Journal of Materials Chemistry A最新文献

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Interfacial In-N orbital hybridization-induced p-band center shift: modulation of intermediate activation and adsorption for enhanced red-light-driven redox catalysis in crystalline carbon nitride/indium sulfide
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-11 DOI: 10.1039/d6ta07939c
Wanting Wang,Hui Yang,Yueyang Tan,Lihua Wu,Wenqing Yu,Bingwen Li,Xinfang Wang,Jiangwei Wen,Limin Huang,Juan Wang,Woon-Ming Lau,Zongzhao Sun
{"title":"Interfacial In-N orbital hybridization-induced p-band center shift: modulation of intermediate activation and adsorption for enhanced red-light-driven redox catalysis in crystalline carbon nitride/indium sulfide","authors":"Wanting Wang,Hui Yang,Yueyang Tan,Lihua Wu,Wenqing Yu,Bingwen Li,Xinfang Wang,Jiangwei Wen,Limin Huang,Juan Wang,Woon-Ming Lau,Zongzhao Sun","doi":"10.1039/d6ta07939c","DOIUrl":"https://doi.org/10.1039/d6ta07939c","url":null,"abstract":"Traditional polymeric carbon nitride/indium sulfide composites exhibit low crystallinity, weak interfacial coupling and poor red-light utilization, limiting their photocatalytic redox performance. Herein, a one-step KSCN molten-salt in-situ strategy is developed to fabricate high-crystallinity PCN/In2S3 heterojunctions (CCNIS) with covalent In-N interfacial bonds, effectively addressing the deficiencies of conventionally assembled composites. The constructed In-N orbital hybridization upshifts the N p-band center, optimizes oxygen intermediate adsorption and activation, and removes the thermodynamic barrier for O2 reduction. Coupled with the built-in electric field-induced efficient charge separation and extended red-light response, the optimal CCNIS50 achieves prominent and stable photocatalytic H2O2 generation (509.42 mM g -1 h -1 under visible light and 5.47 mM g -1 h -1 under red light). It also enables red-light-driven synthesis of high-value α-trifluoromethyl ketones, demonstrating excellent multifunctional photocatalytic potential. This work reveals the orbital-modulated structure-activity relationship of n-n heterojunctions and provides a universal guideline for the design and preparation of high-efficiency, broad-spectrum carbon nitride-based photocatalysts for energy conversion and organic synthesis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"88 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374930","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}
引用次数: 0
Concurrent regulation of catalytic kinetics and oxygen bubble dynamics strain-coupled interfacial reconstruction of commercial stainless steel felt for ampere-level alkaline water electrolysis 催化动力学与氧泡动力学的同步调控——商业不锈钢毡在安培级碱性电解中的应变耦合界面重构
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta08266a
Greeshma Suresh,Chaehyeon Moon,Mohsin Ali,Si Eun Je,Seok Hwa Jeong,JinHa Shim,Sung Yul Lim,Byung-Hyun Kim,Jin Ho Bang
{"title":"Concurrent regulation of catalytic kinetics and oxygen bubble dynamics strain-coupled interfacial reconstruction of commercial stainless steel felt for ampere-level alkaline water electrolysis","authors":"Greeshma Suresh,Chaehyeon Moon,Mohsin Ali,Si Eun Je,Seok Hwa Jeong,JinHa Shim,Sung Yul Lim,Byung-Hyun Kim,Jin Ho Bang","doi":"10.1039/d6ta08266a","DOIUrl":"https://doi.org/10.1039/d6ta08266a","url":null,"abstract":"Ampere-level alkaline water electrolysis is jointly limited by sluggish oxygen-evolution kinetics and by oxygen-bubble accumulation that blocks active sites—two bottlenecks conventionally addressed by separate strategies. As both originate at the electrode/electrolyte interface, we hypothesize that a single interfacial-reconstruction step reshaping surface chemistry, wettability, and local strain can co-regulate catalytic kinetics and bubble dynamics through one shared lever. We test this hypothesis on commercial 316L stainless-steel felt, whose heterogeneous Fe/Ni/Cr alloy, native Cr-rich passivation, and industrial-grade robustness make it a uniquely non-substitutable model platform. A scalable, one-pot sequential HCl/H2SO4 treatment dissolves the Cr2O3 layer and converts the exposed Fe/Ni domains into an amorphous, hydroxylated Fe/Ni-rich oxide layer harboring heterogeneous tensile/compressive strain. This single reconstruction concurrently produces hydroxyl-rich active sites, Wenzel-regime superhydrophilicity, and a two- to three-fold reduction in bubble departure diameter that is nearly invariant with current density. Density functional theory calculations indicate that localized tensile strain thermodynamically favors surface hydroxylation, providing a plausible link between lattice distortion and the density of hydroxylated sites proposed to act as bubble nucleation centers. The optimized anode delivers accelerated oxygen evolution reaction kinetics together with durable operation at industrially relevant current densities in an anion exchange membrane electrolyzer, establishing strain-coupled interfacial reconstruction as a transferable design principle for earth-abundant gas-evolving anodes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"24 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374977","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}
引用次数: 0
Local transition-metal coordination and lithium site occupancy energetics govern structural evolution in layered NMC cathodes
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta07290a
kun Li,teng li,Lunhua He,Xiaoyong Zhang,Baohua Li,Kun Qian
{"title":"Local transition-metal coordination and lithium site occupancy energetics govern structural evolution in layered NMC cathodes","authors":"kun Li,teng li,Lunhua He,Xiaoyong Zhang,Baohua Li,Kun Qian","doi":"10.1039/d6ta07290a","DOIUrl":"https://doi.org/10.1039/d6ta07290a","url":null,"abstract":"Nickel-rich layered oxides are promising cathodes for high-energy-density lithium-ion batteries, yet their cycling stability remains challenging. Although it is known that bulk Ni content is often correlated with the structural instability, the underlying atomic-scale mechanisms are not fully resolved, particularly how local transition-metal (TM) coordination governs lithium extraction, lattice evolution, and oxygen redox behavior. Here, we adopt a site-energy perspective to re-examine crystal structure evolution and lithium vacancy distribution in layered oxides with 80%, 70%, and 60% Ni in the TM layer. Using neutron powder diffraction, operando X-ray diffraction, and first-principles calculations, we propose a unified framework that incorporates Li-site energy, TM coordination, and oxygen charge. This framework helps understand which lithium ions are preferentially extracted from the lithium layer and where the remaining Li-ions are trapped. These findings reveal that local TM–O coordination is a key descriptor of structural stability, thus enabling the design of cathodes that achieve both high energy density and long-term durability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374927","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}
引用次数: 0
Interfacial Phosphide-Phosphate Engineering in NiCoP-POₓ/Carbon Heterostructures for Efficient Piezoelectric-Driven Self-Charging Asymmetric Supercapacitors 高效压电驱动自充电非对称超级电容器NiCoP-POₓ/碳异质结构界面磷化-磷化工程
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta05900g
T. B. Naveen,Ajay Rakkesh Rajendran
{"title":"Interfacial Phosphide-Phosphate Engineering in NiCoP-POₓ/Carbon Heterostructures for Efficient Piezoelectric-Driven Self-Charging Asymmetric Supercapacitors","authors":"T. B. Naveen,Ajay Rakkesh Rajendran","doi":"10.1039/d6ta05900g","DOIUrl":"https://doi.org/10.1039/d6ta05900g","url":null,"abstract":"The growing demand for portable and wearable electronics calls for energy storage devices integrated with energy harvesters. Self-charging asymmetric supercapacitors (SCASCs) do this with a piezoelectric separator, where the output depends on both an efficient separator and a high-performance, robust cathode. Here, we present a tailored strategy in which a MOF-templated phosphorization pathway yields a NiCoP-POx/C heterostructure cathode (nickel-cobalt phosphide/phosphate anchored on a conductive carbon network), forming a hierarchical architecture that enhances electron transport, active-site accessibility, and interfacial redox kinetics. Owing to the synergistic effects of the MOF-derived carbon framework and the phosphide-phosphate heterointerface, the electrode delivers 1145 F g-1 at 1 A g-1 and retains 87.6% of its capacitance after 10,000 cycling steps. An aqueous asymmetric supercapacitor (ASC) assembled using biomass-derived rGO as the counter electrode demonstrates strong capacitive behaviour and stable cycling, highlighting its suitability for practical device integration. Building on this performance, SCASC is constructed by incorporating a PVDF-2% ZnO piezoelectric separator capable of harvesting mechanical energy. The device autonomously charges to 220 mV within 44 seconds under repeated palm compressions, representing a remarkably rapid charging response compared with typical SCASCs. These results highlight the potential of MOF-derived NiCoP-POx/C heterostructures for energy-dense, rapidly chargeable, and self-sustained power systems tailored for portable and wearable applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"4 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374937","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}
引用次数: 0
Inverse Temperature Crystallization of Metal Halide Perovskite Single Crystals: From Growth Chemistry to Composition Engineering and Optoelectronic Applications 金属卤化物钙钛矿单晶的反温结晶:从生长化学到组成工程及光电应用
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta07680g
Tianqi Zhang,Jiawei Gu,Yu Chen,Yuchen Zhou,Yue Zhao,Zihan Xia,Zhong Chen,Shuli Wang,Yue Lin,Qingsen Zeng
{"title":"Inverse Temperature Crystallization of Metal Halide Perovskite Single Crystals: From Growth Chemistry to Composition Engineering and Optoelectronic Applications","authors":"Tianqi Zhang,Jiawei Gu,Yu Chen,Yuchen Zhou,Yue Zhao,Zihan Xia,Zhong Chen,Shuli Wang,Yue Lin,Qingsen Zeng","doi":"10.1039/d6ta07680g","DOIUrl":"https://doi.org/10.1039/d6ta07680g","url":null,"abstract":"Metal halide perovskite single crystals (MHP-SCs) are attractive platforms for high-performance optoelectronic and radiation-detection devices owing to their long-range crystallographic order, low defect densities, long carrier diffusion lengths, and highly tunable electronic structures. Inverse temperature crystallization (ITC), which exploits the inverse-solubility behavior of selected precursor–solvent systems, has emerged as a powerful solution-based approach for the rapid and controllable growth of high-quality MHP-SCs. This review provides a comprehensive overview of the materials chemistry of ITC-grown MHP-SCs, connecting crystallization control, composition engineering, and device functionality. We first discuss the thermodynamic and kinetic principles underlying ITC, with particular emphasis on supersaturation, nucleation, solute transport, and interfacial growth, as well as advanced strategies involving space confinement, seed-assisted growth, additive engineering, in situ monitoring, and sustainable solvent systems. We then examine A-, B-, and X-site composition engineering and establish how site-specific regulation influences lattice stability, defect chemistry, ion migration, electronic structure, and carrier transport. These growth- and composition-dependent properties are further correlated with device performance in solar cells, photodetectors, high-energy radiation detectors, light-emitting diodes, and lasers. Finally, remaining challenges and future opportunities are discussed, including mechanistic understanding of inverse crystallization, scalable and reproducible growth, sustainable solvent design, suppression of ion migration, and integration of SCs into practical devices. By linking solution chemistry and crystallization kinetics with composition–structure–property relationships, this review provides a framework for the rational design and controlled growth of high-quality MHP-SCs for next-generation optoelectronic and radiation-detection technologies.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374923","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}
引用次数: 0
Facet-Engineered CoWO4/BiVO4 S-scheme Heterojunction for Exceptional Bifunctional Photocatalytic H2 Evolution and Tetracycline Degradation 表面工程CoWO4/BiVO4 S-scheme异质结用于特殊双功能光催化H2演化和四环素降解
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta07429d
Zhenglong Shen,Meng Wang,Meiting Song,Yanxia Zhao,Yahui Zhang,Kang Zhang,Xiaoyu Chai,Yuhang Wu
{"title":"Facet-Engineered CoWO4/BiVO4 S-scheme Heterojunction for Exceptional Bifunctional Photocatalytic H2 Evolution and Tetracycline Degradation","authors":"Zhenglong Shen,Meng Wang,Meiting Song,Yanxia Zhao,Yahui Zhang,Kang Zhang,Xiaoyu Chai,Yuhang Wu","doi":"10.1039/d6ta07429d","DOIUrl":"https://doi.org/10.1039/d6ta07429d","url":null,"abstract":"Photocatalytic hydrogen evolution and organic contaminant degradation are attractive strategies for addressing the two fundamental issues of the energy crisis and environmental pollution. Here, we design a facet selective S-scheme heterostructure by in-situ decoration of decahedral BiVO4 crystals with exposed (010) facets using CoWO4 nanoparticles. Under simulated solar irradiation, the optimized CoWO4/BiVO4 composite delivers a H2 evolution amount of 1144.36 µmol·g-1 after 5 h in a TEOA aqueous solution, which is 25.67 times that of pristine CoWO4 under identical conditions. In a separate test, the same composite achieves 99.8% tetracycline degradation within 25 min in a PMS containing solution. The electrochemical catalytic effect induced by the integration of photocatalysis and electrocatalysis is achieved when the CoWO4/BiVO4 was applied under photoelectrochemical reaction conditions, where a cumulative hydrogen production of 6713.77 µmol·g-1 was obtained over 5 h.The enhanced photoelectrochemical and photocatalytic performance are caused by the facet-controlled deposition of CoWO4 on the electron accumulating (010) facet of the BiVO4, thus generating the close-knit integrated interface for the efficient charge transfer. According to density functional theory calculations, in-situ X-ray photoelectron spectroscopy and EPR characterization, the S-scheme charge transfer behavior is found to be driven by the internal electric field. The resulting charge transfer mode favors the efficient separation of the photogenerated carriers to different components while preserving the robust redox ability of both components. This construction strategy highlights a practical avenue to the rational design of bifunctional photocatalysts with enhanced photocatalytic efficiency for the dual purpose of clean energy generation and environmental remediation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"30 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374924","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}
引用次数: 0
Composition-Driven Electronic Structure Modulation in Dy-Modified Nanocatalysts for Efficient Bifunctional Alkaline Water Electrolysis 高效双功能碱水电解中dy修饰纳米催化剂组成驱动的电子结构调制
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta07316f
Anto Priyanka E,Sreenivasan Nagappan,Alloffy Mary A,Vidya Ravindran,J. Judith Vijaya,Subrata Kundu
{"title":"Composition-Driven Electronic Structure Modulation in Dy-Modified Nanocatalysts for Efficient Bifunctional Alkaline Water Electrolysis","authors":"Anto Priyanka E,Sreenivasan Nagappan,Alloffy Mary A,Vidya Ravindran,J. Judith Vijaya,Subrata Kundu","doi":"10.1039/d6ta07316f","DOIUrl":"https://doi.org/10.1039/d6ta07316f","url":null,"abstract":"The rational design of bifunctional electrocatalysts with optimized electronic structures and rapid charge-transfer characteristics is essential for achieving efficient alkaline water electrolysis. Herein, Dy-doped copper neodymium oxides (CuNd(2-x)DyₓO4) were successfully prepared via a microwave-mediated sol-gel process, followed by their integration with carbon nanotubes (CNT) through a facile sonication process. The resulting change in material properties on Dy substitution was systematically analysed experimentally and theoretically. The incorporation of Dy effectively tailored the local electronic environment, generating abundant catalytic sites and promoting enhanced interactions with reaction intermediates, whereas the CNT framework accelerated charge transport and enhanced electrochemically accessible surface area. Consequently, the optimized CuNd1.9Dy0.1O4@CNT electrocatalyst exhibited superior bifunctional activity, requiring low overpotentials of 181 and 289 mV for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 10 mA cm-2 in 1 M KOH. Correspondingly, the Tafel slopes of 109.58 and 70.59 mV dec⁻¹ were obtained for the respective reactions. The catalyst further achieved an outstanding operational durability over 50 h. The enhanced catalytic activity is ascribed to the synergistic effects of Dy-induced electronic structure modulation and the highly conductive CNT network. This study presents a promising strategy for engineering rare-earth-based oxide/carbon heterostructures and offers valuable insights into the design of highly efficient and robust bifunctional electrocatalysts for overall water splitting and sustainable hydrogen production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"36 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374928","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}
引用次数: 0
Tin Stabilised Lithium-Rich Cobalt-Free Cathodes for High Voltage Lithium-ion Batteries 高压锂离子电池用锡稳定富锂无钴阴极
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta05845k
Chenglong Wu,David Burnett,Tengfei Song,Wilgner Lima da Silva,Bo Dong,Dominika Gastol,Sang Pham,Dominic Spencer-Jolly,Peter R. Slater,Emma Kendrick
{"title":"Tin Stabilised Lithium-Rich Cobalt-Free Cathodes for High Voltage Lithium-ion Batteries","authors":"Chenglong Wu,David Burnett,Tengfei Song,Wilgner Lima da Silva,Bo Dong,Dominika Gastol,Sang Pham,Dominic Spencer-Jolly,Peter R. Slater,Emma Kendrick","doi":"10.1039/d6ta05845k","DOIUrl":"https://doi.org/10.1039/d6ta05845k","url":null,"abstract":"Lithium-rich cobalt-free cathodes are among the most promising next-generation cathode materials for lithium-ion batteries owing to their high specific capacity. Nevertheless, practical applications are hindered by intrinsic challenges such as phase transitions, microstructural defects, and voltage decay during cycling. Here, we report a Sn-doped lithium-rich, manganese-based, cobalt-free cathode material, Sn-modified Li 1.2 Mn 0.5 Ni 0.3 O 2 , engineered via dual-site Sn modification to enhance structural stability and electrochemical performance. As a bulk dopant, Sn expands the Li-layer interlayer spacing and strengthens the transition metal-oxygen framework. As a surface-localised species, the formation of the surface layer mitigates transition metal dissolution and maintains efficient Li⁺ transport. This synergistic design enables rapid Li + diffusion while preserving both bulk crystallinity and interfacial integrity. The optimised Snmodified cathode achieves an excellent improvement in cycling stability, with a 22.4% increase in capacity retention after 400 cycles at 0.3C in full cells, together with a high initial specific capacity (241 mAh g -1 at 10 mA g -1 ) and superior high-rate performance (127 mAh g -1 at 1000 mA g -1 ) in half cells. This work systematically demonstrates that dual-site Sn modification, by simultaneously stabilising the bulk lattice and constructing a robust cathode-electrolyte interface, is an effective and scalable strategy to address the practical limitations of this lithium-rich, manganese-based, cobalt-free oxide.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374929","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}
引用次数: 0
Beyond boundary lines: predicting P2/O3 phase fractions in layered Na-ion cathodes 超越边界线:预测层状钠离子阴极中P2/O3相分数
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta05776d
Arsalan Zare,Hirbod Salari,Reza Khadem Hosseini,Hirad Salari,Mahdi Hamidi
{"title":"Beyond boundary lines: predicting P2/O3 phase fractions in layered Na-ion cathodes","authors":"Arsalan Zare,Hirbod Salari,Reza Khadem Hosseini,Hirad Salari,Mahdi Hamidi","doi":"10.1039/d6ta05776d","DOIUrl":"https://doi.org/10.1039/d6ta05776d","url":null,"abstract":"Layered Na-transition-metal oxides for sodium-ion batteries often form mixed P2/O3 phases and the proportion of these phases can change with slight modifications in composition or calcination temperature. This makes materials design frustratingly empirical. Commonly used boundary-line criteria, based on cationic and sodium potential, can identify single-phase compositions. However, they offer very limited insights for quantifying the mixed P2/O3 fractions and largely overlook synthesis temperature. Here, we present a data-driven framework that considers composition–calcination conditions in predicting the P2 fraction directly from composition and processing variables, offering continuous, quantitative composition–calcination-condition phase maps alternative to existing single/biphasic classification schemes. Among the models evaluated, including random forest, XGBoost, gradient boosting, and Gaussian process regression, the MLP model achieves the highest predictive accuracy on the held-out test set (R2 = 0.93), and is further validated against 26 experimentally synthesized compositions, yielding a mean absolute error of 0.137. The model accurately captures biphasic behavior where boundary-line criteria fall short. By incorporating calcination temperature as an explicit input variable, the resulting maps serve as a compositional reference for targeting specific P2/O3 ratios within the Ni–Fe–Mn–Ti system. This reduces the number of trial compositions needed to approach a target phase fraction, supporting more efficient optimization of layered Na-ion cathodes in the biphasic regime.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"23 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374934","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}
引用次数: 0
Mechanochemical-induced structural evolution governs lithium extraction kinetics in LiMn₂O₄ ion sieves 机械化学诱导的结构演化决定了LiMn₂O₄离子筛中锂的萃取动力学
IF 11.9 2区 材料科学
Journal of Materials Chemistry A Pub Date : 2026-11-10 DOI: 10.1039/d6ta07519c
Mohsen Sadeqi-Moqadam,Hung Q Nguyen,Quoc-Anh Tran,Peter Kunnas,Jin Feng,Daniel Rettenwander
{"title":"Mechanochemical-induced structural evolution governs lithium extraction kinetics in LiMn₂O₄ ion sieves","authors":"Mohsen Sadeqi-Moqadam,Hung Q Nguyen,Quoc-Anh Tran,Peter Kunnas,Jin Feng,Daniel Rettenwander","doi":"10.1039/d6ta07519c","DOIUrl":"https://doi.org/10.1039/d6ta07519c","url":null,"abstract":"Mechanochemical processing is widely used to improve lithium-ion sieves for direct lithium extraction (DLE), yet its influence on lithium extraction kinetics remains poorly understood. Here we show that mechanochemical milling exerts a non-monotonic and cycledependent influence on lithium extraction from spinel LiMn₂O₄-derived ion sieves. Although intensive milling substantially increases the specific surface area, it simultaneously generates a defect-rich surface characterized by lattice disorder, partial amorphization, and dispersion instability, resulting in reduced lithium uptake and slower extraction kinetics despite the smaller particle size. During desorption process as it exposed to acidic solution, these unstable surface regions are preferentially dissolved, progressively reconstructing the adsorption interface and restoring extraction performance upon cycling. A modified shrinking-core model quantitatively links this structural evolution to lithium extraction kinetics by separating diffusion, surfacereaction, and mass-transfer contributions. Together, the experiments and modeling establish a processing-structure-kinetics relationship that shows lithium extraction is governed not by particle size alone but by the balance between mechanochemical-induced disorder and regeneration-driven surface reconstruction. This framework provides design principles for engineering robust ion sieves for direct lithium extraction.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149374982","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}
引用次数: 0
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