Journal of Materials Chemistry A最新文献

{"title":"Atomic-Scale Visualization of Single Atom Formation in Metal-Organic Frameworks","authors":"Kai-Yuan Hsiao, Yi-Dong Lin, Yu-Ru Lin, Ching-Wei Chin, Chun-Hui Lin, Ruei-Hong Cyu, Yan-Gu Lin, Yu-Lun Chueh, Ming-Yen Lu","doi":"10.1039/d4ta07390h","DOIUrl":"https://doi.org/10.1039/d4ta07390h","url":null,"abstract":"Recently, non-noble metal single atoms (SAs) emerge as a groundbreaking class of materials, offering enhanced efficiency, reduced metal consumption, and widespread applicability. In the present study, zeolite imidazole frameworks-8 (ZIF-8) acts as a template for encapsulating Fe precursors and transform into porous nitrogen-doped carbon (PNC) upon pyrolysis, effectively capturing Fe SAs at nitrogen defect sites. The evolutions of Fe SA formation within porous ZIF-8 structure using atomic-scale in situ high-resolution scanning transmission electron microscopy (HR-STEM) from 325 ℃ to 400 ℃ are investigated. The formation rates of SAs increase with temperature, most importantly, the formation rates of SAs are rapid in the early stage and then slow down with prolonged pyrolysis time, e.g. the densities of SAs are 2.04 × 105 /μm2 and 4.21 × 105 /μm2 at 400 oC for 3 min and 30 min, respectively. The two-stage formation process may be governed by the atomization of Fe atoms from dispersed and clustered Fe(acac)3 precursors, respectively. Theoretical calculations are implemented to understand the formation mechanisms of the two stages. These insights, facilitated by atomic-scale in situ observation, offer precise control over synthesis pathways, thereby advancing the design of tailored SA materials for catalytic applications and beyond.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"145 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164951","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 Fluoride-Incorporated Composite Electrolyte Enabling High-Voltage All-Solid-State Sulfide-based Lithium Batteries","authors":"Ziyu Lu, Siwu Li, Lin Li, Liang Ming, Ziling Jiang, Miao Deng, Zhenyu Wang, Chen Liu, Chuang Yu","doi":"10.1039/d5ta03109e","DOIUrl":"https://doi.org/10.1039/d5ta03109e","url":null,"abstract":"All-solid-state lithium batteries (ASSLMBs) employing sulfide electrolytes exhibit remarkable energy density and inherent safety, and the integration of high-voltage cathode materials further enhances their advantage in performance. Nevertheless, the interfacial degradation between high-voltage cathodes and sulfides during long cycling remains a significant challenge. Herein, a biphasic composite electrolyte integrating halide electrolyte Li3AlF6 with sulfide electrolyte Li5.5PS4.5Cl1.5 is constructed to combine high ionic conductivity and high-voltage adaptability in ASSLMBs. Specifically, the biphasic electrolyte obtained via ball-milling retains ionic conductivity exceeding 1 mS cm-1. Furthermore, Li3AlF6 effectively mitigates surface degradation and irreversible phase transitions in the LiCoO2 cathode material at high voltages by enhancing interfacial charge transfer kinetics. As a result, ASSLMBs integrating the biphasic electrolyte and uncoated LiCoO2 cathode deliver an ultra-high specific capacity of 161.1 mAh g-1 at 0.1C (4.2 V vs. Li-In), excellent rate performance of 128.3 mAh g-1 at 1C, and long-term cyclability retaining 86.0 mAh g-1 after 100 cycles. This discovery underscores the significant efficacy of the halide compositing strategy in improving the electrochemical stability of sulfide electrolytes. It also offers valuable insights for the design of ASSLMBs tailored to high-voltage applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"36 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164958","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":"Atomic layer deposition of a thin TiO2 layer on nickel-rich cathode NCM83 for improved cycling stability","authors":"Can Liu, Danyang Li, Shu Zhao, Hao Li, Fujie Li, Guangrong Zeng, Hai-Chao Chen, Chao Wang, Xiu Song Zhao","doi":"10.1039/d5ta02510a","DOIUrl":"https://doi.org/10.1039/d5ta02510a","url":null,"abstract":"Nickle-rich layered oxides (NCMs) are promising cathode materials for high energy-density lithium-ion batteries (LIBs). However, NCMs suffer from poor cycling stability because of severe interfacial side reactions and phase transitions during cycling. Here, we show that by coating a thin and uniform layer of titanium dioxide (TiO2) on the surface of NCM83 (LiNi0.83Co0.11Mn0.06O2) using the atomic layer deposition (ALD) method, its cycling stability is significantly improved with 87.3% capacity retention after 100 cycles at 1C, in sharp contrast to NCM83 without TiO2 coating with only 44.3% capacity retention under the same electrochemical measurement conditions. XPS and ToF-SIMS characterization results reveal that the coated TiO2 layer promotes the formation of a LiF-rich stable cathode/electrolyte interphase (CEI), which effectively suppresses interfacial side reactions and mitigates phase transitions. In-situ XRD characterization results show that the TiO2 coating layer regulates the phase transition process due to mechanical confinement effects, which alleviates crystal distortion and stress accumulation. This work offers an effective approach to modifying nickel-rich cathode materials for high energy-density LIBs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"40 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164960","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":"Breaking structural symmetry to facilitate fast reaction kinetics","authors":"Woosik Min, Seokhyun Lee, Juncheol Hwang, Sangho Yoon, Duho Kim","doi":"10.1039/d5ta02769a","DOIUrl":"https://doi.org/10.1039/d5ta02769a","url":null,"abstract":"Breaking the intrinsic symmetry in crystal structures has emerged as a powerful strategy to enhance electrochemical reaction kinetics in advanced battery materials. In this study, we systematically investigate how introducing larger heteroatoms (e.g., Se, Te) into a cubic host lattice disrupts its symmetry, thereby creating new pathways for ionic transport. By expanding and splitting bond lengths, doping weakens the local bonding environment and reduces chemical hardness, which in turn lowers the energy barriers for (de)lithiation and accelerates phase-transition kinetics. Furthermore, Li kinetic calculations reveal that the resultant lattice distortions give rise to multiple diffusion routes, including newly formed channels with notably lower migration barriers. These findings underscore the critical role of structural asymmetry in improving charging rates and mitigating voltage hysteresis. Overall, this work highlights symmetry breaking as a promising design concept for developing high-performance battery materials, offering a pathway to faster Li-ion transport.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"153 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153915","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":"Rate-determining Step Backshift Effectively Boost ORR Performance by Excess Electrons Transfer to O-O Antibonding Orbital","authors":"Lili Zhang, Shengwei Yu, Xiang Xie, Jiaxi Zeng, Hongliang Jiang, Jianhua Shen, Hai Bo Jiang, Chunzhong Li","doi":"10.1039/d5ta01709b","DOIUrl":"https://doi.org/10.1039/d5ta01709b","url":null,"abstract":"Pt23Pd77 nanosheets (NSs) were successfully synthesized with a thickness of 1.33 nm and the mass activity (MA) of 6.78 A mgPGM-1, achieving excellent oxygen performance of 45.2 times higher than commercial Pt/C (0.15 A mgPt-1). Furthermore, the Tafel slope of Pt23Pd77 NSs is as low as 39.52 mV dec-1 compared to Pt/C (70.55 mV dec-1) indicating the rate-determining step (RDS) is transferred from *OOH cleavage to the second electron transfer. First-principles calculations show a decline in the barrier of *OOH → *O + *OH, thus the second electron transfer succeeds the RDS. In the kinetic-controlled region, the apparent activation energy (Ea) of Pt/C does not change with the change of overpotential, and the reaction order of OH- is close to 0, while the Ea of the NSs decreases with the increase of overpotential, and the reaction order is negative. All of this proves that the RDS moves backwards. This paper provides another idea for improving the performance optimization strategy of oxygen reduction, that is, the kinetic RDS backshift.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"58 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144164955","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: Sodium 4-styrenesulfonyl(trifluoromethanesulfonyl)imide-based single-ion conducting polymer electrolyte incorporating molecular transporters for quasi-solid-state sodium batteries","authors":"Clemens Wunder, Thanh-Loan Lai, Edina Šić, Torsten Gutmann, Eric De Vito, Gerd Buntkowsky, Maider Zarrabeitia, Stefano Passerini","doi":"10.1039/d5ta90118a","DOIUrl":"https://doi.org/10.1039/d5ta90118a","url":null,"abstract":"Correction for ‘Sodium 4-styrenesulfonyl(trifluoromethanesulfonyl)imide-based single-ion conducting polymer electrolyte incorporating molecular transporters for quasi-solid-state sodium batteries’ by Clemens Wunder <em>et al.</em>, <em>J. Mater. Chem. A</em>, 2024, <strong>12</strong>, 20935–20946, https://doi.org/10.1039/D4TA02329C.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"1 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145557","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":"Photon-induced isomerization enables high-performance polymer solar cells","authors":"Hanzhi Wu, Jiawei Qiao, Jinqun Xu, Mingxu Zhou, Zhen Fu, Peng Lu, Hang Yin, Xiaoyan Du, Wei Qin, Kangning Zhang, Xiao-Tao Hao","doi":"10.1039/d5ta02550h","DOIUrl":"https://doi.org/10.1039/d5ta02550h","url":null,"abstract":"The introduction of isomeric components into the active layers demonstrates effective mitigation of morphological defects arising from thermodynamic immiscibility in all-polymer solar cells (all-PSCs). Nevertheless, conventional isomerization methods for donor and acceptor materials remain complex and challenging to implement for intensifying photovoltaic performance. To overcome this limitation, we propose a photo-isomerization strategy involving ultraviolet laser irradiation of polymer materials in solutions. Structural and photophysical characterizations reveal that neat polymer films present enhanced crystallinity, prolonged exciton lifetime, and extended exciton diffusion length through the isomeric component incorporation. These benefits further synergistically strengthens intermolecular π-π stacking interaction and optimizes vertical distribution gradient in the active layers fabricated via layer-by-layer deposition, delivering an ideal bicontinuous interpenetrating network morphology. Notably, the refined morphology of the active layers increases the proportion of local excitons converting into charge transfer states to facilitate exciton dissociation, improves charge transport, and suppresses charge recombination. Ultimately, the laser-processed PM6:PY-IT devices achieve a promising power conversion efficiency of 18.21% and ameliorated stability including both thermal stability and photostability. This work confirms that ultraviolet laser irradiation can serve as a facile and effective approach for inducing isomerization of organic photovoltaic materials, offering a photochemical perspective toward efficient and stable PSCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145812","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 critical review on Recent advancement on Metal -Organic Frameworks (MOFs) for CO2 capture, storage and utilization","authors":"Swati Kumari, Mahek Gusain, Bhawna Yadav Lamba, Sanjeev Kumar","doi":"10.1039/d5ta02338f","DOIUrl":"https://doi.org/10.1039/d5ta02338f","url":null,"abstract":"One of the biggest problems our world is currently facing is global climate change brought on by rising atmospheric CO2 levels. The creation of technology that encourage \"negative carbon emissions\" is necessary to address this worldwide catastrophe. As the shift to more sustainable energy infrastructures advances, carbon capture and storage (CCS) and CCU (Carbon capture and utilization) technologies are essential for removing CO2 from current emission sources, such as industrial and energy production facilities. Metal-organic frameworks (MOFs) are a new class of solid porous materials that have attracted a lot of interest recently in addition to conventional inorganic adsorbents. MOFs as an adsorbent are a rapidly expanding subject due to their versatility in structure and function. Innovation in carbon capture solutions is still being fuelled by the promising performance of MOF-based technology. An ever-increasing number of current publications and citations, as well as the ongoing expansion of study scope and researcher interaction, demands a summarization of the approaches made in this time regarding MOFs. Here in this review at first, insight to MOFs has been given followed by the routes to MOFs from conventional (For e.g., Solvothermal/hydrothermal) to contemporary (Microwave-assisted, mechanochemical, electrochemical, microemulsion, Sonochemical, dry-gel conversion method) to other methods (for e.g., green synthesis, ionic-liquid based and discarded material as a synthesis medium). Later characterization techniques (for e.g., XRD, FTIR, TGA, BET) has been discussed briefly. Thereafter application of MOFs for CO2 capture (mainly focused on MOFs for post combustion CO2 capture and Direct air capture), CO2 storage and CO2 conversion (for e.g., MOFs as photocatalyst and MOFs as electrocatalyst) has been mentioned. Further Commercialization, scalability and environmental impact of MOFs are summarized. Finally, some suggestions for the future development of the MOFs are outlined, and we hope that the valuable insights accumulated in this review will be helpful for future research.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Regulation of Transition Metal Atoms Supported on Defective h-BN by Adjacent Monovacancies for Electrochemical CO2 Reduction: Mechanism and d-band Spin-Polarization Effect","authors":"Wenjie Wang, Meiyun Zhang, Jinhao Zhou, Bingfeng Fan","doi":"10.1039/d5ta01487e","DOIUrl":"https://doi.org/10.1039/d5ta01487e","url":null,"abstract":"Transition metal (TM)-doped defective hexagonal boron nitride (h-BN) single-atom catalysts (SACs) show significant promise for the electrochemical carbon dioxide reduction reaction (CO2RR). Given that defect engineering has emerged as a potent strategy for enhancing the catalytic performance of two-dimensional SACs and extensive experimental studies have observed that doping transition metals into defective two-dimensional substrates promotes the formation of adjacent vacancies, a comprehensive theoretical investigation is essential to elucidate the impact of different adjacent vacancies on the catalytic properties of TM-doped h-BN SACs. This study employs density functional theory calculations to investigate the regulatory effects and mechanisms of five types of adjacent boron and nitrogen monovacancies on the CO2RR catalytic performance of Fe, Co, and Mo atoms anchored on defective h-BN (denoted as M-vac@BN, where M = Fe, Mo, Co and vac = B1, B2, B3, N1, N2). Stability analysis reveals that the position and type of adjacent monovacancies significantly impact the stability of the supported metal atoms. Volcano plot and linear relationship analysis demonstrate that the CO adsorption energy (EB(CO)) serves as a reliable descriptor for predicting the overpotential for CO2RR on M-vac@BN. Strategic introduction of specific adjacent monovacancies can effectively tune the CO adsorption strength, thereby influencing the catalytic activity. More interestingly, a strong linear relationship is observed between the magnetic moments of transition metal atoms M in M-vac@BN (M = Co, Mo) and the integrated projected crystal orbital Hamiltonian population (IpCOHP) of the M-C bonds in CO adsorption intermediates, which arises from the linear relationship between the M-C bond strength in CO adsorption intermediate and the d-band spin polarization of the M atom in M-vac@BN. Specifically, enhanced d-band spin polarization strengthens the M-C bond by broadening the bonding peak in the projected crystal orbital Hamiltonian population (pCOHP) of the M-C bond.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"24 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145555","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":"Acidic-Neutral Decoupled Biphasic Electrolytes Enhance Deposition-Dissolution Chemistry in Zn–Mn Batteries","authors":"Yidan Cui, Qingyun Dou, Jiewen Yang, Jingke Yang, Xiaoxi Zhao, Guosheng Li, Pengwei Jing, Qingyue Yin, Caihong Tao, Xingbin Yan","doi":"10.1039/d5ta02521d","DOIUrl":"https://doi.org/10.1039/d5ta02521d","url":null,"abstract":"Aqueous Zn–Mn batteries are emerging as promising candidates for next-generation energy storage technologies owing to their advantages including high energy density, low cost, and excellent reliability. However, conventional aqueous electrolytes struggle to meet the dual deposition-dissolution requirements of the Mn2+/MnO2 cathodes and Zn2+/Zn anodes simultaneously. The Mn2+/MnO2 two-electron redox reaction in cathodes demands an acidic condition to achieve a theoretical capacity of 616 mAh g−1, twice that of neutral and alkaline systems, yet such a condition inevitably exacerbates Zn anode corrosion and undesirable hydrogen evolution reaction. To address this fundamental conflict, this study designs a self-stratifying aqueous-organic biphasic electrolyte, which successfully decouples the working conditions of the Mn cathodes and Zn anodes. The proof-of-concept Zn–Mn battery employing this biphasic electrolyte enables efficient Mn2+/MnO2 redox chemistry in the acidic aqueous phase and stable Zn plating-stripping in the neutral organic phase, therefore achieving a high discharge voltage of ~1.8 V, along with a stable cycling life of 90% capacity retention over 250 cycles. This work demonstrates an effective strategy for decoupling acidic and neutral conditions in a biphasic electrolyte and provides insights into the development of high-energy Zn–Mn batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144145810","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}