ACS Materials Au最新文献

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Terminal Group Effects on Molecular Organization and Charge Extraction in Self-Assembled Monolayers/Perovskite Interfaces 自组装单层/钙钛矿界面中末端基团对分子组织和电荷提取的影响
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-16 DOI: 10.1021/acsmaterialsau.6c00070
Arthur P. Machado, Felipe C. Braga, Carlos H. Stadtlober, Paulo E. Marchezi, Douglas S. Ribeiro, Murillo H. M. Rodrigues, Zeno C. Brandão, Diogo M. G. Neto, Caio C. Oliveira, Ana F. Nogueira
{"title":"Terminal Group Effects on Molecular Organization and Charge Extraction in Self-Assembled Monolayers/Perovskite Interfaces","authors":"Arthur P. Machado,&nbsp;Felipe C. Braga,&nbsp;Carlos H. Stadtlober,&nbsp;Paulo E. Marchezi,&nbsp;Douglas S. Ribeiro,&nbsp;Murillo H. M. Rodrigues,&nbsp;Zeno C. Brandão,&nbsp;Diogo M. G. Neto,&nbsp;Caio C. Oliveira,&nbsp;Ana F. Nogueira","doi":"10.1021/acsmaterialsau.6c00070","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00070","url":null,"abstract":"<p>The structural nature of self-assembled monolayers (SAMs)criticallydetermines interfacial quality, film formation, and charge transportin inverted perovskite solar cells (iPSCs). While variations in SAMfunctional groups have been explored, these studies have focused ontheir impact on device performance metrics. In contrast, a fundamentalunderstanding of how subtle molecular structural variations governthe molecular organization of SAMs, and how it modulates surface energy,interfacial properties, and the growth of perovskite films depositedatop these monolayers, remains limited. In addition, as perovskitetechnology advances toward industrial deployment, gaining fundamentalinsight into how SAMs govern film quality is essential for guidingthe development of efficient and stable devices. Here, we systematicallyinvestigate the effects of SAM terminal groups (electron-withdrawing,neutral, and electron-donating) on the morphology and optoelectronicproperties of perovskite films. Our results demonstrate that the electronicnature of the terminal group plays a decisive role in determiningSAM molecular organization, which in turn directly affects interfacialhole extraction efficiency.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1121–1130"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148924000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rewriting the mRNA Delivery Map: Albumin Hitchhiking Lipid Nanoparticles for Safer and Smarter Nanomedicine 重写mRNA传递图谱:白蛋白搭便车脂质纳米颗粒用于更安全和更智能的纳米药物
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-06-18 DOI: 10.1021/acsmaterialsau.6c00068
Abdul Shadab, Usama Ahmad, Yahya E. Choonara, Md Faiyazuddin
{"title":"Rewriting the mRNA Delivery Map: Albumin Hitchhiking Lipid Nanoparticles for Safer and Smarter Nanomedicine","authors":"Abdul Shadab,&nbsp;Usama Ahmad,&nbsp;Yahya E. Choonara,&nbsp;Md Faiyazuddin","doi":"10.1021/acsmaterialsau.6c00068","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00068","url":null,"abstract":"<p>LNPs are the basis of mRNA and nucleic acid-based therapeutics.However, their remarkable clinical potential is limited by a persistentchallenge, i.e., nonspecific accumulation in the liver and associatedhepatotoxicity. Traditional strategies, such as PEGylation and lipidionization modification, have reached a point of low therapeutic value-addto control biodistribution. Recently published studies present aninnovative concept: LNPs that recruit albumin, exploiting interactionswith endogenous albumin to avoid liver accumulation and simultaneouslyimprove delivery through the lymphatic system for immune-modulation.This review provides a concise incursion into such strategies thatredefine stealth nanomedicine, not as chemical camouflage but as abiological alliance with plasma transport proteins, paving the wayfor a new paradigm of self-protecting nanocarriers for safer and moreprecise mRNA therapeutics.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"956–973"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923923","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
From Assembly to Application: A Comprehensive Review of Metal–Hydrogen-Bonded Organic Frameworks 从组装到应用:金属-氢键有机框架的综合综述
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-07 DOI: 10.1021/acsmaterialsau.6c00112
Lamia A. Siddig, Khadega A. Al-Maqdi, Abdalla S. Abdelhamid, Ahmed Alzamly
{"title":"From Assembly to Application: A Comprehensive Review of Metal–Hydrogen-Bonded Organic Frameworks","authors":"Lamia A. Siddig,&nbsp;Khadega A. Al-Maqdi,&nbsp;Abdalla S. Abdelhamid,&nbsp;Ahmed Alzamly","doi":"10.1021/acsmaterialsau.6c00112","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00112","url":null,"abstract":"<p>Metal–hydrogen-bonded organic frameworks (M-HOFs)have emergedas novel crystalline porous materials that integrate robust metalcoordination units with extensive hydrogen-bonded networks, enablingarchitectures that offer both structural stability and tunable functionality.Extensive hydrogen bonding confers structural integrity, while incorporationof metal ions enhances chemical and thermal stability and introducescatalytic and sensing properties. Their tunable porosity, diversetopologies, and mild synthesis conditions render them highly desirablefor applications in chemical separation, gas storage, catalysis/photocatalysis,and environmental monitoring. This review provides a comprehensiveoverview of recent advances in the structural elucidation, and functionaldevelopment of M-HOFs. The self-assembly of these frameworks governedby the careful selection of metal centers and organic linkers criticallydetermines pore architecture, topology, and overall stability. Withinthis context, hydrogen-bonding interactions serve as essential supramolecularforces that direct and stabilize framework formation. Structural investigationshave revealed the remarkable adaptability of hydrogen-bonding networks,which can be finely tuned to modulate pore dimensions, enhance frameworkrobustness, and introduce tailored functionalities. These tunablestructural features directly influence the performance of M-HOFs,enabling their effective use in a wide range of practical applications.M-HOFs have already demonstrated strong potential in (photo) catalysis,adsorption, sensing, and drug delivery, underscoring their versatilityas next-generation porous materials. Finally, key opportunities arehighlighted in environmental remediation, clean energy technologies,and advanced functional applications.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"994–1018"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cathodoluminescence Analysis of Defects and Grain Boundaries in Zn3P2 Thin Films Grown on Graphene by MOVPE and MBE 石墨烯表面生长Zn3P2薄膜的阴极发光缺陷和晶界分析
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-28 DOI: 10.1021/acsmaterialsau.6c00120
Thomas Hagger, Mohammadreza Hassanzadeh, Aidas Urbonavicius, Ahmed El Alouani, Victor Boureau, Gulnaz Ganeeva, Nico Kawashima, Raphael Lemerle, Kamil Artur Wodzislawski, Sebastian Lehmann, Kimberly A. Dick, Silvana Botti, Adrien Michon, Anna Fontcuberta i Morral, Simon Escobar Steinvall
{"title":"Cathodoluminescence Analysis of Defects and Grain Boundaries in Zn3P2 Thin Films Grown on Graphene by MOVPE and MBE","authors":"Thomas Hagger,&nbsp;Mohammadreza Hassanzadeh,&nbsp;Aidas Urbonavicius,&nbsp;Ahmed El Alouani,&nbsp;Victor Boureau,&nbsp;Gulnaz Ganeeva,&nbsp;Nico Kawashima,&nbsp;Raphael Lemerle,&nbsp;Kamil Artur Wodzislawski,&nbsp;Sebastian Lehmann,&nbsp;Kimberly A. Dick,&nbsp;Silvana Botti,&nbsp;Adrien Michon,&nbsp;Anna Fontcuberta i Morral,&nbsp;Simon Escobar Steinvall","doi":"10.1021/acsmaterialsau.6c00120","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00120","url":null,"abstract":"<p>Zn<sub>3</sub>P<sub>2</sub> is a promising earth-abundantabsorberfor thin-film photovoltaics, yet its development is hindered by thelack of lattice-matched substrates, its incompatible thermal expansioncoefficient, and a complex defect landscape. Here, we demonstratethe quasi-van der Waals epitaxy of Zn<sub>3</sub>P<sub>2</sub> ongraphene by metal–organic vapor phase epitaxy (MOVPE) and demonstratea clear spatial correlation between antiphase boundary density andlocal variations in the optical emission using correlative electronmicroscopy and cathodoluminescence (CL). Moreover, CL measurementsshow that grain boundaries act as efficient non-radiative recombinationcenters, with an effective recovery length extending several micrometresinto the grains, indicating that grain boundaries can significantlyinfluence carrier transport and recombination in Zn<sub>3</sub>P<sub>2</sub>. Further comparison with molecular beam epitaxy grown filmsreveals the suppression of strain-related sub-bandgap emission inMOVPE-grown material. Overall, quasi-van der Waals epitaxy of Zn<sub>3</sub>P<sub>2</sub> by MOVPE resulted in larger grains and improvedmaterial quality. These results establish clear relationships betweenextended defects and the local optical response in Zn<sub>3</sub>P<sub>2</sub>, while highlighting grain-size control as a key strategyfor improving earth-abundant photovoltaic absorbers.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1172–1185"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stoichiometry-Defined Phase Selection and Hydrophobic Molecular Sealing in Bioderived Deep Eutectic Solvents 生物衍生的深共晶溶剂中化学计量学定义的相选择和疏水分子密封
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-06-25 DOI: 10.1021/acsmaterialsau.6c00088
Shunsuke Yamada, Takashi Honda
{"title":"Stoichiometry-Defined Phase Selection and Hydrophobic Molecular Sealing in Bioderived Deep Eutectic Solvents","authors":"Shunsuke Yamada,&nbsp;Takashi Honda","doi":"10.1021/acsmaterialsau.6c00088","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00088","url":null,"abstract":"<p>Deep eutectic solvents (DESs) are promising ionic mediaowing totheir abundance, ionic conductivity, and wide potential windows. BioderivedDESs based on choline chloride are attractive due to their biodegradabilityand biocompatibility; however, their strong hygroscopicity leads tosevere moisture uptake and instability. Here, we report a bioderivedmoisture-resistant DES of acetylcholine chloride as a hydrogen bondacceptor (HBA) and 3-phenylpropionic acid as a hydrophobic hydrogenbond donor. The hydrophobic component acts as a molecular seal, shieldingthe hygroscopic HBA from moisture through hydrogen-bond network reconfiguration.Systematic variation of the molar ratio reveals four distinct regimes:immiscible mixtures (1:1), saturated states (1:1.5), a homogeneousglass-forming liquid at the eutectic composition (1:2, <em>T</em><sub>g</sub> = −57.9 °C), and crystallizable phases athigher HBD contents (1:3 and 1:4). Only the eutectic composition stabilizesa uniform liquid without observable melting transitions, exhibitingover 75% reduction in moisture uptake relative to the parent saltat 58% relative humidity. The DES demonstrated a high ionic conductivity(197 μS cm<sup>–1</sup>) and a wide potential window(2.43 V). Moreover, the DES exhibited high biodegradability (&gt;90%),exceeding the OECD criterion for ready biodegradability (&gt;60% within28 days). These findings establish stoichiometry as a governing parametercoupling phase stability with moisture affinity in robust, biodegradableDESs.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1141–1149"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923939","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Toward Transformative Ambient Rare Earth Metal Electrorefining: A Perspective on Electrolyte Design and Circular Processing 面向环境稀土金属电解精炼:电解液设计和循环处理的观点
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-25 DOI: 10.1021/acsmaterialsau.6c00091
Abderrahman Atifi
{"title":"Toward Transformative Ambient Rare Earth Metal Electrorefining: A Perspective on Electrolyte Design and Circular Processing","authors":"Abderrahman Atifi","doi":"10.1021/acsmaterialsau.6c00091","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00091","url":null,"abstract":"<p>Ambient electrochemical production of rare earth metals(REMs)in organic electrolytes has emerged as a promising alternative toconventional high-temperature and chemically intensive processes.Over the past two decades, a limited number of research groups havedemonstrated the feasibility of REM electrodeposition under room temperatureconditions. However, practical implementation remains limited by challengesin metal stability, selectivity, electrolyte performance, and scalability.This perspective critically assesses reported ambient REM electrochemicalsystems, including ionic liquid, solvent-based, ligand-coordinated,and mediated strategies. Particular attention is given to effortstoward coupling REM production with rare earth element recovery, includingdirect and indirect electrorefining of spent NdFeB magnets. Whileconceptually promising, these approaches reveal key limitations, suchas complex hydrometallurgical processing, limited anodic dissolutionand loss of REM selectivity. Another central focus is the insufficientvalidation of electrodeposition product quality and performance, asreported characterization techniques often provide inconclusive evidenceregarding purity and metallic REM formation. Future progress requiresintegrated advances in coordination chemistry, interfacial electrochemistry,electrolyte and electrode design, alongside process engineering andtechnoeconomic assessment. Within this framework, a conceptual M2REM(Magnet-To-Rare Earth Metal) is illustrated as an example of integratedelectrorefining platform for the direct and ambient transformationof spent magnets into REMs, paving the way for energy-efficient andcircular rare earth metal processing.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"927–938"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Photocurable Polymer Coatings from Renewable Sources – Perspective Applications for Electronics, Surface Protection, and Advanced Systems 可再生材料的光固化聚合物涂层——电子、表面保护和先进系统的前景应用
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-15 DOI: 10.1021/acsmaterialsau.6c00087
Vojtěch Jašek, Radek Přikryl
{"title":"Photocurable Polymer Coatings from Renewable Sources – Perspective Applications for Electronics, Surface Protection, and Advanced Systems","authors":"Vojtěch Jašek,&nbsp;Radek Přikryl","doi":"10.1021/acsmaterialsau.6c00087","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00087","url":null,"abstract":"<p>The photocurablecoating industry relies mostly on fossil-based,high-performing, and multifunctional polymerizable systems, oftencomprising acrylic, epoxy, polyurethane, and unsaturated structuralcomponents suitable for efficient photopolymerization, exhibitingstable chemical structures and sufficient reproducibility. This workoffers a broad discussion of reactive systems derived and synthesizedfrom renewable sources. The main aim is to introduce different structuralprecursors and employ various photopolymerization strategies, includingradical and cationic polymerization and thiol–ene photocuring.Besides the reported inventions of biobased photocurable precursors,exemplified only by assisting matrices and the substitution of petroleum-derivedphotopolymerized materials, our work targeted and evaluated functionalcomponents from renewable sources and introduced their irreplaceableand unique purpose across commercial, material, and advanced applicationsincorporating photocurable polymer coatings. We divided the discussedprecursors into utility-focused subsections and comprehensively evaluatedtheir primary roles in the application fields.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"912–926"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Revisiting Vertical Orientation in Block Copolymer Complexes through Controlled Solvent Vapor Annealing 通过控制溶剂蒸汽退火重新研究嵌段共聚物配合物的垂直取向
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-06-26 DOI: 10.1021/acsmaterialsau.6c00018
Chizoba Livina Iheme, Nayanathara Hendeniya, Sharif Tasnim Mahmud, Shabari Dutta, Gabriel Mogbojuri, Shaghayegh Abtahi, Gregory Doerk, Boyce S. Chang
{"title":"Revisiting Vertical Orientation in Block Copolymer Complexes through Controlled Solvent Vapor Annealing","authors":"Chizoba Livina Iheme,&nbsp;Nayanathara Hendeniya,&nbsp;Sharif Tasnim Mahmud,&nbsp;Shabari Dutta,&nbsp;Gabriel Mogbojuri,&nbsp;Shaghayegh Abtahi,&nbsp;Gregory Doerk,&nbsp;Boyce S. Chang","doi":"10.1021/acsmaterialsau.6c00018","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00018","url":null,"abstract":"<p>Block copolymers (BCPs) are macromolecules made up oftwo or morechemically different polymer blocks that are covalently bound together.Their mutual incompatibility causes them to separate into nanoscalemicrophases, which allows the blocks to self-assemble into orderedshapes, such as lamellae, spheres, and cylinders. The ability to self-assembleoffers a versatile route for forming well-ordered nanoscale architecturesrelevant to nanolithography, membranes, and functional materials.Incorporating hydrogen-bonding small molecules to form supramolecularBCP complexes expands structural diversity by altering domain size,interfacial energies, and chain mobility. These complexes expand therange of parameters for precise control over nanoscale morphologywhile also providing highly ordered nanostructures that can be usedas soft templates for the formation of inorganic films and porousnetworks. However, the added complexity raises challenges in obtainingvertically oriented nanostructures, which are crucial in nanopatterningapplications. In the case of solvent vapor annealed films, the effectof swelling parameters on vertical orientation has not been thoroughlyinvestigated. Here, we demonstrate that swelling-induced surface neutralitypromotes vertical orientation in PS-<em>b</em>-P4VP(PDP) thinfilms, where P4VP(PDP) is the majority block and PS the minority block.Morphological transitions were observed, including horizontal, mixed,and vertical orientations, as film thickness, PDP ratio, and swellingratio were varied. A swelling ratio window ranging from ∼1.6 to 1.8 that reliably stabilizes vertical orientation was discovered.Significantly, vertical structures require a balance between selectiveswelling for surface energy neutrality and sufficient chain mobilityfor domain re-organization. These findings depart from previous reportswhere the formation of hierarchical lamellar structures within P4VP(PDP)was described as a key requirement for vertical orientation. Overall,this study identified solvent and wetting parameters that influencethe BCP orientation, thereby advancing supramolecular block copolymerthin films for nanopatterning and functional material applications.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1087–1097"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pyrimidine-Mediated Electronic Modulation of Ionic Carbon Nitrides for Green Light-Driven Photocatalysis 嘧啶介导的离子氮化碳的电子调制在绿光驱动光催化中的应用
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-07-03 DOI: 10.1021/acsmaterialsau.6c00080
Anna Lo Presti, Serge Arnold Benedoue, Sonia Zoltowska, Sue-Faye Ng, Sergio Navalón, Christian Mark Pelicano
{"title":"Pyrimidine-Mediated Electronic Modulation of Ionic Carbon Nitrides for Green Light-Driven Photocatalysis","authors":"Anna Lo Presti,&nbsp;Serge Arnold Benedoue,&nbsp;Sonia Zoltowska,&nbsp;Sue-Faye Ng,&nbsp;Sergio Navalón,&nbsp;Christian Mark Pelicano","doi":"10.1021/acsmaterialsau.6c00080","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00080","url":null,"abstract":"<p>Solar-driven organic transformations offer a sustainablestrategyfor the synthesis of high-value fine chemicals. However, most photoredoxsystems rely on high-energy light and costly molecular photosensitizers.Developing robust heterogeneous photocatalysts capable of efficientoperation under low-energy visible light remains a critical challenge.Herein, we present a pyrimidine-mediated electronic modulation strategyto engineer ionic carbon nitrides for green-light-driven photocatalysis.Incorporation of 2,4,6-triaminopyrimidine during the thermal polymerizationof potassium poly(heptazine imide) induced controlled carbon dopingwithin the framework, enabling band structure tuning, extended visible-lightabsorption, and enhanced charge separation and transport. The optimizedmaterial (0.5T-K) exhibited significantly improved photophysical properties,which translated into efficient catalytic performance under green-lightirradiation. As a representative demonstration, the material enabledC–N cross-coupling with up to 99% conversion and sustainedactivity in extended reactions, while maintaining good recyclability.This work establishes a general strategy for tailoring the electronicstructure of ionic carbon nitrides and highlights their potentialas efficient, fully heterogeneous photocatalysts for low-energy, sustainablephotoredox transformations.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1131–1140"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148915831","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ligand-Driven Structural Control in Rare Earth-TNDI MOFs: Topological Diversity and Mixed Matrix Membranes for Real-Time Amine Detection 配体驱动的稀土- tndi mof结构控制:用于实时胺检测的拓扑多样性和混合基质膜
IF 9.1
ACS Materials Au Pub Date : 2026-09-09 Epub Date: 2026-05-16 DOI: 10.1021/acsmaterialsau.6c00020
Govu Radha, Ayalew H. Assen, Vincent J. Smith, Himanshu Aggarwal
{"title":"Ligand-Driven Structural Control in Rare Earth-TNDI MOFs: Topological Diversity and Mixed Matrix Membranes for Real-Time Amine Detection","authors":"Govu Radha,&nbsp;Ayalew H. Assen,&nbsp;Vincent J. Smith,&nbsp;Himanshu Aggarwal","doi":"10.1021/acsmaterialsau.6c00020","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.6c00020","url":null,"abstract":"<p>Rare-earth (RE) MOFs are notable for their structuraltunabilityand diverse connectivity, making them promising for applications ingas separation, storage, and sensing. This work reports two new isostructuralRE-based MOFs, Y-TNDI and Eu-TNDI, synthesized by using a rigid tetracarboxylatelinker bearing a naphthalenediimide (TNDI) core. Unlike their Zr-TNDIcounterpart, which features a single 4-c hexanuclear cluster and structuralinterpenetration, the RE-TNDI MOFs possess dual molecular buildingblocks: an 8-c hexanuclear cluster (RE<sub>6</sub>) and a 4-c mononuclearRE center. This discovery challenges the notion that dual-clusterformation arises solely from a linker asymmetry, showing that a symmetricrigid TNDI linker can also give rise to such structural heterogeneity.Building on this structural ingenuity, we investigated the Eu-TNDIMOF for the rapid and visual detection of volatile organic amines,chemicals with well-documented health hazards. The MOF displayed analmost 100% quenching efficiency. Interestingly, the MOF exhibitsphotochromic behavior upon exposure to visible light due to the formationof radicals, as confirmed by EPR. When embedded in a mixed-matrixmembrane, this MOF exhibits remarkable colorimetric changes upon exposureto amines, transforming molecular design into an effective strategyfor real-time detection. This work underscores the crucial role ofmetal and ligand selection as well as the structural characteristicsof RE MOFs in driving advancements in both materials science and environmentalmonitoring.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"6 5","pages":"1098–1109"},"PeriodicalIF":9.1,"publicationDate":"2026-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148923876","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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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