Journal of Materials Chemistry A最新文献

{"title":"Chaotropic anion-mediated ionic coordination structure and dynamic interface enabling stable alkaline zinc–nickel batteries with ultra-low N/P under high DOD","authors":"Xiaorui Liu,Hao Li,Ziyi Wang,Jianghao Liang,Gengmao Shang,Qingyu Li,Hechen Liu,Haozhi Wang","doi":"10.1039/d6ta06353e","DOIUrl":"https://doi.org/10.1039/d6ta06353e","url":null,"abstract":"Alkaline aqueous zinc-based batteries hold great potential for large-scale energy storage, but their commercialization is hindered by dendrite growth and hydrogen evolution side reaction on the zinc electrode. In this study, a multiscale interface regulation strategy is developed to stabilize the zinc electrode by introducing trace amounts of NaFSI into the electrolyte. Leveraging its pronounced chaotropic effect, FSI− optimizes the coordination structure of Zn(OH)42− to homogenize ion flux while preferentially adsorbing onto the inner Helmholtz layer and decomposing to form an in situ ZnS/ZnF2 interfacial phase. This interface layer synergistically suppresses side reactions and guides uniform deposition through physical barrier effects and three-dimensional confined growth. Consequently, the zinc symmetric cell exhibits prolonged lifespan for over 520 hours at 17 mA cm−2/17 mAh cm−2. The 1 Ah pouch cell with an ultra-low N/P ratio of 1 delivers a long cycling life for over 600 hours at 1.3 A (~34 mA cm−2) and a 52% depth of discharge; and the 5 Ah cell stably cycles for over 800 hours under a high current density of 6 A (~83 mA cm−2), highlighting its promising prospects for practical application.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067313","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":"Accelerating the Discovery of MOF Photocatalysts for CO 2 Mitigation via Interpretable Machine Learning and Molecular Fingerprinting","authors":"Ruting Huang,Fan Wen,Weihao Pan,Xiaojian Chen,Guoqiang Zhang,Yi Yang,Shuai Huang,Xiaohui Wang,Ying Yu","doi":"10.1039/d6ta05367j","DOIUrl":"https://doi.org/10.1039/d6ta05367j","url":null,"abstract":"The escalating CO2 emissions necessitate efficient photocatalysts for carbon reduction. Metal-organic frameworks (MOFs) are promising, but traditional trial-and-error design is highly resource-intensive. This study introduces an interpretable machine learning (ML) framework to predict and optimize the photocatalytic CO2 reduction performance of MOFs. Based on a comprehensive dataset of 368 samples, we developed four ML models, identifying CatBoost as the most accurate (RMSE = 0.66). Shapley Additive Explanations (SHAP) and Partial Dependence Plots (PDP) revealed that composite mass percentage, bandgap, and catalyst concentration primarily dictate catalytic efficiency. Furthermore, extended-connectivity fingerprints (ECFPs) provided complementary local structural information, revealing nitrogen-rich and C=C-containing molecular environments captured by the model. The predictive performance of the model was experimentally evaluated using ten MOF samples, yielding an R2 of 0.794. This data-driven approach significantly reduces energy and material waste in catalyst development, providing a robust, environmentally friendly paradigm for accelerating the design of high-performance materials for CO2 mitigation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"15 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067310","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":"Solvent-solvent dipole engineering of a low-concentration electrolyte for high-performance wide-temperature sodium-ion batteries","authors":"Xiaolong Cai,Jinhan Teng,Yuxiao Gao,Feixue Luo,Sicheng Liu,Xin Tang,Xinyu Chen,Yuhua Chen,Hao Hou,Jing Li","doi":"10.1039/d6ta05645h","DOIUrl":"https://doi.org/10.1039/d6ta05645h","url":null,"abstract":"Low-concentration electrolytes represent a promising direction for sodium-ion batteries by significantly reducing salt consumption and formulation cost. However, their limited low-temperature conductivity and high-temperature interfacial stability have so far precluded operation across the full wide-temperature spectrum. In this work, we demonstrate that dipole-dipole interactions, mediated by the fluorinated co-solvent 1,1,2,2,3,3-tetrafluoropropyl ether (TTE), provide a molecularlevel strategy to reorganise the solvation structure of a 0.6 M NaPF 6 /PC/DEC electrolyte, enabling stable operation across an exceptional temperature range of -40 to 70 ℃. Spectroscopic and theoretical investigations decipher the Fδ --Hδ + coupling between TTE and both PC and DEC, which weakens Na + -solvent coordination, enriches the solvation sheath with PF 6 -anions, and facilitates inorganic-rich electrode-electrolyte interphases. Consequently, Na 4 Fe 3 (PO 4 ) 2 P 2 O 7 ||hard carbon full cells exhibit stable cycling throughout this entire range, and a 25 Ah pouch cell retains 95.78% capacity after 1300 cycles. This work provides the first validation of a lowconcentration electrolyte for wide-temperature sodium-ion batteries, establishing dipole-dipole solvation engineering as a transferable design principle for nextgeneration energy storage materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067311","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":"Intrachain and Interchain Electrical-Thermal Transport Regulation Enabled by Covalent UiO-66/Polyimide Interfaces for High-Temperature Dielectric Energy Storage","authors":"Qinyun Yu,Qixiong Zhang,Rujian Zhao,Jiujun Zhu,Renlu Han,Yafei Hou,Jing Cuan,Weiping Li","doi":"10.1039/d6ta05827b","DOIUrl":"https://doi.org/10.1039/d6ta05827b","url":null,"abstract":"Polymer dielectric capacitors are widely used, but their performance deteriorates under elevated temperature due to the enhanced electro-thermal coupling, including the intensified charge injection, thermally activated carrier transport and inefficient heat dissipation. Conventional polymer-inorganic composites are typically prepared via physical blending, where weak interfacial interactions and structural discontinuity limit effective regulation of charge and heat transport. Herein, x wt.% UiO-66-NH 2 /polyimide (PI) composites are constructed via an interfacial covalent integration strategy, in which UiO-66-NH 2 reacts in situ with carboxyl-containing poly (amic acid) precursors during thermal imidization, forming a covalently integrated and structurally continuous interface. Both experimental and simulation results demonstrate that the covalently integrated interface effectively suppresses charge migration and mitigates space charge accumulation, while simultaneously promoting more uniform heat dissipation throughout the composite. The incorporation of UiO-66-NH 2 therefore improves the electrical performance and thermal stability of the composite at elevated temperatures. Accordingly, the 0.25 wt.% UiO-66-NH 2 /PI composite delivers an energy density of 4.2 J•cm -3 at 150 °C, 3.0 J•cm -3 at 200 °C, and 2.4 J•cm -3 at 250 °C, with η >90%. This work demonstrates that covalently integrated interfaces provide an effective strategy for regulating charge transport and heat dissipation in polymer composites, offering a practical route toward reliable high-temperature energy storage.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"30 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067312","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":"Low-coercive-field multiphase engineering unlocks efficient cryogenic energy harvesting in lead-free piezoelectric ceramics","authors":"Jun Zhao,Wenlong Xu,Kaibiao Xi,Mupeng Zheng,Yudong Hou","doi":"10.1039/d6ta04192b","DOIUrl":"https://doi.org/10.1039/d6ta04192b","url":null,"abstract":"Sub-zero environments pose challenges for self-powered wireless sensor networks (WSNs), where piezoelectric materials, despite being promising for energy harvesting, suffer from significant performance degradation due to suppressed domain dynamics at low temperatures. Here, a synergistic strategy combining multiphase coexistence and a low coercive field is proposed to enhance polarization switching under low-temperature conditions. Three representative lead-free systems, BiFeO3–BaTiO3 (BFBT), (K, Na) (Nb, Sb)O3–(Bi, Na)ZrO3 (KNNS–BNZ) and (Ba, Ca) (Ti, Zr)O3 (BCZT), are systematically studied. Among them, BCZT, benefiting from rhombohedral–orthorhombic–tetragonal (R–O–T) multiphase coexistence, a low coercive field (3.5 kV cm−1) and rich domain configurations with nanodomain features, reduces the energy barrier for domain switching and maintains high domain activity at −40 °C, leading to superior piezoelectric performance (489 pC/N). As a result, the corresponding piezoelectric energy harvester (PEH) delivers an output power density of 124 µW cm−3 at −40 °C, which is substantially higher than that of the KNNS–BNZ PEH (∼14 µW cm−3), while the BFBT PEH shows nearly no effective power output under the same conditions. This work provides an effective design strategy for piezoelectric materials and supports the development of WSNs in harsh environments.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"31 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067403","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 synergistic structure-directing strategy to construct a Cu-TCPP NSs/TiCT NSs fiber supercapacitor with good energy density and high flexibility","authors":"Xiaojie Xu,Xiumei Chen,Qi Li,Xuexia He,Jie Sun,Ruibin Jiang,Zhibin Lei,Kui Zhao,Zong-Huai Liu","doi":"10.1039/d6ta05486b","DOIUrl":"https://doi.org/10.1039/d6ta05486b","url":null,"abstract":"Using Ti3C2Tx nanosheets (NSs) as a nematic birefringence agent, a structure-directing template and Cu-TCPP NSs as assembling units with high capacitance, a synergistic structure-directing strategy was developed to prepare Cu-TCPP NSs/Ti3C2Tx NSs hybrid fiber electrodes with good flexibility and superior electrochemical performance by wet spinning in a coagulated bath of acetic acid. Ti3C2Tx NSs with liquid-crystalline behavior could structure-template-orient Cu-TCPP NSs and effectively induce their high alignment to construct an ordered and flexible one-dimensional fibrous architecture. The interfacial hydrogen-bond interaction between –OH groups on Ti3C2Tx NSs and –COOH groups on Cu-TCPP NSs provided appropriate ion diffusion space and enhanced the tensile strength of the obtained fiber. The optimizable Cu4M6 fiber electrode exhibited a high specific capacitance of 655 F cm−3, with 86.8% capacitance retention after 10 000 cycles and a tensile strength of 24 MPa. The assembled Cu4M6 symmetric fiber supercapacitor delivered an energy density of 16.3 mWh cm−3 and capacitance retention of 94% after 500 bending cycles from 0° to 180°. This synergistic structure-directing strategy provides a new approach for preparing a MOF-based fiber electrode with an optimizable balance between flexibility and capacitance. This research could expand the application of MOF-based materials in flexible energy storage.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"58 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067408","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":"Synergistic structural and functional design of thiolated ZIF nanosheets for accelerated and selective uranium extraction","authors":"Wen Yao,Siyuan Yu,Juanjuan Yang,Shuangyi Zhu,Tianxin Li,Hongwen Liu,Jie Yang,Xinrong Guo","doi":"10.1039/d6ta05398j","DOIUrl":"https://doi.org/10.1039/d6ta05398j","url":null,"abstract":"Efficient and selective uranium extraction from seawater is a significant challenge in energy utilization. Conventional materials often exhibit poor performance due to limited mass transfer and a lack of specific recognition sites. Here, a rational design strategy with synergistic structural and functional features was proposed, and a thiolated material (ZIF-A-SH5) with a hierarchical nanosheet structure was successfully prepared for uranium capture. Its unique self-assembled nanosheet structure provided superior mass transfer channels, effectively overcoming the diffusion bottlenecks associated with traditional ZIFs. Additionally, the grafted –SH groups offered high-affinity sites for uranium. The results demonstrated that ZIF-A-SH5 achieved a theoretical maximum adsorption capacity of up to 94.42 mg g−1, ultra-fast reaction kinetics, excellent adsorption selectivity in complex ionic matrices, and stable recyclability. X-ray photoelectron spectroscopy and density functional theory calculations revealed that its superior performance resulted from a unique coordination mechanism: strong S–U coordination interactions formed between thiol groups and uranyl ions. Furthermore, the material's remarkable selectivity against competing ions was quantitatively rationalized by a significant thermodynamic preference (ΔE = 0.53 eV) for uranium, confirming a highly covalent and selective S/N synergistic coordination pathway. This work presents a promising adsorbent for practical uranium extraction from seawater and provides important theoretical guidance for designing advanced functional materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067407","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":"Magnetic proximity-induced spin injection suppresses singlet oxygen for durable water electrolysis","authors":"Lin Wu,Yuhang Lei,Lixiang Li,Han Zhang,Lin Tao,Hongwei Zhao,Qingdong Li,Xueyuan Zhang,Chengguo Sun,Dongying Ju,Baigang An","doi":"10.1039/d6ta04728a","DOIUrl":"https://doi.org/10.1039/d6ta04728a","url":null,"abstract":"While spin polarization accelerates the oxygen evolution reaction (OER) kinetics, the parasitic generation of singlet oxygen (1O2) triggers oxidative degradation of catalytic active sites, limiting the lifespan of water electrolysis. Herein, we design a 1D directionally ordered CoFeB/CoFe-LDH (CFB/LDH) heterostructure to realize spin-injection via the magnetic proximity effect (MPE). Through exchange coupling, the ferromagnetic CFB core breaks the local spin symmetry of the ultrathin LDH shell. Under a magnetic field (MF), this MPE-induced spin alignment dynamically steers the OER toward the lattice oxygen mechanism. By enforcing spin conservation, the parallel-aligned heterostructure promotes effective interfacial spin filtering, which suppresses the 1O2 pathway by 6% h−1 in favor of ground-state triplet oxygen. Consequently, the MPE-driven catalyst achieves a 36 mV reduction in OER overpotential. When integrated into a practical anion-exchange membrane water electrolyzer, it delivers a cell voltage of 1.78 V at 500 mA cm−2, representing a 40 mV reduction compared to the cell without MF, and sustains stable operation for 200 h with a negligible potential increase. This work establishes MPE-induced spin injection as a materials-design strategy for coupling interfacial spin polarization with durable and efficient water electrolysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"11 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067409","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":"Interfacial ion–electron coupling enables synergistic solar evaporation, hydrovoltaic electricity generation, and photocatalytic degradation","authors":"Chunhui Shi,Xiaoming Cao,Peng Kong,Fengqin Tang,Yunxiang Xiao,Ke Tian,Shiyu Jia,Beibei Sun,Weiliang Tian,Libing Hu","doi":"10.1039/d6ta06132j","DOIUrl":"https://doi.org/10.1039/d6ta06132j","url":null,"abstract":"Solar-driven systems capable of simultaneously producing freshwater, removing pollutants, and generating energy offer a promising solution to interconnected water-energy-environment challenges. However, the interplay between ion transport and electron transfer in multifunctional platforms remains poorly understood, hindering the rational design of integrated systems. Herein, we developed a vermiculite (VM)-supported CNTs/MoS2 heterostructured membrane (VM/CNTs@MoS2), which demonstrated that interfacial ion–electron coupling governed its solar evaporation, photocatalytic, and hydrovoltaic behaviors. X-ray photoelectron spectroscopy and density functional theory calculations revealed spontaneous charge redistribution at the CNTs/MoS2 heterointerface, leading to the formation of a built-in electric field (BIEF) that promoted charge separation and electron transport. Coupled with directional ion migration through negatively charged VM nanochannels, this electronically coupled structure established an efficient ion–electron transport pathway. As a result, the VM/CNTs@MoS2 membrane achieved a solar evaporation rate of 2.44 kg m−2 h−1 with an energy conversion efficiency of 92.62% and simultaneously generated a stable hydrovoltaic output with an open-circuit voltage of 0.40 V and a maximum power density of 370 mW m−2 under one-sun illumination, while retaining excellent salt tolerance and operational stability. Moreover, the enhanced interfacial charge utilization enabled MoS2 to generate hydroxyl radicals favorable for 91.2% degradation of methylene blue within 8 h. Mechanistic investigations revealed that evaporation-induced ionic flux and interfacial electron transport are dynamically coupled through the engineered heterointerface. The dynamic coupling between these ionic and electronic processes served as the common origin of the enhanced evaporation, photocatalytic activity, and electricity generation. This work establishes interfacial ion–electron coupling as an effective strategy for integrating water purification, environmental remediation, and energy generation within a single platform, providing new insights into the design of next-generation solar-driven multifunctional systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"57 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067406","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":"Insights into the MoS Lithium-Ion Battery Lithiation Mechanism via Big Data Electrochemical Analysis","authors":"Alexandar Dimitrov Marinov,Ami R. Shah,Christopher A Howard,Patrick Cullen","doi":"10.1039/d6ta03464k","DOIUrl":"https://doi.org/10.1039/d6ta03464k","url":null,"abstract":"Molybdenum disulfide (MoS2) is a potential alternative to the commercial graphite anode in lithium-ion batteries (LIBs) due to its higher theoretical capacity (670 mAh/g) and natural earth abundance. However, the deep discharge potential range (3.00 – 0.01 V) enabling MoS2 high specific capacities is highly debated and suffers from a rapid degradation process (< 40 cycles). To investigate the MoS2 deep lithiation mechanism, long-term electrochemical testing, restrictive potential ranges after an initial deep discharge, and in situ electrochemical impedance spectroscopy (EIS) were applied. Electrochemical analysis reveals that the three cathodic reactions (labelled G, H, and I) are either parallel or series-independent, forming reversible redox couples with the single anodic peak (W). The inclusion of each additional cathodic peak increases cell capacity but accelerates capacity decay. As the redox peaks responsible for the high initial capacities vanish, we verify that capacity is stored entirely through capacitance in the long term (> 40 cycles). Our electrochemical analysis highlights that current MoS2 lithiation mechanism proposals are unable to accurately describe the phenomena observed when restricting the potential range of MoS2 after deep lithiation. Therefore, we propose a set of three electrochemical conditions that must be justified by any lithiation mechanism hypothesis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"5 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067398","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}