes biomass oxidation and H2 generation reaction. This study provides a green approach for agricultural biomass upgrading through photocatalysis strategy.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"20 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Poly (ethylene oxide) (PEO) composite solid-state electrolytes have been considered as promising candidate electrolytes for all-solid-state lithium batteries with high safety and excellent mechanical properties. However, the ionic conductivity of PEO-based electrolytes is usually low at room temperature, which limits their performance in practical applications. Moreover, the interfacial compatibility with high-voltage cathode materials remains a challenge despite the better compatibility with lithium metal anodes. The inevitable problem of lithium dendrite growth is also affecting the safety performance of this battery. Ionic liquids (ILs) with high conductivity and ionic mobility, enabling batteries to achieve a higher electrochemical window, offers a new platform for more environmentally friendly and sustainable all-solid-state lithium batteries. Considering that there has been a surge of exciting research activities in the field of PEO/ILs systems, this review is tended to summarize the mechanism of different kinds of ILs in PEO-based solid polymer electrolytes, and provide a comprehensive overview of the application of ILs in all-solid-state lithium batteries from a view of fillers. Ultimately, this information is expected to guide the design and optimization of novel PEO/ILs systems with enhanced properties for real-world applications.
{"title":"Advances in the Application of Ionic Liquids in PEO-based Lithium Ion Solid-State Electrolytes: From A View of Fillers","authors":"Changchun Ai, Yilei Shu, Ziheng Zhao, Huijuan Guo, Shangqing Chen, Qun Yi","doi":"10.1039/d4ta09243k","DOIUrl":"https://doi.org/10.1039/d4ta09243k","url":null,"abstract":"Poly (ethylene oxide) (PEO) composite solid-state electrolytes have been considered as promising candidate electrolytes for all-solid-state lithium batteries with high safety and excellent mechanical properties. However, the ionic conductivity of PEO-based electrolytes is usually low at room temperature, which limits their performance in practical applications. Moreover, the interfacial compatibility with high-voltage cathode materials remains a challenge despite the better compatibility with lithium metal anodes. The inevitable problem of lithium dendrite growth is also affecting the safety performance of this battery. Ionic liquids (ILs) with high conductivity and ionic mobility, enabling batteries to achieve a higher electrochemical window, offers a new platform for more environmentally friendly and sustainable all-solid-state lithium batteries. Considering that there has been a surge of exciting research activities in the field of PEO/ILs systems, this review is tended to summarize the mechanism of different kinds of ILs in PEO-based solid polymer electrolytes, and provide a comprehensive overview of the application of ILs in all-solid-state lithium batteries from a view of fillers. Ultimately, this information is expected to guide the design and optimization of novel PEO/ILs systems with enhanced properties for real-world applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"27 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Prussian blue analogues (PBAs) are a promising cathode material for sodium-ion batteries, and the iron-based Prussian blue has a higher specific capacity while being widely available and inexpensive, so it has received more widespread attention. However, Fe2+ in the aqueous phase will form the structure of [Fe(H2O)6]2+, water molecules will inevitably be introduced during the synthesis process, resulting in water molecule residues and vacancy defects, which greatly affects the cycling life of PBAs, energy density and bring safety issues. Herein, a facile “ligand pre-exchange strategy” is proposed to synthesize highly crystallized PBAs. Ethylene glycol (EG) is introduced for exchanging water molecules in [Fe(H2O)6]2+ to form a water-deficient solvated structure of [Fe(EG)x(H2O)6-x]2+, which reduces the coordinated water and vacancy defects in the Prussian blue material and forms high-quality Prussian blue crystals. Meanwhile, the formation of [Fe(EG)x(H2O)6-x]2+ was demonstrated by Fourier Transform Infrared Spectrum (FT-IR) and quantum chemical calculations using Density functional theory (DFT), proving this strategy's feasibility. The PB-EG-5 electrode prepared by this strategy has excellent sodium storage performance and fast kinetics, with a specific capacity of 91.3 mAh g-1 at 1000 mA g-1 in a half cell and capacity retention of 70% after 1000 cycles, while, the full cell also has excellent electrochemical performance. This work provides a new feasible solution for the large-scale preparation of high-quality PBAs.
{"title":"Lessening Prussian blue analogues coordinated water with a novel strategy as cathode for Sodium-ion batteries","authors":"Yunfang Gao, Yongdong Wang, Shiji Zhu, Xin Xu, chen yang, Zhennan Wu, Junzi Zheng, Jie Wu","doi":"10.1039/d5ta00120j","DOIUrl":"https://doi.org/10.1039/d5ta00120j","url":null,"abstract":"Prussian blue analogues (PBAs) are a promising cathode material for sodium-ion batteries, and the iron-based Prussian blue has a higher specific capacity while being widely available and inexpensive, so it has received more widespread attention. However, Fe2+ in the aqueous phase will form the structure of [Fe(H2O)6]2+, water molecules will inevitably be introduced during the synthesis process, resulting in water molecule residues and vacancy defects, which greatly affects the cycling life of PBAs, energy density and bring safety issues. Herein, a facile “ligand pre-exchange strategy” is proposed to synthesize highly crystallized PBAs. Ethylene glycol (EG) is introduced for exchanging water molecules in [Fe(H2O)6]2+ to form a water-deficient solvated structure of [Fe(EG)x(H2O)6-x]2+, which reduces the coordinated water and vacancy defects in the Prussian blue material and forms high-quality Prussian blue crystals. Meanwhile, the formation of [Fe(EG)x(H2O)6-x]2+ was demonstrated by Fourier Transform Infrared Spectrum (FT-IR) and quantum chemical calculations using Density functional theory (DFT), proving this strategy's feasibility. The PB-EG-5 electrode prepared by this strategy has excellent sodium storage performance and fast kinetics, with a specific capacity of 91.3 mAh g-1 at 1000 mA g-1 in a half cell and capacity retention of 70% after 1000 cycles, while, the full cell also has excellent electrochemical performance. This work provides a new feasible solution for the large-scale preparation of high-quality PBAs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"33 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Electrocatalytic nitrate reduction reaction (eNitRR) plays an essential role in maintaining the nitrogen cycle balance and the development of carbon-free energy sources. However, the complex reduction processes results in the preparation of ammonia with low Faraday efficiency and selectivity. Here, we constructed a tandem catalyst composing of dual active sites of copper and cuprous oxide by a facile electrodeposition technique, which effectively promotes the adsorption of nitrate and the conversion of nitrite, achieving high Faraday efficiency of 95.8% and ammonia yield of 1.583 mmol h-1 cm-2. Density Functional Theory (DFT) calculations revealed that the Cu2O surface could significantly reduce the energy barrier associated with NO3- adsorption, and the Cu component could capture the *NO2 produced by the Cu2O component in time for the subsequent reaction. Furthermore, when the catalyst was used as the cathode of the Zn-NO3- cell, the assembled cell achieved an open-circuit voltage of 1.37 V and a power density of as high as 3.78 mW cm-2 in neutral electrolyte. This study provides new insights into the mechanism of electrocatalytic NH3 production.
{"title":"The promotion of nitrate conversion into ammonia via the construction of tandem dual active sites of copper and cuprous oxide","authors":"Yujiao Wang, Zhiman Bai, Kun Huang, Shan Wang, Fusheng Wang, Mingzai Wu","doi":"10.1039/d5ta01268f","DOIUrl":"https://doi.org/10.1039/d5ta01268f","url":null,"abstract":"Electrocatalytic nitrate reduction reaction (eNitRR) plays an essential role in maintaining the nitrogen cycle balance and the development of carbon-free energy sources. However, the complex reduction processes results in the preparation of ammonia with low Faraday efficiency and selectivity. Here, we constructed a tandem catalyst composing of dual active sites of copper and cuprous oxide by a facile electrodeposition technique, which effectively promotes the adsorption of nitrate and the conversion of nitrite, achieving high Faraday efficiency of 95.8% and ammonia yield of 1.583 mmol h-1 cm-2. Density Functional Theory (DFT) calculations revealed that the Cu2O surface could significantly reduce the energy barrier associated with NO3- adsorption, and the Cu component could capture the *NO2 produced by the Cu2O component in time for the subsequent reaction. Furthermore, when the catalyst was used as the cathode of the Zn-NO3- cell, the assembled cell achieved an open-circuit voltage of 1.37 V and a power density of as high as 3.78 mW cm-2 in neutral electrolyte. This study provides new insights into the mechanism of electrocatalytic NH3 production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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