Accounts of materials research最新文献

{"title":"Design of a Catalyst\u0000of Multiple Single-Atom Sites\u0000through the Synergic Effect for Chemical Transformation and Fuel Production","authors":"Felix F. Tao,Xupeng Zong,Takat B. Rawal","doi":"10.1021/accountsmr.6c00032","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00032","url":null,"abstract":"Conspectus We defined the synergic effect in single-atom catalysis and demonstrated that the catalytic performance of a reaction involving two or more reactants (R1 + R2 → P) on a catalyst of multiple single-atom sites (CatM1+A1) can benefit from the coexistence of two types of single-atom sites M1α and M1β if they are responsible for activating reactants R1 and R2, respectively. The kinetics feature is that the activation barrier [Ea(CatM1+A1)] of this catalyst is lower than that of a catalyst with only one type of single-atom site [Ea(CatM1or CatA1)]. Such a catalyst can be prepared through coprecipitation/deposition, sequential precipitation/deposition, or atomic layer deposition. The synergistic effect of two types of single-atom sites on a support makes it possible to catalyze a reaction at a thermodynamically allowed low temperature. One example of such catalytic materials is Mo1+Pd1/Co3O4 consisting of two sets of single-atom sites Pd1Ox and Mo1Oy, and a support, Co3O4. While the Pd1 site activates H2 to form atomic H, the Mo1 site responds by activating C–O of C6H5OCH3 to form C6H5. The H atoms formed on the Pd1 site can diffuse on Co3O4 to couple with C6H5, leading to the formation of benzene at 110 °C. In contrast, Pd nanoparticles are not active for anisole HDO at 110 °C since Pd atoms of Pd nanoparticles preferentially chemisorb atomic H but do not activate the C–O bond of anisole at 110 °C. Another type of synergic effect in single-atom catalysis is the coupling between the role of each of the two types of single-atom sites in the catalytic cycle of a reaction. For instance, the two types of single-atom sites, Ni1Oa and Ru1Ob on CeO2 (Ce0.90Ni0.05Ru0.05O2), play a synergistic role in methane steam reforming (MSR) in which Ni1Oa is responsible for activating CH4 to form CH3, CH2O, CHO, and then CO. The oxygen vacancy on the CeO2 surface is refilled by O of H2O through the activation and dissociation of H2O by Ru1 and its adjacent oxygen vacancy (Ru1 + OVac); the synergistic role of Ni1Oa and Ru1+Ovac makes MSR occur at 500 °C, bringing the high working temperature of the solid oxide fuel cell of methane down to an intermediate temperature. A synergic effect can occur between two of the same type of single-atom sites anchored on two different supports. The two single-atom sites (M1/Zα and M1/Zβ) have different reactivities since they have different chemical and coordination environments. An intermediate of reactant A formed on a single-atom site M1 anchored on one support (M1/Zα) can spillover to another support (Zβ) to couple with the intermediate of reactant B formed on another type of single-atom site (M1/Zβ), enabling a synergistic effect of the two types of single-atom sites anchored on different supports (M1/Zα and M1/Zβ). For instance, two Pd1 sites are anchored on C3N4 and SnO2, forming Pd1/C3N4 and Pd1/SnO2, respectively. Pd1/C3N4 activates H2 to form atomic H, whereas Pd1/SnO2 responds by activating O2. We discussed future ap","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149022064","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}

{"title":"Ladder-Type π-Conjugated Heteroatom-Reinforced Nanoarchitectonics: Transformative Materials for Imaging of Cellular Components","authors":"Linawati Sutrisno,Masayasu Taki,Katsuhiko Ariga,Shigehiro Yamaguchi","doi":"10.1021/accountsmr.6c00184","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00184","url":null,"abstract":"Cell populations are inherently heterogeneous, and the molecular mechanisms that govern cellular plasticity and fate operate across broad spatial and temporal scales. Early signaling events emerge within seconds to minutes, whereas phenotypic transitions associated with differentiation, adaptation, and disease progression may unfold over hours, days, or longer. Elucidating these dynamic processes requires molecular imaging tools capable of quantitatively monitoring biochemical events with high spatial resolution, temporal precision, and molecular specificity in living systems. However, achieving this goal demands the integration of multiple design principles that are rarely realized within a single molecular platform. Therefore, the development of such tools remains a central challenge in chemical biology because molecular recognition, fluorescence signaling, organelle targeting, and photostability must be integrated within a single molecular architecture. In this Account, we present a historical overview of the evolution of our unique molecular imaging toolbox, tracing its development from fundamental studies of molecular recognition in artificial systems to multiplex visualization of organelle dynamics in living cells, and ultimately to their successful translation into bioimaging probes. Our early efforts established how hydrogen-bonding interactions at artificial lipid membrane interfaces can be exploited to enhance biomolecular recognition under aqueous conditions. These studies further revealed that tuning membrane mechanical properties provides a powerful strategy for discriminating structurally similar nucleotide targets and regulating selective molecular recognition. The principles derived from these artificial systems were subsequently extended to fluorescence sensing platforms for recognition of biologically relevant analytes. Building upon these molecular recognition strategies, we developed heteroatom-containing π-conjugated fluorophores in which phosphorus, sulfur, and nitrogen elements were strategically incorporated into ladder-type π-conjugated compounds to modulate electronic structure, fluorescence properties, and bioimaging performance. Systematic molecular engineering transformed these fluorophores from intracellular ion sensors into highly selective organelle-targeting probes and, ultimately, multiplex imaging platforms capable of simultaneously visualizing dynamic interactions among multiple subcellular compartments. Importantly, heteroatom engineering also enabled exceptional photostability, allowing long-term imaging of gradual cellular transitions that are inaccessible with conventional probes. A recurring theme throughout this work is the rational integration of molecular components to bridge chemical structure and biological function. Through precise tuning of fluorophore scaffolds, linker architectures, molecular recognition motifs, and organelle-targeting units, we established modular design principles that govern in","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"269 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149013709","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}

{"title":"Determinants of Phase-Separation Propensities, Material States, and Material Properties of Biomolecular Condensates","authors":"Huan-Xiang Zhou","doi":"10.1021/accountsmr.6c00147","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00147","url":null,"abstract":"Phase separation of various materials has been studied for one and a half centuries, laying foundational principles in materials science. In the last two decades, phase separation of proteins and nucleic acids has received enormous attention, due to its relevance to cellular functions. Despite this explosion of empirical data, many observations on the resulting biomolecular condensates lack a rigorous theoretical underpinning. The first goal of this Account is to put forward theoretical frameworks for the phase-separation propensities, material states, and material properties of biomolecular condensates. Using these frameworks, I rationalize mechanistic interpretations in our recent experimental and computational studies, and synthesize these studies with prior literature to draw novel, unifying conclusions. To evaluate phase-separation propensities, I establish a direct relationship between the threshold (or saturation) concentration (Cth) and the excess chemical potential in the dense phase (μIIex). μIIex is fundamentally dictated by the collective strength and valency of intermolecular interactions. The relationship between Cth and μIIex readily rationalizes the effects of amino-acid composition and solvent conditions like temperature, pH, and salt on phase-separation propensities. Regarding material states, I posit that liquid droplets represent the completion of phase separation, whereas other states─including amorphous dense liquids, reversible aggregates, and gels─arise from premature termination of spinodal decomposition. Specifically, amorphous dense liquids occur near the critical point and early during spinodal decomposition, kinetically trapped as overly weak interactions prevent further condensation. Gels and aggregates are different forms of dynamically arrested states, one driven by directional interactions that favor tip growth, extending outward into system-spanning networks, the other driven by monomer addition at interior sites to maximize valency, producing densely packed, amorphous particles. For material properties, I highlight the crucial roles of the stress relaxation time (τ1), which is determined by the mean lifetime of intermolecular bonds in a condensate. This relaxation time dictates how the condensate manifests viscoelasticity, including shear thickening and shear thinning, and accounts for the wide variation in zero-shear viscosity (ηz) among different condensates. Indeed, I propose a correlation between ηz and τ1, which is supported by available data. I also devise a theoretical model to explain the relative constancy of surface tension. Given this constancy, the inverse fusion speed can be used as an indicator of viscosity. Validating and expanding these conclusions will further strengthen the theoretical foundations of the biomolecular condensate field. Looking forward, several high-impact opportunities emerge. First, it may be possible to bridge the persistent gap between all-atom molecular dynamics (MD) simulat","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"32 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973685","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}

{"title":"How High Ionic Conductivity Makes Low-Capacity Lithium Iron Chlorides Competitive","authors":"Kostiantyn V. Kravchyk,Maksym V. Kovalenko","doi":"10.1021/accountsmr.6c00215","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00215","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"150 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973684","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}

{"title":"Supramolecular Materials Based on Methylene-Linked Water-Soluble Macrocyclic Calixpyridinium and Pillarpyridinium","authors":"Kui Wang,Xiang Li,Yan-Xi Li","doi":"10.1021/accountsmr.6c00204","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00204","url":null,"abstract":"While transitioning supramolecular materials into aqueous environments is critical for biological and environmental applications, designing macrocyclic hosts that are simultaneously easy to synthesize, intrinsically water-soluble, and dynamically responsive remains a formidable challenge. Intrinsically water-soluble macrocycles constructed from bipyridinium or pyridinium cations linked via π-electron-conjugated groups are highly representative hosts, where a major limitation of the pioneering “Blue Box” is its susceptibility to irreversible structural decomposition in alkaline media, severely restricting its application scope. To overcome this fundamental limitation, extensive systematic exploration over the past decade has been dedicated to a unique class of non-π-electron-conjugated methylene-linked pyridinium macrocycles: calixpyridinium and pillarpyridinium. Both of these intrinsically water-soluble macrocycles are accessible via a simple one-step synthesis. Furthermore, calixpyridinium uniquely exhibits an extraordinary response to alkaline conditions without any skeletal decomposition.\u0000This Account chronicles our decade-long systematic efforts to translate these simple molecular building blocks into sophisticated, multiresponsive supramolecular materials. We begin by establishing the foundational rulebook governing host–guest binding. Crucially, beyond conventional factors such as the guest’s geometry, charge number, and size, we highlight our significant discovery that the π-electron-conjugated degree of the guest acts as a pivotal influencing factor, which broadened traditional guest selection criteria and vastly expanded the scope of viable guests for designing calixpyridinium-based supramolecular materials.\u0000While these noncovalent host–guest interactions enabled the construction of various supramolecular assemblies, the true watershed moment in our research was the discovery of an extraordinary, nondestructive structural transformation: under alkaline conditions or irradiation with 254 nm UV light, the acidic methylene of calixpyridinium undergoes a site-specific deprotonation. The deprotonation process triggers a cascade of profound changes. Specifically, the generated carbanions conjugate with adjacent pyridinium cations to yield unsaturated double bonds, not only enhancing the skeleton’s photoactivity but also facilitating the dynamic regulation of supramolecular morphologies. Moreover, the ability of the deprotonated skeleton to act as a dynamic proton acceptor makes it an exceptional building block for engineering biomimetic, far-from-equilibrium dissipative pathways. Furthermore, the resulting decrease in positive charge predictably weakens the host’s affinity toward anionic guests, which can be harnessed to develop smart nanocarriers for on-demand drug delivery. Finally, the transition from a colorless, nonfluorescent state to a highly π-electron-conjugated, brightly colored, and fluorescent state provides dual visual signals, fa","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"144 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973686","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}

{"title":"Element-Resolved Imaging of Electrochemical Materials with X-ray Fluorescence Microscopy","authors":"Yetong Jia, Dawei Xia, Changlian Wen, Feng Lin, Kejie Zhao, Luxi Li","doi":"10.1021/accountsmr.6c00091","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00091","url":null,"abstract":"<p>Electrochemical systems feature complex and spatially heterogeneouselemental distributions that evolve during operation. Revealing theseelemental dynamics is critical to understanding operation and degradationmechanisms, and thus to improving energy storage and conversion systems.X-ray fluorescence microscopy (XFM) provides a powerful, nondestructive,and element-specific probe for mapping elemental distributions withspatial resolution across relevant length scales. These capabilitiesenable XFM to address key questions in electrochemical materials research,including materials synthesis and compositional engineering, post-mortemanalysis of aged materials, and operando visualization of elementalredistribution during electrochemical processes.</p><p>In this Account,we first introduce the mechanics and experimentalsetup of XFM, followed by its major capabilities and applicationsin electrochemical systems. We highlight its element specificity,high sensitivity, multielement detection, penetration power, and compatibilitywith operando and nondestructive measurements, which together makeit suitable for probing complex and spatially heterogeneous electrochemicalmaterials. We also compare XFM with other elemental analysis techniquesto clarify its distinctive advantages. We then summarize ex situ XFMstudies of electrochemical materials. In materials design and compositionalengineering, XFM can directly verify whether intended elemental architecturesare successfully realized, including surface coatings, elemental doping,and concentration-gradient designs in battery electrodes. This capabilityis important because the performance of engineered materials oftendepends not only on the presence of specific elements but also ontheir spatial distribution. In postcycling analysis, XFM reveals unintendedelemental redistribution associated with degradation, such as transition-metaldissolution and deposition, polysulfide migration, electrolyte heterogeneity,and the formation of spatially localized reaction products or byproducts.These examples show how XFM connects elemental heterogeneity withelectrochemical function and failure mechanisms. We further highlightoperando and in situ XFM studies that directly visualize dynamic elementalevolution in working electrochemical systems. These studies are discussedin two categories: elemental evolution within bulk electrochemicalmaterials and interfacial processes at electrode–electrolyteinterfaces. By repeatedly probing the same region during operation,XFM can track dynamic electrochemical phenomena such as dissolution–redeposition,reversible and irreversible phase evolution, and elemental diffusionlayers, which are difficult to reconstruct from post-mortem analysisalone. Dynamic behavior captured by XFM enables the correlation ofspatial, temporal, and compositional information with electrochemicalperformance.</p><p>Following representative scientific case studies,we finally discussthe current limitations and future opportuni","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 8","pages":"860–870"},"PeriodicalIF":14.1,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148858965","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}

{"title":"Probing the Frontiers of Nanoscale Thermal Transport with Transient Thermal Gratings and Atomistic Green’s Function Simulations","authors":"Chen Li,&nbsp;Zhiting Tian","doi":"10.1021/accountsmr.5c00352","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00352","url":null,"abstract":"<p>The relentless increase in powerdensity and advancements in nanoengineeringin modern electronic and energy conversion technologies have pushedthermal management to its physical limits, where ballistic transportphenomena and the wave nature of phonons become important. Our researchtackles this frontier using a dual approach: advanced experimentaltools to accurately probe thermal transport across ballistic and diffusiveregimes, and predictive theoretical methods to resolve wave-basedphonon transport with atomic precision.</p><p>On the experimentalfront, transient thermal grating (TTG) spectroscopyhas emerged as a crucial noncontact optical technique for probingcomplex material systems that are inaccessible to other methods, includingnew classes of materials such as two-dimensional (2D) covalent organicframeworks (COFs) and hybrid perovskites. Studying in-plane thermaltransport in these materials is particularly challenging due to theirsmall dimensions or fragility. On the theoretical front, the atomisticGreen’s function (AGF) is a quantum-mechanical framework thatdescribes phonon transport as wave propagation and accounts for interactionswith the atomic structure, defects, and interfaces from first-principles,providing fundamental physical insights.</p><p>This Account summarizeshow we leveraged TTG and AGF for scientificdiscoveries. For instance, we used TTG to directly measure the in-planethermal conductivity of novel 2D COFs, revealing a high value of ∼1.18 W/(m·K). We also applied TTG to unveil remarkably weak anisotropyof 1.5 in thermal conductivity of 2D hybrid perovskites. Furthermore,we developed TTG to uniquely characterize micrometer-thick metallicinterfaces, smaller than the laser beam size. In the theoretical domain,we developed anharmonic AGF method for three-dimensional (3D) interfacesand discovered enhanced thermal interface conductance due to anharmonicityat the interface. We also found enhanced conductance due to a bridgingeffect caused by atomic mixing. We applied AGF to directly capturephonon Anderson localization in aperiodic superlattices and coherentphonon transport in periodic superlattices. The collective insightsgained from these distinct experimental and theoretical advances arebuilding a framework for the rational design of materials with tailoredthermal transport properties, paving the way for next-generation solutionsin electronics packaging, thermoelectrics, thermal insulation, andbeyond.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 8","pages":"819–831"},"PeriodicalIF":14.1,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148858950","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}

{"title":"Shaping a Circular Future with Bio-derived Resins in Additive Manufacturing","authors":"Arianna Brandolese,&nbsp;Thiago O. Machado,&nbsp;Andrew P. Dove","doi":"10.1021/accountsmr.5c00354","DOIUrl":"https://doi.org/10.1021/accountsmr.5c00354","url":null,"abstract":"&lt;p&gt;The integrationof circular principles into chemical manufacturingis poised to significantly transform the production of plastics. Thisshift will have impacts across the value chain, including raw materialsourcing, recyclability, and cost. In recent years, interest in photopolymer-basedadditive manufacturing (AM) has grown, driven by the increasing demandfor multifunctional 3D printing. Photopolymer printing is widely appliedin academia and industry as it provides high resolution and rapidprint speeds and allows for the construction of plastic products withcomplex geometries. Therefore, in addition to the benefits of usingenergy from light, rather than higher energy thermal curing, to createthe printed materials, AM offers the advantages of waste reductionthrough dematerialization. Among the photopolymer-based AM techniques,digital light processing (DLP) is commonly applied due to its highaccuracy and resolution and low capital cost for equipment. Whileadvances in equipment are making production-scale photopolymer printinga reality, resin design is largely embedded in the chemistry of thepast. However, the nascent state of this industry presents an opportunityto embed sustainability within its material set as it grows, preventingmany of the environmental and human health impacts that are linkedwith the current use of petrochemically derived plastics. While furtheringfunctionality or performance of the materials produced remains anongoing target for the field, to enhance its sustainability credentialsresearch is focused on (i) switching from petrochemical to biomass-derivedmonomer feedstocks and (ii) enhancing material circularity such thatresins can be printed, depolymerized, and re-printed in a closed-loop,circular manner. Achieving these milestones requires considerationof resin feedstock sourcing and the design of monomers with dynamicbonds to enable recyclability and reprocessability.&lt;/p&gt;&lt;p&gt;To expandthe portfolio of biomass-derived photopolymer resins,we, along with others, have explored the use of bio-derived and bio-derivable(i.e., those chemical feedstocks that have the potential to be bio-derivedbut at present are not) monomers that are easily derivatized and compatiblewith DLP systems. Typical approaches leverage the reactive functionalgroups in bio-derived monomer sources to create acrylates or epoxidesthat enable rapid crosslinking, to achieve high-quality 3D-printedpolymers. Our approach has focused on leveraging double bonds thatnaturally occur in biomass-derived chemicals to reduce the numberof reaction steps by promoting polymer formation through direct reactionof that double bond via thiyl radical addition chemistry. This step-growthaddition method has enabled us to create materials that can be fullydegraded to small molecules, but it has also provided opportunitiesto leverage double-bond stereochemistry to achieve photosets withtunable mechanical properties. Monomer bio-sourcing, however, onlyaddresses half of the problem─the a","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 8","pages":"808–818"},"PeriodicalIF":14.1,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148858953","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}

{"title":"Cucurbituril-Mediated Conformational Control: From Molecular Manipulation to Functional Applications","authors":"Dongdong Sun,&nbsp;Xie Han,&nbsp;Simin Liu","doi":"10.1021/accountsmr.6c00108","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00108","url":null,"abstract":"&lt;p&gt;Molecular conformation is afundamental determinantof intramolecularinteractions, reactivity, and conjugation extent in organic molecules,directly influencing properties ranging from photophysical characteristicsto chemical reactivity. Consequently, precise control over molecularconformation represents both a significant challenge and opportunityin organic chemistry and materials science, enabling the rationaldesign of functional materials. Beyond covalent modifications suchas steric group incorporation, molecular conformation can also beeffectively regulated through noncovalent host–guest complexationin supramolecular chemistry. Among the various supramolecular toolsavailable, the cucurbit[&lt;em&gt;n&lt;/em&gt;]uril (CB[&lt;em&gt;n&lt;/em&gt;], &lt;em&gt;n&lt;/em&gt; = 5–8, 10) family of synthetic macrocycleshas emerged as a powerful tool for conformational manipulation. CB[&lt;em&gt;n&lt;/em&gt;] hosts feature rigid, hydrophobic cavities and electronegativecarbonyl portals, providing excellent binding affinity and selectivitytoward cationic guest molecules through a combination of hydrophobiceffects, ion–dipole interactions, and hydrogen bonding. Largerhomologues such as CB[7], CB[8], and CB[10] possess cavities capableof encapsulating and precisely manipulating molecular conformationsthrough host–guest interactions, thereby profoundly alteringguest properties. The evolution of CB[&lt;em&gt;n&lt;/em&gt;] hosts fromsimple molecular containers to conformational regulators has enabledthe construction of diverse functional supramolecular materials. Recently,numerous supramolecular assemblies have been developed through CB[&lt;em&gt;n&lt;/em&gt;]-mediated conformational control.&lt;/p&gt;&lt;p&gt;This Account providesan overview of recent fundamental advancesand applications in CB[&lt;em&gt;n&lt;/em&gt;]-mediated conformationalcontrol, establishing clear structure–property relationshipsbetween conformation manipulation and material functionality. We categorizeCB[&lt;em&gt;n&lt;/em&gt;]-mediated conformationally adaptive guest moleculesinto five representative paradigms, each demonstrating a distinctmode of conformational modulation: the induced U-shaped folding offlexible alkyl chains within the hydrophobic cavity, the folded conformationof charge-transfer complexes within CB[&lt;em&gt;n&lt;/em&gt;], controllablephotoresponsiveness of diarylethene molecular photoswitches, controlledtwisting of sterically constrained molecules, and linear donor–acceptortype molecules. Through a careful evaluation of selected examples,we demonstrate that CB[&lt;em&gt;n&lt;/em&gt;] functions as a conformationalregulator rather than merely a molecular container with the confinedmicroenvironment effectively shifting the conformation into normallydisfavored states. More importantly, this complexation process yieldshost–guest systems with unique properties markedly differentfrom the free guest molecules, including tunable fluorescence or roomtemperature phosphorescence (RTP) emission as well as different responsivebehaviors toward light and external mechanical stimulation. We furtherexplore the appl","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 8","pages":"871–883"},"PeriodicalIF":14.1,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148859066","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}

{"title":"Marine-Coating-Sourced Microplastics: A Long-Standing yet Overlooked Global Issue","authors":"Qingyi Xie,&nbsp;Chunfeng Ma","doi":"10.1021/accountsmr.6c00130","DOIUrl":"https://doi.org/10.1021/accountsmr.6c00130","url":null,"abstract":"","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"7 8","pages":"792–795"},"PeriodicalIF":14.1,"publicationDate":"2026-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148858951","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}