Journal of Materials Chemistry A最新文献

{"title":"Ultrahigh peak power density of rechargeable Zn-Air batteries using quadruple perovskite as air-cathode electrocatalyst","authors":"Sujan Sen, Tapas Kumar Mandal","doi":"10.1039/d5ta00184f","DOIUrl":"https://doi.org/10.1039/d5ta00184f","url":null,"abstract":"Developing highly active, low-cost and stable bifunctional electrocatalysts is vital for the commercialization of rechargeable Zn-air batteries (ZABs). By far, among the various materials used as catalysts for ZABs, perovskite oxides have gained significant attention due to their structural and compositional flexibility. Herein, we report a quadruple perovskite oxide LaCu3FeTiRu2O12 as a highly efficient OER and ORR active bifunctional electrocatalyst for rechargeable ZABs. An excellent activity with a bifunctional index (BI) of 0.80 V comparable to the state-of-the-art OER-ORR electrocatalyst RuO2-Pt/C (BI = 0.75 V) is demonstrated by the quadruple perovskite. The outstanding bifunctional activity of the compound is believed to stem from its unique crystal structure that provides energetically favorable Fe/Ti/Ru−Cu bridging active sites for the electrocatalysis. The ZAB fabricated using LaCu3FeTiRu2O12 as air-cathode electrocatalyst shows long cyclic stability with an unprecedented peak power density of 635 mW/cm2, which is three times higher than that of the benchmark RuO2-Pt/C.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"68 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598918","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}

{"title":"Ultra-low Content Induced Intercalation Anomaly of Graphite Anode Enables Superior Capacity at Sub-zero Temperatures","authors":"Febri Baskoro, Po-Yu Yang, Hong-Jhen Lin, Robin Chih-Hsing Wang, Hui Qi Wong, Hsinhan Tsai, Chun-Wei Pao, Heng-Liang Wu, Hung-Ju Yen","doi":"10.1039/d4ta08958h","DOIUrl":"https://doi.org/10.1039/d4ta08958h","url":null,"abstract":"The rapid development of energy storage devices has pushed Li-ion batteries (LIBs) bear down for higher performance, better safety, lower cost, and capable to operate in wide range temperatures. However, most LIBs are used only in favorable environments rather than extreme conditions such as in ocean exploration, tropical areas, high altitude drones, and polar expeditions. When chronically or periodically exposed to these harsh environments, conventional LIBs will fail to operate due to hindered ion conductivity, interfacial issues, and sluggish desolvation of Li-ion. Additionally, graphite has been recognized as the-state-of-the-art LIBs negative electrode due to their mechanical stability, electrical conductivity, cost-efficiency, and abundant availability. However, limited Li+ storage capacity of 372 mA h g-1 via LiC6 coordination has become a bottleneck and hindered its further application for next-generation LIBs. Here we reported intercalation anomaly under ultra-low graphite content that enables super-lithiation stage in the electrode. The ultrahigh rate capability (2200 mA h g-1 at 1C and 1100 mA h g-1 at 30C) in graphite anode was achieved by reducing its amount within the electrode and adding more conductive filler in the electrode creating a highly conductive system. When operated at -20 °C, the ultra-low graphite anode keeps 50% capacity (1100 mA h g-1) of room temperature, and ranks the best among LIB anodes toward commercialization. Systematical spectroscopy analysis reveals that additional capacitive behavior and a distinct structural evolution, which leads to Li+ intercalation anomaly up to LiC2, within ultra-low graphite content electrode significantly improve graphite electrode capacity beyond 372 mA h g-1. Additionally, when the battery operated at sub-zero temperature, this unique electrode structure with higher conductive environment help to overcome the sluggish desolvation process at interface and slow diffusion in the bulk electrodes. This finding shed a new light in the graphite chemistry and pave the way on the development of anode-less lithium-ion batteries..","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"31 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599035","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}

{"title":"Regulation of nitrogen reduction reaction catalytic performance by varying sp/sp2 hybrid carbon ratio in graphyne/graphene heterojunction catalysts","authors":"Zexiang Yin, Zijun Yang, Yingmei Bian, Heng Zhao, Beijia Chen, Yuan Liu, Yang Wang, Yida Deng, Haozhi Wang","doi":"10.1039/d5ta01226k","DOIUrl":"https://doi.org/10.1039/d5ta01226k","url":null,"abstract":"This study investigates the impact of the sp/sp2 hybrid carbon ratio on the nitrogen reduction reaction (NRR) catalytic performance of γ-graphyne and graphene-based heterojunction catalysts. Through density of states (DOS) calculations, crystal orbital Hamiltonian population (COHP), and charge density difference plots, it is found that the sp/sp2 hybrid carbon ratio significantly influences the electronic properties and NRR activity of the catalysts. The Ti@GY1/Gr catalyst exhibites superior performance, attributed to its sensitivity to changes in the sp/sp2 hybrid environment, especially when combined with graphene. An increase in the sp/sp2 hybrid carbon ratio lead to a decrease in NRR activity, while also modulating the interaction between Ti and the carbon support. The findings highlight the importance of the sp/sp2 hybrid carbon ratio in regulating the electronic properties and catalytic performance of heterojunction catalysts, providing insights for the design of more efficient NRR catalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"203 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598913","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}

{"title":"Efficient Ethane Production viaSnCl4Lewis Acid-EnhancedCO2Electroreduction in a Flow Cell Electrolyser","authors":"Sankeerthana Bellamkonda, Ian Brewis, Venkateswarulu Gedela, Rana Faisal Shahzad, Mohamed Mamlouk, Shahid Rasul","doi":"10.1039/d5ta00176e","DOIUrl":"https://doi.org/10.1039/d5ta00176e","url":null,"abstract":"The development of efficient and selective catalysts for electrochemical CO2 reduction (CO2RR) is critical for advancing sustainable energy solutions. Here, we report a unique catalyst system based on SnCl4 Lewis acid-modified Cu2O, demonstrating enhanced performance in CO2 electroreduction to ethane. The SnCl4 modification introduces chloride ions directly onto the Cu O surface, creating a synergistic interaction between Sn, Cl, and Cu2 active sites that optimizes the electronic environment for CO2RR. The catalyst was coated onto a gas diffusion electrode (GDE) and tested in a flow cell electrolyser, with a Fumapem F950 cation exchange membrane and a platinum (Pt) foil as the anode. This system achieved a peak Faradaic efficiency of 34.8% for ethane production at -1.0 V vs. RHE, along with 11.3% efficiency for ethylene. Electrochemical studies revealed that the SnCl4-modified Cu2O exhibits low charge transfer resistance and high stability during prolonged electrolysis, with total current densities reaching 74.8 mA cm-2. Mechanistic investigations, supported by density functional theory, Raman, XRD, and electrochemical Impedance spectroscopy analyses, highlight the critical role of chloride ions in stabilizing CO intermediates and facilitating C-C bond formation, essential for C2 product generation. Operating in a flow cell configuration, the system demonstrated high energy efficiency and selectivity, establishing the SnCl4-modified Cu2O (CTC) as a promising catalyst for CO2RR. These findings offer a scalable and economically viable pathway for renewable hydrocarbon production, paving the way for practical applications in carbon-neutral energy cycles.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"4 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598917","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}

{"title":"Reduced graphene oxides prepared via mass loading controlling non-explosive thermal reduction for high volumetric capacitance supercapacitors","authors":"Jianing Tan, Zhaoyuan Liu, Wei Guo, Gang Li, Wei Wu","doi":"10.1039/d5ta01172h","DOIUrl":"https://doi.org/10.1039/d5ta01172h","url":null,"abstract":"Graphene oxide (GO) is known to undergo volume expansion during rapid and high temperature heat treatment, resulting in a low packing density and thus a poor volumetric capacitance. This paper reports a non-explosive thermal reduction strategy (NET) to prepare compact thermal reduced graphene oxide (NE-TRGO) by controlling the mass loading of the GO film below a typical value (< 5 mg cm-2). On one hand, the NET strategy effectively inhibits the expansion of graphene sheets, and thus the optimized NE-TRGO exhibits a high packing density of 1.94 g cm-3. On the other hand, NET strategy contributes to preserve the electrochemically active C-OH and C=O groups. Due to the high packing density and the abundance of electrochemically active groups, the gravimetric and volumetric capacitance of the optimized NE-TRGO were 314 F g-1 and 609 F cm-3 @ 0.1 A g-1, respectively, with excellent rate capability (160 F g-1 and 310 F cm-3 @ 10 A g-1) and significant cycling performance (~ 99% capacitance retention after 9 000 cycling at 5 A g-1). The assembled symmetric supercapacitor delivers an energy density of 9.5 W h L-1 at a power density of 96.7 W L-1 and 1.5 W h L-1 at a power density of 1056.3 W L-1. This NET strategy represents a simple and feasible heat treatment approach to control the packing density and oxygen functional groups of graphene-based materials toward compact energy storage devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"17 2 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598916","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}

{"title":"Blade-Coated Organic Photovoltaics with Dichlorophthalic Acid Self-Assembled Monolayer","authors":"Yingcong Zheng, Cenqi Yan, Hongxiang Li, Wei He, Jiayuan Zhu, Yingyue Hu, Jiayu Wang, Yufei Gong, Lei Meng, Yongfang Li, Pei Cheng","doi":"10.1039/d5ta00713e","DOIUrl":"https://doi.org/10.1039/d5ta00713e","url":null,"abstract":"To meet the demands of future industrialization, organic photovoltaics (OPVs) necessitate improved power conversion efficiency (PCE) and optimized manufacturing processes. Anode interfacial layer (AIL) is a critical component within OPV architecture. Yet, the prevalent PEDOT:PSS AIL exhibits hygroscopic and acidic nature, undermining device stability. Herein, we introduce 4,5-Dichlorophthalic Acid (2C2BA), a self-assembled monolayer (SAM) material, as an AIL. The 2C2BA AIL is formed by in situ self-assembly following the deposition of the donor:acceptor:2C2BA solution, obviating extra monolayer processing. Both active layer of small- and large-area devices are fabricated by blade coating. Devices with a PM6:BO-4Cl active layer and 2C2BA AIL achieve a high PCE of 17.8%, exceeding PEDOT:PSS-based devices at 17.4%. Devices with PM6:BTP-eC9 and 2C2BA achieve a high PCE of 18.1%, and an notable short-circuit current density (JSC) of 28.2 mA cm-2. Scaling to 2cm2, PM6:BTP-eC9-based OPVs with 2C2BA hit a PCE of 16.7%, outperforming OPV devices or modules with areas ≥ 2 cm2 with SAM from the literature. This work stands as an advancement in the application of SAM for large-area OPVs, providing insights into the scalable and high-throughput OPV manufacturing.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"54 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598922","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}

{"title":"A role of CuO sintering additive on the sinterability of Ba-based perovskite electrolytes for protonic ceramic electrochemical cell applications","authors":"George Starostin, Mariam Akopyan, Inna A Starostina, Guangming Yang, Dmitry Medvedev, Zongping Shao","doi":"10.1039/d5ta00875a","DOIUrl":"https://doi.org/10.1039/d5ta00875a","url":null,"abstract":"The addition of sintering additives is frequently regarded as an effective approach to increase the density of proton-conducting oxide materials for their subsequent application as thin-film electrolytes for high-efficiency and high-performance protonic ceramic fuel cells (PCFCs) and electrolysis cells (PCECs). Although the positive effects of sintering additives on the sinterability of materials have been repeatedly confirmed, the nature of their localization in produced ceramics remains unclear. In particular, an analysis of approximately 20 studies related to the use of CuO for the densification of Ba-based ceramics does not allow solid conclusions about the real role of CuO to be drawn. Some researchers believe that CuO acts as a dopant, whereas others detect no significant solubility but instead observe the formation of Cu-containing impurities. To overcome the ambiguity of the different experimental results, we selected a reference system of BaSn0.8Y0.2O3−δ + x wt% CuO (BSYx, 0 ≤ x ≤ 2) and performed complex structural, microstructural, and electrochemical characterization using the as-prepared (oxidized) and H2-treated (reduced) ceramics. Our results indicate that CuO facilitates liquid-phase sintering and therefore cannot act as a dopant, as CuO segregates at the grain boundaries or surface ceramic sites upon cooling. Furthermore, the high-temperature sintering of the studied materials at 1500 °C allows for the evaporation of the majority of the CuO (~90%), thereby reducing the potential negative effects of CuO on proton transport. Electrochemical impedance spectroscopy analysis demonstrated that the BSYx ceramics exhibit high grain boundary proton transport, which is beneficial for the prospective application of such or similar electrolyte systems in PCFCs and PCECs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"39 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598912","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}

{"title":"Fully-Packed Ultrasmall Au Nanoclusters in Covalent Organic Frameworks as Positive Electrodes for Supercapacitors","authors":"Jianxin Ma, Yanping Sun, Zhongjie Cai, Faisal Ahmad, yelan xiao, Tong Shu, Xueji Zhang","doi":"10.1039/d4ta08510h","DOIUrl":"https://doi.org/10.1039/d4ta08510h","url":null,"abstract":"Supported metal nanoclusters have emerged as highly promising class of materials with great potential across a wide range of applications including electrochemistry. However, fully-metal-loading of supports with ultrasmall pore structures, such as covalent organic frameworks (COFs), which might yield new performances, remains a challenge. Learning from the synthetic strategy of atomically-precise Au nanoclusters, Au elements are first complexed with alkynyl-modified building blocks prior to synthesis of COFs and a subsequent in-situ reduction then allows the size-focused formation of Au nanoclusters within each pore. With a partially-reduced Au content as high as ~50.8 wt %, the composites of Au nanocluster-filled COFs surprisingly exhibit a remarkable decrease in resistance as low as 80.16 Ω compared to their parent COFs, i.e. 4341 Ω for the pristine COFs and 3328 Ω for the Au(I) complex-tethered COFs, this dramatic reduction in resistance opens up the possibility for the construction of supercapacitors. The composites show impressive specific capacitance of 241.4 F·g-1 at a current density of 0.1 A·g-1 along with excellent rate capability at high scan rate of 200 mV·s-1. This work can be expanded to a general strategy for molecularly designing COFs with various metal NCs, potentially endowing the composites with novel application possibilities.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"20 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143598921","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}

{"title":"Pt-Mn-Al trimetallic nanoporous catalyst for reversible hydrogenation/oxidative dehydrogenation of N-heterocycles","authors":"Yunpeng Wang, Ziyi Zhang, Shize Wang, Qiang Xu, Xiujuan Feng, Yanhui Li, Xuan Zhang, Yoshinori Yamamoto, Ming Bao","doi":"10.1039/d5ta00724k","DOIUrl":"https://doi.org/10.1039/d5ta00724k","url":null,"abstract":"An unsupported trimetallic nanoporous catalyst PtMnAlNPore was developed as an efficient catalyst for hydrogenation/oxidative dehydrogenation of N-heterocycles. The catalyst showed 92% yield with 100% selectivity for the hydrogenation of quinolines into 1,2,3,4-tetrahydroquinolines (py-THQs) and 95% yield with 96% selectivity for the oxidative dehydrogenation of py-THQs into quinolines. SEM and XPS revealed a unique nanoporous structure and the electron interactions between the metallic elements of PtMnAlNPore. The excellent hydrogen-activation ability and oxygen-activation ability were identified to be intrinsic of outstanding activity of PtMnAlNPore in the dual catalytic process. The PtMnAlNPore has a stable structure and can be reused several times without loss of activity. This study demonstrated the exceptional catalytic performance of the PtMnAlNPore in hydrogenation/dehydrogenation of N-heterocycles, presenting new possibilities for the application of PtMnAlNPore in the field of catalysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"87 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599034","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}

{"title":"A 7.5 V window dual-functional planar micro-device based on biopolymer ionogel electrolyte for charge storage and neuromorphic computing","authors":"Simantini Majumdar, Ann Mary Antony, Giridhar U. Kulkarni","doi":"10.1039/d5ta00490j","DOIUrl":"https://doi.org/10.1039/d5ta00490j","url":null,"abstract":"The increasing demand for miniaturized electronics arises from the need for compact, energy-efficient devices that can perform complex functions, enabling advancements in applications such as wearable technology, the Internet of Things (IoT), and high-performance computing systems. Current miniaturized electronics face challenges in integrating efficient energy storage with adaptive, synaptic-like behaviours, often requiring complex interfaces and additional protective coatings, which limit scalability and performance. Conventional supercapacitors and neuromorphic devices are typically developed separately, hindering the development of compact, multifunctional systems. This work overcomes these limitations by introducing a dual-functional micro-device that combines charge storage with synaptic plasticity, eliminating the need for extra coatings and enabling the seamless integration of energy storage and neuromorphic functionality in miniaturized electronics. The device utilizes a lithium-ion conducting biopolymer ionogel electrolyte, composed of a chitosan/gelatin blend and 1-Butyl-3-methylimidazolium tetrafluoroborate ionic liquid in an interdigitated microelectrode configuration, which enables a sufficiently high ionic conductivity (~10-4 S/cm), and remarkable dielectric constant (~1610). The device demonstrates an exceptionally wide electrochemical potential window of 7.5 V, showcasing exceptional supercapacitive performance with an areal capacitance of 5.78 F/cm², positioning it as a high-performance micro-supercapacitor. The same device also exhibits synaptic plasticity behaviour, with potentiation and depression phases driven by ion migration, charge accumulation, and redox reactions, demonstrating tunable behaviour through pulse width and pulse number modulation. This unique electrochemical response, coupled with ionic double layer formation at the electrode/ionogel interface, underscores the potential of the device for both energy storage and neuromorphic computing applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"68 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143600036","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}