化学最新文献

{"title":"Interplay between Thermal Denaturation and Dynamic Covalent Chemistry Generates High-Performance Recyclable Protein Plastics","authors":"Youwei Ma,&nbsp;Francesco Stellacci","doi":"10.1021/acsmacrolett.6c00434","DOIUrl":"10.1021/acsmacrolett.6c00434","url":null,"abstract":"<p>Chemically recyclable and/or biobased polymers are promisingalternativesto conventional petroleum-derived plastics, yet strategies that simultaneouslyimprove their performance and recyclability remain scarce. Here, wereport that the combined use of thermal denaturation and dynamic covalentchemistry can transform protein materials into strong, chemicallyrecyclable bioplastics with enhanced hydrolytic stability. Cross-linking <em>a priori</em> brittle bovine serum albumin (<strong>BSA</strong>)with dynamic vinylogous urethane (<strong>VU</strong>) linkages producesrobust plastics with tensile strengths of up to 35 MPa. Simultaneously,thermal denaturation at 80 °C restructures <strong>BSA</strong> fromα-helices into more hydrophobic β-sheet-rich domains,reducing water absorption and thereby stabilizing the otherwise hydrolyzable <strong>VU</strong> cross-links. The resulting protein networks are chemicallyrecyclable in acidic water, allowing the recovery of both <strong>BSA</strong> and cross-linkers. Overall, by exploiting the reciprocal interplaybetween dynamic covalent cross-linking and protein thermal denaturation,this work offers a fresh perspective to overcome the trade-off betweenpolymer stability and recyclability.</p>","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"15 10","pages":"1558–1564"},"PeriodicalIF":4.9,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092472","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":"Interfacial Confinement Enables Dual Hosting of Sulfur Mustard and Mustard Sulfoxide in NU-1000","authors":"Farrah S. McCormick,&nbsp;Liangliang Huang","doi":"10.1021/acs.langmuir.6c04057","DOIUrl":"10.1021/acs.langmuir.6c04057","url":null,"abstract":"<p>Zirconium-based metal–organicframeworks have emerged aspromising materials for the capture and detoxification of chemicalwarfare agents, but the molecular mechanism by which a hierarchicalMOF differentiates a hydrophobic reactant from its oxidized productremains incompletely understood. Here, we use molecular dynamics simulations,grand-canonical Monte Carlo adsorption calculations, and periodicdensity functional theory to examine the dual-hosting behavior ofNU-1000 toward sulfur mustard (HD) and mustard sulfoxide (HDO). Ratherthan treating NU-1000 only as an adsorbent or oxidation catalyst,we resolve how its internal micropore, mesopore, and c-pore interfacesimpose distinct confinement environments on reactant and product species.Density functional theory (DFT) calculations show that HD binds mostfavorably in the c-pore region, with a binding energy of approximately−12.5 kcal/mol, and similarly favorable stabilization in confinedmicropore environments, whereas substantially weaker binding is observedin the mesopore. Molecular dynamics simulations also reveal sharplydifferent pore residence patterns: HD localizes predominantly in micropores,occupying this region for ∼80% of the trajectory, while HDOsamples larger pore environments more broadly, with ∼45% mesoporeand ∼34% c-pore occupancy. This pore-selective behavior persistsunder mixed HD/HDO coadsorption conditions, demonstrating that reactant–productdifferentiation is intrinsic to the NU-1000 pore network rather thanan artifact of isolated single-component simulations. Radial distributionfunctions further show that HD is stabilized by dispersion-dominatedconfinement and weak halogen–hydrogen contacts, whereas HDOis governed by more localized, orientation-dependent interactionswith hydrated zirconium node sites. These interaction differencesproduce a pronounced transport asymmetry, with HDO exhibiting a self-diffusioncoefficient of 10.6 ± 2.11 × 10^–10 m²/s compared with 0.5 ± 0.09 × 10^–10 m²/s for HD at comparable loading. The results identifyNU-1000 as a dual-function molecular host that couples reactant retentionwith product mobility, providing an interface-level mechanism relevantto selective CWA detoxification and confined transport in hierarchicalporous catalysts.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"42 41","pages":"30833–30846"},"PeriodicalIF":4.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effect of Vibration on Droplet Impact Dynamics on Superhydrophobic Surfaces under Moderate Low Pressure","authors":"Jiwen Wang,&nbsp;Hongbin Liu,&nbsp;Zehua Xu,&nbsp;Yanbin Zhang,&nbsp;Xiaosen Wang,&nbsp;Qiang He","doi":"10.1021/acs.langmuir.6c04959","DOIUrl":"10.1021/acs.langmuir.6c04959","url":null,"abstract":"<p>The rebound behavior of dropletsimpacting superhydrophobicsurfacesis ubiquitous in natural and industrial processes and is closely associatedwith a wide range of practical applications. In special applicationscenarios such as aircraft and high-altitude equipment, surfaces areoften subjected to both vibration and low pressure. However, existingstudies are mostly based on atmospheric pressure or stationary surfaces.It remains unclear how moderate low pressure and external vibrationjointly affect droplet spreading. In this work, high-speed photographywas employed to first investigate the impact dynamics of dropletson a stationary superhydrophobic surface under low pressures (97,74.6, and 60 kPa). The influence of pressure on the spreading processwas examined. Subsequently, at 60 kPa, the effects of vibration phase,frequency, and amplitude on droplet impact were studied. The resultsshow that the maximum spreading coefficient increases gradually withdecreasing pressure. This can be attributed to the reduction of gas-phasedissipation during droplet spreading under low pressure. Meanwhile,vibration introduces an additional phase-dependent energy input mechanism.The maximum spreading coefficient exhibits a pronounced periodic variationwith the initial phase angle. Moreover, as the vibration frequencyand amplitude increase, the fluctuation of the maximum spreading coefficientwith phase becomes more significant. Based on energy conservationanalysis, an empirical mathematical model was developed for the maximumspreading diameter of a droplet impacting a vibrating superhydrophobicsurface under low pressure. The model elucidates the regulatory mechanismsby which pressure and vibration modulate energy input and dissipationduring impact. This study contributes to understanding the interfacialdynamics of droplet impact under coupled low-pressure and vibrationconditions, and provides useful insights into droplet impact behaviorunder relevant environmental conditions.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"42 41","pages":"31077–31089"},"PeriodicalIF":4.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Multiscale Investigation and Mechanistic Insights into TiO2@CoAl-LDH-Modified Asphalt for the Photocatalytic Degradation of NOx","authors":"Canlin Zhang,&nbsp;Peng Jin,&nbsp;Ting Wang,&nbsp;Minxuan Chen,&nbsp;Zhengyang Fang,&nbsp;Zenghua Sun,&nbsp;Peng Xia","doi":"10.1021/acs.langmuir.6c03522","DOIUrl":"10.1021/acs.langmuir.6c03522","url":null,"abstract":"<p>For the eco-friendly asphalt pavements with NO_<em>x</em> degradation performance, TiO₂@CoAl-LDHswere preparedand applied as asphalt modifiers. X-ray diffraction (XRD) and X-rayphotoelectron spectroscopy (XPS) indicated that TiO₂ wasuniformly loaded onto the surface of the CoAl-LDHs, and TiO₂@CoAl-LDHs have been successfully synthesized. The integration ofTiO₂ and CoAl-LDHs reduced the energy barrier for electron–holepair formation upon light irradiation, resulting in the stronger absorbanceof TiO₂@CoAl-LDHs in both ultraviolet and visible lightranges. After combining TiO₂ with CoAl-LDHs, the photogeneratedelectron transfer and separation efficiency of TiO₂@CoAl-LDHswere significantly enhanced, and the recombination of electron–holepairs was concomitantly suppressed. Compared with TiO₂ andCoAl-LDHs, TiO₂@CoAl-LDH-modified asphalt exhibited strongerinteraction with NO_<em>x</em>. Meanwhile, NO_<em>x</em> diffused more easily and had a larger penetrationproportion in TiO₂@CoAl-LDH-modified asphalt. All of thesecontributed to better NO_<em>x</em> photocatalyticdegradation capability of TiO₂@CoAl-LDH-modified asphalt.This study promotes the development of eco-friendly asphalt pavements.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"42 41","pages":"30663–30675"},"PeriodicalIF":4.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150931","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Periodic Thermal Oscillation Induces Mesoscale Soft Aggregates in a Fully Miscible Ethanol–Water Liquid","authors":"Xinyue Jiang,&nbsp;Yating Shang,&nbsp;Jianhui Li,&nbsp;Zhaoyong Zou,&nbsp;Yanxia Zuo,&nbsp;Yuqun Xie","doi":"10.1021/acs.langmuir.6c05269","DOIUrl":"10.1021/acs.langmuir.6c05269","url":null,"abstract":"<p>Inducing and stabilizing mesoscale structures in fullymisciblemolecular liquids remains challenging because local heterogeneityis usually transient and rapidly averaged out. Here, we show thatperiodic thermal oscillation drives a 50% (v/v) ethanol–watermixture along a traceable nonequilibrium ordering pathway from transientethanol–water clusters to kinetically stabilized soft aggregates.The system evolves from initial clusters to water-containing dropletsas liquid–liquid microphase-separated intermediates, then toethanol-rich acicular flakes, and ultimately to micron-scale flake-stackedaggregates. Fluorescence spectroscopy, two-dimensional correlationanalysis, and nuclear magnetic resonance reveal that this processbegins with perturbation and relaxation of the water-dominated hydrogen-bondnetwork, proceeds through a water–ethanol coassociated intermediate,and culminates in ordered ethanol aggregates. Thermal analysis andin situ Raman spectroscopy further show progressive stabilizationacross the structural hierarchy. These findings demonstrate that periodicthermal forcing can amplify transient molecular heterogeneity intomesoscale soft structures in a fully miscible liquid, providing akinetic perspective on nonequilibrium cluster amplification and microphase-separatedaggregate formation in hydrogen-bonded molecular systems.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"42 41","pages":"31141–31151"},"PeriodicalIF":4.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Buried-Interface Dipole Modulation and Conductive Nanofiber Engineering for High-Performance Flexible Perovskite Solar Cells","authors":"Chenyang Shi,&nbsp;Wen Guo,&nbsp;Jinhuan Jiang,&nbsp;Ruizhi Duan,&nbsp;Lixin Song,&nbsp;Jie Xiong","doi":"10.1021/acs.langmuir.6c04654","DOIUrl":"10.1021/acs.langmuir.6c04654","url":null,"abstract":"<p>Flexible perovskite solar cells (f-PSCs) suffer fromburied-interfaceenergy-level mismatch, severe interfacial recombination, and inefficientcharge transport, which limit both device efficiency and stability.Herein, we develop a synergistic strategy by integrating a trimethoxy[3-(phenylamino)propyl]silane (TEPAPS) dipole interlayer with conductive SnO_<em>x</em>/C nanofibers (NFs) to simultaneously regulate theburied interface and perovskite bulk. The TEPAPS interlayer reducesthe work function, improves energy-level alignment, and passivatesinterfacial Pb²⁺ defects. Meanwhile, TEPAPS-modified SnO_<em>x</em>/C NFs act as conductive one-dimensionalframeworks and crystallization templates, promoting grain growth,reducing defect density, and establishing efficient charge-transportpathways throughout the perovskite layer. As a result, nonradiativerecombination is effectively suppressed and carrier extraction isaccelerated. Owing to the synergistic effects of interfacial dipolemodulation and conductive nanofiber engineering, the optimized rigiddevice and flexible devices achieve power conversion efficiencies(PCEs) of 24.11% and 21.63%, respectively. Moreover, the flexibledevice retains 88.2% of its initial efficiency after 600 bending cycles.This work provides an effective approach for simultaneously engineeringburied-interface energetics and bulk charge transport for high-performanceflexible perovskite photovoltaics.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"42 41","pages":"31020–31034"},"PeriodicalIF":4.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering Self-Woven Hierarchical Bimetallic Nitride Electrode with Built-In Interfacial Electric Field for Enhanced Alkaline Hydrogen Evolution","authors":"Wubin Wan,Xuejing Yang,Tianguo Wang,Cheng Luo,Chuitao Zeng,Xingxing Zhu,Xingyou Lang","doi":"10.1021/acssuschemeng.6c04554","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c04554","url":null,"abstract":"Single-phase transition metal nitrides (TMNs) for alkaline hydrogen evolution reaction (HER) are limited by sluggish charge transfer kinetics, suboptimal adsorption, and restricted accessibility of active sites—intrinsic drawbacks of their electronic structure and conventional electrode architecture. Herein, we circumvent these obstacles by constructing a Ni4N/CoN heterostructure on nickel foam (Ni4N/CoN/NF) with two synergistic features: a built-in interfacial electric field (BIEF) and a hierarchical porous morphology. The work function difference between Ni4N and CoN generates a robust BIEF that drives directional electron transfer from Ni to Co, precisely tailoring the electronic configuration of Ni sites to optimize adsorption energy. Moreover, this hierarchical architecture, assembled from interconnected nanochains and nanosheets, simultaneously enhances active-site exposure, facilitates electron transport, and promotes efficient gas release. Benefiting from these synergistic advantages, the Ni4N/CoN electrode delivers an industrial-level current density of 1000 mA cm–2 at an overpotential of only 213 mV in alkaline media. Moreover, the combination of its robust interwoven nanochain architecture and strong interfacial electronic coupling endows the electrode with outstanding operational stability, sustaining continuous hydrogen evolution for over 500 h at the current density of 500 mA cm–2. This work presents a viable strategy for designing efficient and durable heterostructure electrocatalysts toward practical water electrolysis.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Precision Protein Modification via Ligation and Bioconjugation at Selenocysteine","authors":"Max J. Bedding,&nbsp;Sameer S. Kulkarni,&nbsp;Richard J. Payne","doi":"10.1021/acs.accounts.6c00543","DOIUrl":"https://doi.org/10.1021/acs.accounts.6c00543","url":null,"abstract":"<p>Selenocysteine (Sec), oftenreferred to as the21st amino acid,is a rare yet essential amino acid found in a small number of naturallyoccurring selenoproteins that play critical roles in redox regulation,antioxidant defence, and hormone metabolism. Owing to its distinctchemical properties, namely enhanced nucleophilicity, lower reductionpotential, and versatile redox behaviour of the side chain selenol/diselenidemoiety relative to the thiol/disulfide of Cys, Sec has recently beenleveraged for a range of applications in protein science.</p><p>Inthis account, we summarize our endeavors towards the developmentof selenium-mediated ligation methodologies for the rapid and highlyefficient assembly of proteins, including those bearing native post-translationalmodifications (PTMs) or “designer” modifications. Keyinnovations include the diselenide–selenoester ligation (DSL)and expressed protein selenoester ligation (EPSL). DSL enables therapid fusion of unprotected peptides through a chemoselective reactionbetween peptide selenoesters and selenopeptides. Notably, in the presenceof suitable additives, DSL can be performed at nanomolar concentrations,providing access to challenging classes of modified proteins, suchas lipoproteins, that are difficult to access via other techniques.We also discuss the extension of DSL chemistry to larger proteinsthrough the generation of protein selenoesters from recombinantlyexpressed intein fusion proteins. By combining the advantages of recombinantbacterial expression and the rapid kinetics of DSL at Sec, we highlightthe use of the EPSL technology for the generation of large, aggregation-proneproteins, including the lipidated GTPase YPT6 and mycobacterial lipoproteinsas novel vaccine antigens. Beyond protein synthesis and semi-synthesis,we have also demonstrated the utility of selenocysteine (Sec) as apowerful bioconjugation handle. Specifically, we highlight two novelSec-selective bioconjugation reaction manifolds in this account; thephotocatalytic diselenide contraction (PDC) and electrochemical selenoetherification(e-SE). These transformations enable dimerization and site-specificfunctionalization of peptide and protein diselenides with exceptionalregio- and chemoselectivity, offering significant advantages overother bioconjugation methods.</p><p>Overall, we believe that thesetechnologies represent a major advancein the generation of site-selectively modified peptides and proteins,unlocking new possibilities for applications in fundamental biologybut also the generation of next-generation diagnostics and therapeuticsbearing precise modifications at defined sites on proteins.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"59 20","pages":"3450–3462"},"PeriodicalIF":18.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218980","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Cross-Scale Supply–Demand Matching of Reactive Species in Electrocatalytic Reduction Reactions","authors":"Huai Qin Fu,&nbsp;Peng Fei Liu,&nbsp;Porun Liu,&nbsp;Hua Gui Yang,&nbsp;Huijun Zhao","doi":"10.1021/acs.accounts.6c00559","DOIUrl":"https://doi.org/10.1021/acs.accounts.6c00559","url":null,"abstract":"&lt;p&gt;Electrocatalytic reduction reactions,such as the hydrogen evolutionreaction (HER) and the carbon dioxide, carbon monoxide, and nitrogenelectroreduction reactions (CO&lt;sub&gt;2&lt;/sub&gt;RR, CORR, NRR), providepromising and sustainable routes for energy conversion, carbon utilization,and low-emission chemical manufacturing. Despite significant advancesin catalyst development, the practical implementation of these reactions,particularly under high-current-density conditions, remains severelyconstrained by inefficiencies in activity, selectivity, and stability.The electrocatalyst performance has traditionally been interpretedand optimized largely in terms of intrinsic activity descriptors,such as adsorption free energies of reaction intermediates, electronic-statecharacteristics of active sites, and related electronic-structureparameters, including the d-band center and density of states. Thesedescriptors are typically evaluated in modeling under the implicitassumption that reactive species are continuously and sufficientlysupplied to catalytic active sites. Under practical operating conditions,especially at high reaction fluxes, however, this assumption is oftenno longer valid. A critical limitation arises from the mismatch betweenthe supply capacity of reactive species (e.g., *H, lattice O, andCO&lt;sub&gt;2&lt;/sub&gt;) and the demand strength imposed by active sites. Athigh current densities, electrochemical interfaces operate far fromequilibrium, such that reaction performance is no longer governedsolely by the intrinsic catalytic activity of a single active sitebut also by the rates of generation, replenishment, transfer, andutilization of elementary reaction species. Such supply–demandimbalances can reduce overall reaction rates and alter reaction pathways.However, the role of species supply–demand matching acrossdifferent scales has rarely been systematically incorporated intoreaction mechanisms or catalyst design strategies.&lt;/p&gt;&lt;p&gt;In this Account,we propose a reactive species cross-scale supply–demandmatching framework in electroreduction reactions across atomic, nanoscale,and macroscale regimes. We demonstrate that catalytic performanceis governed not only by intrinsic activity but also by whether theavailability of reactive species becomes insufficient, excessive,or appropriately matched to the demand of active sites. At the nanoscale,we uncover hydrogen spillover as an interfacial mechanism that couples*H generation and consumption sites, enabling *H supply–demandbalance in alkaline HER. At the atomic scale, extending this conceptto proton-coupled electron transfer reactions reveals that efficienthydrogen transfer is governed by spatial proximity, requiring angstrom-scalesite separation. Furthermore, we identify lattice oxygen as an alternativeatomic-scale supply pathway in CO&lt;sub&gt;2&lt;/sub&gt;RR and provide directexperimental evidence for lattice oxygen participation. At the macroscale,we develop quantitative CO&lt;sub&gt;2&lt;/sub&gt; supply–demand matchingmodels that co","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"59 20","pages":"3437–3449"},"PeriodicalIF":18.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chemically Induced Proximity for Targeted Protein O-GlcNAcylation","authors":"Bowen Ma,&nbsp;Tongyang Xu,&nbsp;Zhihao Guo,&nbsp;Billy Wai-Lung Ng","doi":"10.1021/acs.accounts.6c00453","DOIUrl":"https://doi.org/10.1021/acs.accounts.6c00453","url":null,"abstract":"<p><em>O-</em>GlcNAcylationis a ubiquitous post-translationalmodification across the mammalian proteome, yet determining how individual <em>O-</em>GlcNAcylation events control specific protein functionsremains a central challenge. The <em>O-</em>GlcNAc cycle isgoverned by two enzymes: <em>O-</em>GlcNAc transferase (OGT),which installs <em>O-</em>GlcNAc, and <em>O-</em>GlcNAcase(OGA), which removes it. Because these enzymes act on thousands ofproteins, conventional methods, such as pharmacological inhibitionof OGT or OGA, produce broad cellular effects that are difficult toassign to individual substrates. This gap has motivated the developmentof targeted <em>O-</em>GlcNAcylation strategies, includinggenetically encoded and chemical biology tools, which have shown that <em>O-</em>GlcNAc can be selectively installed on defined proteinsto interrogate protein-specific <em>O-</em>GlcNAc functions.</p><p>This Account describes the development of <em>O-</em>GlcNAcTArgeting Chimeras, or OGTACs, as chemical tools for targeted <em>O-</em>GlcNAc installation. OGTACs are bifunctional moleculesthat can recruit OGT to a specific protein of interest. Specifically,an OGTAC consists of an OGT-engaging element, a linker, and a target-recognitionmotif, which together bring OGT into proximity with a selected substrate.</p><p>Our studies show that chemically induced proximity can redirectOGT toward selected proteins, thereby creating targeted <em>O-</em>GlcNAc writing that can partially bypass TPR-domain-mediated substraterecognition under engineered recruitment conditions. A central lessonis that productive <em>O-</em>GlcNAc writing requires notonly recruitment, but also proper ternary-complex formation and noninhibitoryOGT engagement. Moreover, the target-recognition motif determinesthe targetable protein space and achievable selectivity of the platform.By linking local <em>O-</em>GlcNAc installation to changesin protein turnover, signaling, and transcriptional output, OGTACsprovide a conceptual framework for using induced proximity to modulateprotein functions.</p>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":"59 20","pages":"3336–3346"},"PeriodicalIF":18.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}