Journal of Materials Chemistry A最新文献

{"title":"Immobilising molecular redox mediators for the oxygen evolution reaction using self-assembled monolayers","authors":"Samar Gharbi, Isaac Alcón, Jordi Ribas-Ariño, Nuria Crivillers, Stefan T. Bromley, Marta Mas-Torrent","doi":"10.1039/d5ta05164a","DOIUrl":"https://doi.org/10.1039/d5ta05164a","url":null,"abstract":"The development of efficient and economical electrocatalysts for the oxygen evolution reaction (OER) that are stable and free of noble metals remains a significant scientific and technological challenge. The use of redox mediators (RMs) offers a promising approach to enhance the efficiency of electrocatalysts for a range of applications. However, the migration of the RM molecules between the electrodes, also known as shuttle effect, leads to undesirable redox side reactions and a reduction of the OER performance. Here, we show how covalently attaching RMs to the electrode surface in self-assembled monolayers (SAMs) can immobilize them and avoid their diffusion into the electrolyte. For this purpose, we prepared different SAMs using two types of RMs based on tetrathiafulvalene (TTF) derivatives and using indium tin oxide (ITO) and fluorine doped tin oxide (FTO) as substrates. All electrodes showed efficient electrocatalytic activity under alkaline conditions. In this small proof-of-concept set of systems, we could achieve an OER performance with an overpotential of 400 mV at 0.25 mA/cm² and a Tafel slope of 103 mV/dec. We rationalise these experimental findings with computational chemical modelling, which suggests that further improvements could be achieved through targeted chemical modifications to tune the highest occupied molecular orbital energy in these TTF-based RMs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"21 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182973","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":"100 Gram-Scale Organic-free Synthesis of Bi2O2(CO3)2 Nanosheets for High-Selective Formate Production in CO2 Electroreduction","authors":"Minglong Guo, Xiaoyan He, Guangxing Yang, Hongjuan Wang, Feng Peng, Guoqiang Cao, Qiao Zhang, Zhiting Liu","doi":"10.1039/d5ta06873h","DOIUrl":"https://doi.org/10.1039/d5ta06873h","url":null,"abstract":"In the realm of CO 2 electrochemical reduction, Bi 2 O 2 CO 3 nanosheets have garnered attention for their ability to selectively produce formate. However, as CO 2 electroreduction technologies advance toward industrial applications, a scalable and green synthesis method is urgently needed. Our research leverages three common Bi-based inorganic salts-BiCl 3 , Bi 2 (SO 4 ) 3 , and Bi(NO 3 ) 3 -as precursors to develop a straightforward process of hydrolysis followed by anions exchange. This method produces high yields of Bi 2 O 2 CO 3 nanosheets without the need for organic solvents or external heating, even at a large scale of ~100 grams, ensuring both sustainability and cost-efficiency. The resulting nanosheets achieved Faradaic efficiencies exceeding 90% across a wide range of potentials for formate production. The combination of innovative synthesis and effective CO 2 conversion underscores the potential of Bi 2 O 2 CO 3 for industrial-scale applications in sustainable energy and chemical production.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"53 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182971","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":"Precise Design of MOF-Derived Single Atom Catalysts with Symmetric and Asymmetric Coordination for Advanced Lithium-Sulfur Batteries","authors":"Yu Zhang, Xiao-Chen Liu, Hongwei Guo, Zheng Zhou, Kui Chen, Guangning Wu","doi":"10.1039/d5ta05134g","DOIUrl":"https://doi.org/10.1039/d5ta05134g","url":null,"abstract":"Single atom catalysts (SACs) have demonstrated great potential for ideal electrocatalytic hosts of sulfur cathode in lithium-sulfur (Li-S) batteries. The coordination microenvironments of SACs influence hugely on lithium polysulfides (LiPSs) shuttle effect and sulfur reaction kinetics. Recently, metal-organic frameworks (MOFs) have emerged as a versatile platform for the precise synthesis of SACs, stemming from the high metal loading capacity, structurally ordered porosity and atomiclevel tailorability. Many efforts have been made to create symmetric and asymmetric coordination structures in MOF-based SACs in the application of Li-S batteries, but a comprehensive summary on the catalysts design, structural evolution, and performance evaluation is still lacking. In this article, we systematically categorize the design strategies of symmetric and asymmetric coordination structures in the use of sulfur cathode hosts and their action mechanisms in reinforced Li-S batteries. We also deeply discussed the influence of coordination symmetry of SACs derived from MOFs on the adsorption energy of LiPSs and catalytic performance of sulfur conversion. To propel the development of high-performance MOFsderived SACs in Li-S batteries, the current technical challenges and proposed research directions are presented.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"20 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182977","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":"High-Performance Na 3.5 Fe 0.5 V 1.5 (PO 4 ) 3 Cathodes Enabled by Phase Control and CQD-Containing Carbon Coating","authors":"Haoyu Guonie, Changwei Shi, Changlian Chen, Chaoqun Shang, Pu Hu","doi":"10.1039/d5ta06954h","DOIUrl":"https://doi.org/10.1039/d5ta06954h","url":null,"abstract":"Fast-charging sodium-ion batteries (SIBs) demand cathode materials with rapid redox kinetics and robust structural integrity. Herein, a series of Na 3+x V 2-x Fe x (PO 4 ) 3 /C (0 ≤ x ≤ 1) cathodes are synthesized via a citric acid-assisted spray-drying strategy.Citric acid acts as both chelating agent and carbon source, effectively suppressing electrochemically inert NaFePO 4 impurity formation and enabling a phase-pure NASICON framework with a carbon coating containing carbon quantum dots (CQDs).The optimized composition, Na 3.5 Fe 0.5 V 1.5 (PO 4 ) 3 /C, delivers a high reversible capacity of 124 mAh g -1 at 0.5 C and 95 mAh g -1 at 20 C, while retaining 93.1% of its initial capacity over 1000 cycles at 20 C. Detailed kinetic analysis reveals that the elimination of NaFePO 4 and the composite carbon layer with CQDs greatly enhance the Fe 2+ /Fe 3+ and V 4+ /V 5+ redox activity, especially under high-rate conditions. This study underscores the importance of phase and interface engineering in optimizing NASICON-type cathodes and provides a scalable route toward high-power, long-life SIBs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"75 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189213","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":"Advances in reversible protonic ceramic electrochemical cells operated below 723 K: theoretical insights and experimental developments","authors":"Libin Lei, Ruiming Qiu, Feifei Dong, Hanlin Su, Ao Wang, Junyao Wang, Zhipeng Tian, Chao Wang, Bo Liang, Xianglong Luo, Ying Chen, Dmitry A. Medvedev, Jian Xue","doi":"10.1039/d5ta04354a","DOIUrl":"https://doi.org/10.1039/d5ta04354a","url":null,"abstract":"Lowering the operating temperature of ceramic electrochemical cells below 723 K can efficiently mitigate component degradation and reduce system costs. Compared with traditional oxygen-ion conducting ceramic electrochemical cells, reversible protonic ceramic electrochemical cells (R-PCECs) offer greater potential for operation below 723 K due to the low activation energy for proton conduction, thus attracting significant research attention over the past decade. However, maintaining reasonable performance and efficiency at reduced temperatures remains a critical challenge. This review provides a comprehensive summary of theoretical insights and recent experimental advancements in R-PCECs operated below 723 K. In the theoretical aspect, one-dimensional charge transportation models, the kinetics/polarization of electrodes, and two/three-dimensional multi-physics models are summarized, with a critical evaluation of existing models and their simulation results, especially for faradaic efficiency. Experimentally, efficient strategies for enhancing electrolyte, oxygen electrode, and fuel electrode performance are systematically reviewed and critically analyzed. Additionally, the potential of advanced computational approaches, such as high-throughput computation and machine learning-assisted methods, is discussed. Based on the comprehensive and critical discussion, detailed issues in the development of R-PCECs operated below 723 K are identified, and prospective research is outlined.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"30 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182972","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":"Electronic Asymmetry in Janus Ce/ThXY (X, Y= S and Se) Promoting Photocatalytic Oxygen Evolution Reaction in Acidic environments","authors":"Jinhao Xu, Shuxian Hu","doi":"10.1039/d5ta04783h","DOIUrl":"https://doi.org/10.1039/d5ta04783h","url":null,"abstract":"Two-dimensional (2D) materials have emerged as promising candidates for photocatalytic water splitting due to their exceptional electronic and structural properties. While transition metal dichalcogenides (TMDs) have been widely studied, the potential of f-electron-based dichalcogenides remains underexplored. In this study, we employ first-principles density functional theory (DFT) calculations to investigate the structural stability, electronic properties, and photocatalytic performance of monolayer thorium (Th) and cerium (Ce)-based Janus dichalcogenides MXY (M = Th, Ce; X, Y = S, Se, Te). Our findings reveal that the 1T-phase is the most thermodynamically stable configuration, due to f-orbital tend to be Oh symmetry. Band structure analysis indicates that 1T-phase Th-based compounds possess conduction and valence band positions suitable for overall water splitting, while Ce-based materials exhibit limitations due to lower conduction band minima. Optical absorption spectra highlight that ThSe₂, ThSSe, ThTe₂, ThSTe, and ThSeTe demonstrate strong visible-light absorption, making them potential photocatalysts. Additionally, free energy analysis of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) intermediates identifies ThSTe and ThSeTe as highly active for OER across a broad pH range. These findings provide insights into the design of f-electron-based materials for renewable energy applications and highlight their potential as next-generation photocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"92 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182980","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":"Correction: Synergistically enhanced energy storage performance of Bi0.47Na0.47Ba0.06TiO3-based relaxor ferroelectrics via dual engineering of dynamic nanodomains and defect regulation","authors":"Jiangping Huang, Lian Deng, Yu Zhang, Yue Pan, Xiuli Chen, Xu Li, Huanfu Zhou","doi":"10.1039/d5ta90217g","DOIUrl":"https://doi.org/10.1039/d5ta90217g","url":null,"abstract":"Correction for ‘Synergistically enhanced energy storage performance of Bi<small>_0.47</small>Na<small>_0.47</small>Ba<small>_0.06</small>TiO<small>₃</small>-based relaxor ferroelectrics <em>via</em> dual engineering of dynamic nanodomains and defect regulation’ by Jiangping Huang <em>et al.</em>, <em>J. Mater. Chem. A</em>, 2025, <strong>13</strong>, 30053–30064, https://doi.org/10.1039/D5TA04848F.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"78 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183361","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":"Contributors to the Journal of Materials Chemistry A Emerging Investigators 2025 collection","authors":"","doi":"10.1039/d5ta90200b","DOIUrl":"https://doi.org/10.1039/d5ta90200b","url":null,"abstract":"Our 2025 Emerging Investigators themed collection gathers some of the best research being conducted by scientists in the early stages of their independent career. Each contributor was recommended as carrying out work with the potential to influence future directions in materials chemistry. Congratulations to all the researchers featured, we hope you enjoy reading this collection.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"19 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182975","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 Effect of Mechanical Stimuli and Defects on the Catalytic Activity of Janus Transition Metal Dichalcogenides for Hydrogen Evolution Reaction: An Explicit First-Principles Study","authors":"ZeZhang Qi, Jing Xu, Wanlin Guo, Yufeng Guo","doi":"10.1039/d5ta05808b","DOIUrl":"https://doi.org/10.1039/d5ta05808b","url":null,"abstract":"Developing catalysts based on transition metal dichalcogenides (TMDs) represents a promising aspect for the application of TMD materials. Our extensive first-principles calculations and ab initio molecular dynamics simulations, which incorporate an explicit solvation model, reveal that the introduction of vacancy defects into Janus TMD (MXY, where M = Mo or W; X/Y = S, Se, or Te, and X ≠ Y) monolayers can activate their catalytic capability for the hydrogen evolution reaction (HER). The application of biaxial tensile strain further enhances the catalytic activity of vacancy-defected WSeS, WSSe and WTeS monolayers, but weakens that of other Janus TMD monolayers. When the electronegativity of the top surface X atoms of a vacancy-defected MXY monolayer is relatively weaker, applying a biaxial tensile strain leads to lower elastic energy and higher hydrogen adsorption energy at the vacancy site for the MXY monolayer, along with a larger deviation in its hydrogen adsorption Gibbs free energy. The unveiled relationship between mechanical energy, hydrogen adsorption energy, and surface electronegativity deepens our understanding of the role of mechanical stimuli in modulating and improving the catalytic activity of Janus TMDs for the HER.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"155 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183360","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":"Pd composition and dispersion control selectivity in photocatalytic methane oxidation","authors":"Jiawei Wu, Hu Ding, Yan Wang, Ulfi Muliane, Shuji Anabuki, Naoya Murakami, Xinli Zhu, Akira Yamakata, Teruhisa Ohno, Shi Nee Lou","doi":"10.1039/d5ta04478b","DOIUrl":"https://doi.org/10.1039/d5ta04478b","url":null,"abstract":"Selective methane oxidation to methanol under mild conditions presented a significant challenge due to the high bond dissociation energy of methane and the difficulty in achieving high selectivity. This study investigated how Pd composition and dispersion influenced photocatalytic oxidation of methane over brookite TiO<small>₂</small> (BTO) nanorods, using molecular O<small>₂</small> and water as oxidants. <em>In situ</em> time-resolved transient absorption (TA) spectroscopy in the visible to mid-infrared (IR) range, along with X-ray photoelectron spectroscopy (XPS) analysis before and after methane oxidation, revealed that BTO nanorods with high Pd loading and lower Pd dispersion exhibited significant electron trapping in the Pd/PdO nanoparticles under light irradiation. This electron trapping promoted the self-reduction of PdO to metallic Pd (Pd<small>⁰</small>), which in turn drove the selective production of CH<small>₃</small>OH with 98% selectivity. In contrast, a moderate Pd loading and dispersion on the BTO nanorods enhanced electron transfer to O<small>₂</small>, reducing electron trapping, and resulted in a higher concentrations of mixed Pd<small>⁰</small>/PdO nanoparticles, favoring the formation of primary oxygenates – CH<small>₃</small>OOH and CH<small>₃</small>OH. DFT calculations and experimental findings showed that Pd<small>⁰</small> facilitates the direct three-electron reduction of O<small>₂</small> to *OH or ˙OH, which subsequently coupled with *CH<small>₃</small> or ˙CH<small>₃</small> to form CH<small>₃</small>OH. Meanwhile PdO promotes the one-electron reduction of O<small>₂</small> to *OOH or ˙OOH, leading to CH<small>₃</small>OOH formation. This work provides valuable insights into the design of efficient photocatalysts for selective methane oxidation and underscores the critical role of Pd composition and dispersion in modulating charge dynamics and steering product selectivity in methane.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"5 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182974","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}