Journal of Materials Chemistry A最新文献

{"title":"Na-ion storage in hard carbon: From accurate structural models to mechanistic insights via machine learning aided molecular dynamics","authors":"Simone Piccinin,Che-an CL Lin,Huu Duc Luong,Ryoma Sasaki,Kei Kubota,Stefano Fabris,Shinichi Komaba,Yoshitaka Tateyama","doi":"10.1039/d6ta08107j","DOIUrl":"https://doi.org/10.1039/d6ta08107j","url":null,"abstract":"As the most common anode material for Na-ion batteries, hard carbon has been the subject of extensive research aimed at unraveling its storage mechanisms and structure-property correlations. In this work, we employ atomic-scale simulations to investigate the complex structural relationships governing its electrochemical performance. To this end, we developed a machine-learning interatomic potential and generated structural models of hard carbon through a novel protocol, obtaining excellent agreement with experimental pair distribution functions and X-ray diffraction patterns. By simulating the open circuit voltage profiles, we directly correlated the maximum specific capacity and the voltage profile regions with the material's nanoporosity. Our results reveal that while the high-voltage sloping region is remarkably consistent across different densities, the low-voltage plateau region is strongly dependent on the nanopore size. We demonstrate an approximately linear correlation between maximum specific capacity and both density and specific pore volume, suggesting that increasing the specific pore volume up to the optimal value previously proposed in the literature is critical for enhancing capacity. These findings provide a rational framework for the design of high-capacity hard carbon anodes by unraveling how pore architecture influences the electrochemical properties of this material.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368193","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":"Polyaniline-hybridized quantum-confined 1D lepidocrocite titania for ultra-high-energy supercapacitors","authors":"Sukanya Maity,Joseph Halim,Ali Saffar Shamshirgar,Risha Achaiah Iythichanda,Per O. Å. Persson,Michel W. Barsoum,Johanna Rosen","doi":"10.1039/d6ta05686e","DOIUrl":"https://doi.org/10.1039/d6ta05686e","url":null,"abstract":"High-energy capacitors have garnered significant interest due to their dual ability to store energy and deliver high power, influenced by the properties of their electrode materials. Herein, we report a unique composite structure created through in situ polymerization of polyaniline (PANI) in the presence of one-dimensional lepidocrocite (1DL) titania nanofilaments (NFs). The hierarchical 1DL NF structures allow direct and fast ion transport, enhancing both capacity and stability when combined with PANI. The resultant composite (PANI : 1DLs in a 2 : 1 wt ratio) exhibits a specific capacity of 377 mA h g−1 at 0.5 Ag−1, with high mass loading (∼5 mg cm−2). The composite's performance in a symmetric cell configuration demonstrates a specific energy of 154 Wh kg−1 at 0.5 A g−1, which is the highest specific energy among other reported TiO2-based supercapacitor electrodes over a wide voltage window of 3.5 V. A peak specific power of 17 kW kg−1 was measured while maintaining a specific energy of 31Wh kg−1. After 10 000 charge–discharge cycles, the cell retained ∼56% of its initial capacity with 94% coulombic efficiency. To enhance cell stability and reduce self-discharge, an asymmetric arrangement with activated carbon improved voltage retention, resulting in a 29.7% open-circuit potential retention after 24 h and 80% capacitance retention after post-cycling. The synthesis method is inexpensive, sustainable, and potentially scalable, highlighting the potential for high-energy supercapacitors.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"75 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368202","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":"Hollow carbon nanocages with mixed-phase interfaces for durable aqueous zinc–iodine batteries","authors":"Jiahui Ye,Wen Tian,Zeming Li,Weili Yu,Linfeng Jiang,Haohui Dong,Junyi Ji","doi":"10.1039/d6ta03959f","DOIUrl":"https://doi.org/10.1039/d6ta03959f","url":null,"abstract":"Aqueous zinc–iodine (Zn–I2) batteries hold great promise for grid-scale energy storage owing to abundant Zn/I resources, inherent safety, and high theoretical capacity. Nevertheless, their practical application is severely hindered by the polyiodide shuttle effect, caused by the weak iodine confinement and sluggish catalytic conversion kinetics on conventional carbon hosts. Herein, hollow carbon nanocages (CNZ-NC) bearing crystalline/amorphous hybrid phase interfaces are constructed via spatially gradient carbonization of the epitaxially grown core–shell ZIF precursors. The Co sites enriched in the shell layer not only facilitate the graphitization of the carbon matrix, but also serve as catalytic centers to accelerate reversible conversion of iodine active species. Meanwhile, volatilization of Zn from the core region drives the formation of amorphous carbon domains with an appropriate pore size distribution. The hybrid-phase hollow structure significantly improves the interfacial polarity of carbon substrates, realizing strong anchoring toward iodine species. Benefiting from the synergistic merits of robust adsorption and catalytic regulation, the CNZ-NC@I2 cathode exhibits outstanding cycling stability in both long-term continuous cycling and intermittent cycling measurements. In situ spectroscopy confirms effective suppression of polyiodide shuttling, while the post-cycle zinc anode remains flat and corrosion-free. This work provides novel insights into the design of carbon hosts with robust anchoring and reversible catalytic interfaces, as well as their practical applications in halogen-based battery systems.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"64 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368206","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":"Stabilizing Cerium Dioxide Composite Electrodes with Nitrogen-Doped Carbon Nanofibers for Rapid TiO2+/Ti3+ redox kinetics in Ti-Ce redox flow batteries","authors":"Shangwan Fu,Chengxu Zhang,Jiangpeng Lei,Ziming Guo,Yangyang Xie,Yaobin Lai,Jian Li,Xudong Liu,Dongyue Xie,Xuxia Zhang,Peng Guan,Hui Zhang,Tao Qi","doi":"10.1039/d6ta07536c","DOIUrl":"https://doi.org/10.1039/d6ta07536c","url":null,"abstract":"Redox flow batteries (RFBs) are attractive for large-scale energy storage because their power and capacity can be scaled independently, yet the electrode materials often suffer from limited catalytic activity. For Ti-Ce redox flow batteries (Ti-Ce RFBs), the sluggish kinetics of the TiO2+/Ti3+ redox couple further constrain performance. Here we constructed a nitrogen-doped carbon nanofiber (N-CNF) network on the surface of carbon felt by combining hydrothermal synthesis, and successfully confined cerium dioxide (CeO2) nanoparticles within this network. Material characterization confirms that N-CNF markedly improves the hydrophilicity and conductivity of the carbon felt. Working synergistically with CeO2, it substantially increases the density of electroactive sites while suppressing CeO2 dissolution and carbon felt corrosion in strongly acidic media through interfacial interactions between nitrogen atoms and CeO2. Electrochemical testing reveals that the modified electrode delivers a larger active surface area, faster diffusion, and lower charge-transfer impedance. At a current density of 50 mA cm⁻², the Ti-Ce RFB based on CF@CeO2@N-CNF exhibited a discharge capacity decay rate of only 0.03% per cycle and operated stably for more than 2040 cycles. After electrolyte replacement, the battery performance recovered to 90% of its initial state. By contrast, the electrode modified with CeO2 alone suffered a sharp capacity drop after 490 cycles, with near-complete loss of Ce from the electrode surface and significant corrosion. This study demonstrates that the composite modification strategy synergistically enhances both the electrochemical activity and the structural stability of carbon felt electrodes, offering a new approach for designing high-performance, long-lifetime Ti-Ce RFBs","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"37 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368194","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":"HydroBERT-MTL: Deep Semantic Representation of Incomplete Tabular Data for Hydrogen Uptake Prediction","authors":"Rui Luo,Ziliang Zhang,guoxiao xu,Hongli Li,Xiangbo Lin,Rulong Liu,Jinghua Liu,Xinwei Dong","doi":"10.1039/d6ta07972e","DOIUrl":"https://doi.org/10.1039/d6ta07972e","url":null,"abstract":"Predicting hydrogen uptake in porous carbons is critical for adsorbent screening, yet literature datasets frequently lack complete pore-structure descriptors. We introduce HydroBERT-MTL, a missingness-aware text-tabular multi-task framework that overcomes this by combining SciBERT-based text prompts, mask-aware numerical features, and masked descriptor reconstruction. Tested on a curated dataset using controlled masking to simulate incomplete inputs, HydroBERT-MTL achieved superior accuracy (R2 = 0.904, RMSE = 0.798 wt%) with complete data, compared with 0.690–0.853 for Ridge, RF, and XGBoost. Crucially, under 100% structural masking, it maintained robust performance (R2 = 0.863, RMSE = 0.953 wt%), heavily outperforming conventional mean-filled baselines. Ablation and SHAP analyses confirm that text-tabular fusion, dynamic masking and auxiliary reconstruction drive this stability. Notably, under full structural masking, the reconstruction mechanism enables the model to leverage remaining elemental descriptors as compensatory statistical information. These results highlight HydroBERT-MTL as a highly resilient approach for materials prediction under severe data missingness.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"16 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368192","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":"Bridging Transport Properties Across Length Scales via Local Ionic Current Distributions in Solid Electrolytes","authors":"Mariia Ivonina,Tomofumi Tada","doi":"10.1039/d6ta06030g","DOIUrl":"https://doi.org/10.1039/d6ta06030g","url":null,"abstract":"Predicting ionic transport across length scales remains one of the challenges in the computational design of solid electrolytes. In this work, we introduce a mesoscale data driven strategy to predict the ionic current density of large 8 mol % yttria-stabilized zirconia (8YSZ) superblocks from the statistics of kinetic Monte Carlo (KMC) time series of smaller 8YSZ sub-blocks, without explicit atomistic structural descriptors.For each sub-block containing 6000 ion sites, we capture the discretized distribution of KMC ionic current density by counting the passing oxygen vacancies through a plane perpendicular to the ion flux per time interval. The resulting current density distribution characteristics, including the mean value and kernel density estimation (KDE) profile, are used as descriptors to predict the mean ionic current densities of four-and sixteen-fold larger superblocks assembled from identical sub-blocks (homogeneous) and from different sub-blocks (heterogeneous). We benchmark kernel ridge regression (KRR) using KDE profile descriptors against linear ridge regression (LRR) using mean value descriptors and find that KRR yields consistently higher accuracy, especially for heterogeneous superblocks, where interfacial Y configurations between non-identical sub-blocks lead to non-additive ionic transport. Across a dataset of 1140 8YSZ superblocks, the results demonstrate that KDE profiles encode information about local ionic transport, enabling accurate predictions at larger length scales. Although KMC current fluctuations may appear as stochastic noise, this approach utilizes them as transferable descriptors for multiscale prediction of ionic transport in complex solid electrolytes. This concept may also be extended to other stochastic simulation methods and advanced high-resolution experimental current detection techniques.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368189","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":"Nucleation, orientation, and optical properties of ultrathin iron oxide grown by atomic layer deposition","authors":"Alex B. F. Martinson,Ashley R. Bielinski,Asare Dua","doi":"10.1039/d6ta07010h","DOIUrl":"https://doi.org/10.1039/d6ta07010h","url":null,"abstract":"The optoelectronic properties of iron oxide thin films vary widely across metal oxidation states, compositional space, and crystallinity. Ultrathin films of hematite (α-Fe2O3), a visible light absorbing semiconductor in the bulk, are particularly sensitive to nucleation, orientation, crystallinity, and interfacial effects. We demonstrate a templated atomic layer deposition (ALD) process at moderate temperature (200 °C) to produce oriented and crystalline hematite with effective thickness as small as 2 nm. While alternating exposure to ferrocene and ozone typically results in X-ray amorphous or weakly polycrystalline ultrathin Fe2O3 films, we reveal processes conditions under which multiple sapphire substrate orientations template the ALD of crystalline ultrathin hematite with significant nucleation delay. The complex refractive indices of templated ALD Fe2O3 are found to closely resemble those of birefringent hematite single crystals, the reported indices for which we extend deep into the UV using variable angle spectroscopic ellipsometry. The templating effect is observed through ultrathin ALD Ga2O3 underlayers, expanding the range of ultrathin Fe2O3 interface materials. The deposition of crystalline, oriented ultrathin α-Fe2O3 will enable detailed study of the optoelectronic properties of hematite as a function of interfacial quality and surface defects.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"32 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368205","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":"Revealing hidden patterns and HOMO-LUMO gap prediction on a curated phthalocyanine-based HER electrocatalyst database using machine learning models","authors":"Sachidananda Nayak,Selvakumar Karuthapandi","doi":"10.1039/d6ta06834k","DOIUrl":"https://doi.org/10.1039/d6ta06834k","url":null,"abstract":"The development of efficient, low-cost, and earth-abundant electrocatalysts for the hydrogen evolution reaction (HER) is essential for sustainable green hydrogen production and the transition toward a carbon-neutral energy economy. Although phthalocyanine-based molecular electrocatalysts have shown considerable promise for HER, the absence of a standardized experimental database and experimentally accessible descriptors has hindered machine learning-assisted catalyst screening and rational catalyst design. Herein, we developed PhthaloHERDB26, a manually curated database comprising 137 aqueous phthalocyanine-based molecular catalyst entries systematically extracted from the literature. We further established a machine learning framework to identify experimentally accessible descriptors governing HER activity, accelerate catalyst screening, and model prediction. The database integrates 32 experimentally derived descriptors encompassing electrochemical, spectroscopic, structural parameters, including overpotential (OP), Tafel slope (TS), Rct, Cdl, Raman, and UV-Vis spectroscopic characteristics. A comprehensive machine learning workflow involving feature importance analysis, hyperparameter optimisation, supervised learning (Decision Tree, Support Vector Machine, and Naïve Bayes), and unsupervised learning (principal component analysis and K-means clustering) was employed to identify the descriptors governing HER activity and screen promising catalysts. Feature importance analysis identified Rct and Cdl as the dominant electrochemical descriptors to OP, while the HOMO-LUMO gap emerged as the most informative experimentally accessible spectroscopic descriptors. K-means clustering further shortlisted 27 high-performance catalyst entries into distinct performance groups, enabling efficient prioritization of promising phthalocyanine molecular electrocatalysts. Furthermore, an NN-based regression model successfully predicted the HOMO-LUMO gap from experimentally accessible electrochemical descriptors, yielding R2/RMSE values of 0.76/0.052 eV for the training set and 0.90/0.023 eV for the validation set. The proposed data-driven framework provides a practical strategy for accelerating catalyst discovery, reducing experimental effort, and guiding the rational design of high-performance molecular electrocatalysts for sustainable hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"29 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360574","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":"Single-Atom Pd/TiO2 Cooperative Catalyst for Selective Oxidative Upcycling of Polyester Waste into Biodegradable Monomers","authors":"Jingtao Zhou,Yifei Liang,Rui Shi,Lei Kang,Fulai Liu,Qijun Zhang,Yong Chen","doi":"10.1039/d6ta06941j","DOIUrl":"https://doi.org/10.1039/d6ta06941j","url":null,"abstract":"Catalytic conversion of polyethylene terephthalate (PET) waste into biodegradable plastic monomers, terephthalic acid (TPA) and glycolic acid (GA), has emerged as a compelling strategy toward sustainable plastic valorization. Conventional two-step electrocatalytic methods suffer from low production efficiency, while thermocatalytic systems exhibit insufficient product selectivity and rapid catalyst deactivation. Herein, we develop a single-site Pd-loaded TiO2 catalyst (Pd1/TiO2) for one-pot thermo-oxidative conversion of PET into TPA and GA. This cooperative catalyst concurrently facilitates PET hydrolysis and selective EG oxidation, achieving a GA space-time yield of 0.44 g h -1 with 96.1% selectivity and > 99% TPA yield, while maintaining stability over 10 cycles. Mechanistic studies reveal that monodisperse Pd sites enforce selective atop EG adsorption to form key *CHO-CH2OH intermediates, while Pd-TiO2 electronic interactions weaken carbonyl-species adsorption, suppressing catalyst deactivation. TiO2 incorporation and in situ GA generation further shift hydrolysis equilibrium favorably. Life cycle assessment (LCA) and techno-economic analysis (TEA) confirm the process's environmental sustainability and economic profitability. This work establishes an efficient, durable catalytic strategy for PET upcycling, transforming plastic waste into valuable monomers for a circular economy.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"261 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360575","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":"Fluorine incorporation in Sc-doped barium zirconate: F NMR-based quantitative defect chemistry and transport properties","authors":"Kohei Kato,Mei Asakura,Akihiro Ishii,Itaru Oikawa,Hitoshi Takamura","doi":"10.1039/d6ta05303c","DOIUrl":"https://doi.org/10.1039/d6ta05303c","url":null,"abstract":"In recent years, fluorine substitution at oxygen sites in oxide-based proton conductors has attracted considerable attention as a relatively new approach for enhancing proton conductivity. However, the incorporation behavior of fluorine has not yet been investigated in detail, and the mechanism underlying the reported enhancement remains unclear. In this work, 19F nuclear magnetic resonance (19F NMR) spectroscopy was employed to elucidate the incorporation behavior of fluorine in Sc-doped BaZrO3, and the amount of incorporated fluorine was quantitatively evaluated. The results revealed that fluorine can be incorporated as a charge-compensating species for defects generated by acceptor doping, leading to a reduction in proton concentration and indicating a negative impact on proton conductivity. Therefore, fluorine incorporation as an approach to enhance proton conductivity should be carefully considered. In addition, fluorine incorporation into Sc- and Co-co-doped BaZrO3 was investigated, demonstrating that fluorine incorporation in proton-hole conductors has a positive effect on hole conductivity.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360250","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}