ACS Central Science最新文献

{"title":"Dynamically Interacting Protein Networks Provide a Mechanism to Overcome the Enormous Intrinsic Barrier to Orotidine 5′-Monophosphate Decarboxylation","authors":"Pankaj Dubey,&nbsp;Anish Somani,&nbsp;Jessica Lin,&nbsp;Anthony T. Iavarone and Judith P. Klinman*,&nbsp;","doi":"10.1021/acscentsci.5c00590","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00590","url":null,"abstract":"<p >Orotidine 5′-monophosphate decarboxylase (OMPDC) is among the most efficient enzymes known, accelerating the decarboxylation of the OMP by ∼17 orders of magnitude, primarily by lowering the enthalpy of activation by ∼28 kcal/mol. Despite this feature, OMPDC from <i>Methanothermobacter thermautotrophicus</i> requires ∼15 kcal/mol of activation energy following ES complex formation. This study applies temperature-dependent hydrogen–deuterium exchange mass spectrometry (TDHDX) to detect site-specific thermal protein networks that channel energy from solvent collisions to the active site. Comparative TDHDX of native OMPDC and a single-site variant (Leu123Ala) that alters the activation enthalpy for catalytic turnover reveals region-specific changes in protein flexibility, connecting local scaffold unfolding enthalpy to the activation barrier of catalysis. The data implicate four spatially resolved, thermally sensitive networks that originate at distinct protein–solvent interfaces and converge near the substrate phosphate-binding region (R203), the ribose-binding region (K42), and a catalytic loop (S127). These networks are proposed to act synergistically to optimize substrate positioning and active site electrostatics for the activated complex formation. The complexity of the identified thermal activation pathways distinguishes Mt-OMPDC from other TIM barrel enzymes previously studied by TDHDX. The findings highlight the essential role of scaffold dynamics in enzyme function with broad implications for designing efficient biocatalysts.</p><p >This study uncovers multiple thermal energy transfer pathways in OMPDC, highlighting how site-specific protein dynamics facilitate substrate positioning and electrostatics for C−C bond cleavage.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1377–1390"},"PeriodicalIF":10.4,"publicationDate":"2025-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00590","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902115","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Generative Landscapes and Dynamics to Design Functional Multidomain Artificial Transmembrane Transporters","authors":"Fernando Montalvillo Ortega,&nbsp;Fariha Hossain,&nbsp;Vladimir V. Volobouev,&nbsp;Gabriele Meloni*,&nbsp;Hedieh Torabifard* and Faruck Morcos*,&nbsp;","doi":"10.1021/acscentsci.5c00708","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00708","url":null,"abstract":"<p >Design and synthesis of functionally active artificial proteins is challenging, as it requires simultaneous consideration of interconnected factors, such as fold, dynamics, and function. These evolutionary constraints are encoded in protein sequences and can be learned through the latent generative landscape (LGL) framework to predict functional sequences by leveraging evolutionary patterns, enabling exploration of uncharted sequence space. By simulating designed proteins through molecular dynamics (MD), we gain deeper insights into the interdependencies governing structure and dynamics. We present a synergized workflow combining LGL with MD and biochemical characterization, allowing us to explore the sequence space effectively. This approach has been applied to design and characterize two artificial multidomain ATP-driven transmembrane copper transporters, with native-like functionality. This integrative approach proved effective in revealing the intricate relationships between sequence, structure, and function.</p><p >Synergizing latent generative landscapes and molecular dynamics, we design and validate several artificial multidomain transmembrane transporters in <i>in vitro</i> and <i>in vivo</i> assays.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1452–1466"},"PeriodicalIF":10.4,"publicationDate":"2025-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00708","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Carbamate Prodrugs Restrict In Vivo Metabolism and Improve the Pharmacokinetics of Isoniazid","authors":"Jishnu Sankar,&nbsp;Manish Kumar Bajpai,&nbsp;Anjali Chauhan,&nbsp;Ravi Maddheshiya,&nbsp;Nidhi Sharma,&nbsp;Aditya Sharma,&nbsp;Yashwant Kumar and Dinesh Mahajan*,&nbsp;","doi":"10.1021/acscentsci.5c00576","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00576","url":null,"abstract":"<p >Isoniazid (INH), an important first-line drug in tuberculosis (TB) treatment, faces significant challenges primarily due to hepatotoxicity and peripheral neuropathy as major side effects. These adverse effects often lead to poor patient compliance and treatment dropouts. The INH’s <i>in vivo</i> metabolism is responsible for these adverse effects. INH’s reactive terminal −NH₂ group is involved in its undesired <i>in vivo</i> metabolic transformations. To address this, we designed and synthesized carbamate-based prodrugs of INH by masking the −NH₂ group to reduce its metabolic activity. Herein, we report our efforts to develop such prodrugs and their impact on <i>in vivo</i> metabolism and the pharmacokinetic profile of free INH. The <i>ex vivo</i> stability, bioconversion, and <i>in vivo</i> pharmacokinetic profile with detailed metabolite analysis of these prodrugs were determined in mice. The lead prodrug <b>1d</b> demonstrated enhanced systemic exposure of free INH (1.5-fold, AUC ≈ 3948 ng·h/mL), reduced formation of undesired metabolites, and prolonged half-life (1.3-fold, <i>t</i>_1/2 ≈ 0.88 h) compared to naive INH. This prodrug approach represents a promising strategy for safer and more effective TB therapy, with the potential for less frequent dosing and improved patient compliance.</p><p >Carbamate prodrugs of INH were designed and synthesized to mask its reactive -NH₂ group, resulting in reduced metabolism and improved PK profile. Lead 1d showed 1.5x AUC, prolonged t₁/₂, and potential for safer TB therapy.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1467–1480"},"PeriodicalIF":10.4,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00576","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Photoactivatable Electrophilic Glycosylselenosulfonates for Ultrafast Modification of Alkynes and Thiols","authors":"Weitao Yan,&nbsp;Wenchao Liu,&nbsp;Qinshuo Zhang,&nbsp;Wentao Lin,&nbsp;Yujie Liao,&nbsp;Yiqun Geng,&nbsp;Ruo Wang* and Chunfa Xu*,&nbsp;","doi":"10.1021/acscentsci.5c00650","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00650","url":null,"abstract":"<p >Glycosylseleno scaffolds exhibit wide-ranging applications in multidisciplinary fields, particularly in drug discovery and biophysical chemistry, where they serve as valuable tools for biomolecular structural analysis. However, efficient methods toward glycosylseleno scaffolds remain underexplored. Herein, we present the design of a novel class of bench-stable reagents, glycosylselenosulfonates, which uniquely integrate radical reactivity with electrophilic properties, thereby facilitating the straightforward incorporation of glycosylseleno moieties under mild reaction conditions. Upon photoirradiation, the radical addition of alkynes with glycosylselenosulfonates proceeds at an exceptionally fast rate, achieving completion in less than 1 min. Likewise, the functionalization of cysteine-containing molecules is achieved in a comparably short time frame, typically within 1 min in most instances. Additive experiments involving various amino acids confirm the robustness of these transformations, demonstrating consistently high efficiency across diverse reaction environments with negligible interference. Importantly, successful peptide and protein labeling in aqueous conditions highlights the method’s potential for bioorthogonal applications. These findings collectively underscore the broad applicability and operational simplicity of glycosylselenosulfonates in developing rapid and efficient labeling techniques for biological and chemical research. This work not only advances synthetic methodologies for glycosylseleno scaffolds but also opens new avenues for functional studies of complex biological systems.</p><p >Bench-stable glycosylselenosulfonates reagents enable ultrafast (1 min) labeling of cysteine-containing biomolecules and alkynes under mild, aqueous conditions for bioorthogonal applications.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1400–1407"},"PeriodicalIF":10.4,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00650","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Targeted Protein Modification with an Antibody-Based System","authors":"Oded Rimon*,&nbsp;Juraj Konc,&nbsp;Inga Černauskienė,&nbsp;Montader Ali,&nbsp;Vaidehi Roy Chowdhury,&nbsp;Pietro Sormanni,&nbsp;Gonçalo J. L. Bernardes and Michele Vendruscolo*,&nbsp;","doi":"10.1021/acscentsci.5c00651","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00651","url":null,"abstract":"<p >The chemical modification of proteins is one of the major mechanisms used to regulate the properties and functions of these macromolecules in the cell. It is therefore of great interest to develop tools to exploit this type of modification for applications in molecular biology, medicine, and biotechnology. Here we present a method of using antibodies to perform post-translational covalent modifications of endogenous proteins in complex environments by exploiting proximity-driven chemistry. The method is based on the ability of antibodies to hold a weakly reactive group close to its intended site of reaction by binding the target protein on a nearby epitope. We characterize this approach by modifying the green fluorescent protein in increasingly complex environments and illustrate its applicability by targeting the disease-associated protein beta-2 microglobulin.</p><p >An antibody-based system designed to selectively install a post-translational modification on its target achieves robust and selective activity.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1364–1376"},"PeriodicalIF":10.4,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00651","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Identification of Metal–Organic Frameworks for near Practical Energy Limit CO2 Capture from Wet Flue Gases: An Integrated Atomistic and Process Simulation Screening of Experimental MOFs","authors":"Ohmin Kwon,&nbsp;Marco Gibaldi,&nbsp;Kasturi Nagesh Pai,&nbsp;Arvind Rajendran* and Tom K. Woo*,&nbsp;","doi":"10.1021/acscentsci.5c00777","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00777","url":null,"abstract":"<p >Metal–organic framework (MOF) materials have attracted significant attention as solid sorbents for low energy CO₂ capture with adsorption-based gas separation processes. In this work, an integrated screening workflow combining a series of atomistic and process simulations was applied to identify promising MOFs for a 4-step pressure-vacuum swing adsorption (P/VSA) process at three different CO₂ flue gas compositions (6%, 15% and 35%). Starting from 55,818 unique experimentally characterized MOFs, ∼19k porous MOFs were investigated via atomistic grand canonical Monte Carlo (GCMC) simulations and machine learning model-based process optimizations to accelerate the screening of a large candidate database. Thousands of MOFs were identified for each of the CO₂ compositions tested that could achieve within 4% of the practical energy limit of dry CO₂ capture for the P/VSA process while still meeting the 95% CO₂ purity and 90% recovery constraints. From this pool, 3D MOFs without open metal sites were subjected to the multicomponent (CO₂/N₂/H₂O) GCMC simulations at 40% relative humidity. Based on these simulations, hundreds of MOFs were identified at each CO₂ composition that could retain 90% of their CO₂ capture at this humidity while also adsorbing a minimal amount of water. A geometric analysis of these high performing materials revealed that narrow, straight 1D-channels were a common structural motif for low energy wet flue gas CO₂ capture with P/VSA.</p><p >An integrated screening using molecular and process simulations, followed by calculations of CO₂ retainability in humid conditions, identified hundreds of practical sorbents for CO₂ capture.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1438–1451"},"PeriodicalIF":10.4,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00777","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bidirectional Modification of a Galbulimima Alkaloid Identifies Selective Opioid Ligands","authors":"Florian Martin Zielke,&nbsp;Stone Woo,&nbsp;Samuel Kasmali,&nbsp;Allison Volf,&nbsp;Vuong Q. Dang,&nbsp;Jake B. Bailey,&nbsp;Milan Gembicky,&nbsp;Laura M. Bohn* and Ryan A. Shenvi*,&nbsp;","doi":"10.1021/acscentsci.5c00573","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00573","url":null,"abstract":"<p >We report a bidirectional diversification and optimization campaign of the newly identified <i>mu</i>- and <i>kappa</i>-opioid receptor antagonist GB18, a naturally occurring <i>Galbulimima</i> alkaloid. First, we find that replacement of the GB18 piperidine with pyridine alters the pharmacology from antagonism to partial agonism, with reduced potency but markedly higher receptor selectivity for <i>kappa-</i> over <i>mu-</i>. Second, we optimize this hit via development of a mutually chemoselective cross-coupling of an alkyl iodide/vinyl triflate pair that leads to a series of low- and sub-nanomolar KOR-selective full agonists, some of which demonstrate bias for G protein activation over β-arrestin2 recruitment. Third, we advance three leads to <i>in vivo</i> (mouse) analysis and demonstrate brain penetrance and behavioral effects. In an open-field activity assay, we demonstrate that by increasing G protein signaling preference, agonists display an increase in exploratory, anxiolytic-like behaviors with no signs of sedation. The brevity and success of this campaign, combined with <i>in vitro</i> and <i>in vivo</i> pharmacology, demonstrate GB18 and its analogs as tractable new opioid scaffolds that allow favorable properties to be dialed in and unwanted properties removed.</p><p >Newly discovered GB opioids can be diversified in two steps by mutually chemoselective attached-ring cross-coupling, yielding a series of high potency, G protein-biased, KOR-selective agonists.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1391–1399"},"PeriodicalIF":10.4,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00573","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902067","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigation on Reactivity and Selectivity of Electrocatalytic CO2 Reduction in Photochemically Synthesized Ag19 and Alloyed Ag19Cu2 and Ag12Cu7 Nanoclusters","authors":"Yu-Xin Wang,&nbsp;Jijie Li,&nbsp;Fu-Qiang Zhang,&nbsp;Zhikai Qi,&nbsp;Fengwei Zhang and Xian-Ming Zhang*,&nbsp;","doi":"10.1021/acscentsci.5c00784","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00784","url":null,"abstract":"<p >Atomically precise nanoclusters are desirable for understanding the structure–property relationships in the electrocatalytic CO₂ reduction reaction (eCO₂RR), but suitable related models are lacking, especially those of low- or zerovalent noble metal nanoclusters and their alloyed analogues. We first developed a photochemical method toward silver nanocluster Ag₁₉(4-^<i>t</i>BuPhC≡C)₁₄(Dpppe)₃(SbF₆)₃ (<b>Ag</b>_<b>19</b>-<b>2e</b>) and then related copper-doped alloyed nanocluster Ag₁₂Cu₇(4-^<i>t</i>BuPhC≡C)₁₄(Dpppe)₃Cl₃(SbF₆)₂ (<b>Ag</b>_<b>12</b><b>Cu</b>_<b>7</b>-<b>0e</b>). Herein, we present a larger alloyed nanocluster, Ag₁₉Cu₂(4-^<i>t</i>BuPhC≡C)₁₆(Dpppe)₄(SbF₆)₃ (<b>Ag</b>_<b>19</b><b>Cu</b>_<b>2</b>-<b>2e</b>) and investigate the relationship between the structures and the eCO₂RR performance of those related nanoclusters. The UV–vis and mass spectra revealed that <b>Ag</b>_<b>19</b><b>Cu</b>_<b>2</b>-<b>2e</b> forms via light-induced <b>Ag</b>_<b>19</b>-<b>2e</b> generation followed by Cu(II) attachment. eCO₂RR tests showed that <b>Ag</b>_<b>19</b>-<b>2e</b> is the least efficient, while its dicopper alloyed <b>Ag</b>_<b>19</b><b>Cu</b>_<b>2</b><b>-2e</b> favors formate, highlighting the important role of copper doping in regulating Ag cluster catalysis. This conclusion is further confirmed by the good catalytic performance of <b>Ag</b>_<b>12</b><b>Cu</b>_<b>7</b>-<b>0e</b>, which demonstrated the best C₁ product selectivity for both CO and formate. Experimental and theoretical calculations indicate that its excellent catalytic performance is attributed to the removal of Cl ligands, exposing active Ag sites for launching the eCO₂RR process. This work not only demonstrates that copper-doped silver nanoclusters significantly enhance catalytic activity but also reveals that varying copper doping levels enable modulation of product selectivity in eCO₂RR.</p><p >This study establishes three structurally related nanocluster catalytic models and reveals that Cu-doping level significantly influences the eCO₂RR product selectivity of Ag nanoclusters.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1428–1437"},"PeriodicalIF":10.4,"publicationDate":"2025-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00784","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902059","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Targeting Sialidase to PD1 Enhances T cell Function and Tumor Control","authors":"Brett M. Garabedian,&nbsp;Eleanor E. Bashian,&nbsp;Xiaoshuang Wang,&nbsp;Andrew J. Thompson and James C. Paulson*,&nbsp;","doi":"10.1021/acscentsci.5c00510","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00510","url":null,"abstract":"<p >Immune therapies targeting the PD1 axis have transformed outcomes in cancer treatment by enhancing T cell-mediated immune responses. However, many tumors evade immune clearance through orthogonal escape mechanisms. Excessive production of immunosuppressive sialic acid-containing glycans (sialoglycans) can impair immune surveillance by recruiting inhibitory Siglecs to the immune synapse where, like PD1, they act as checkpoints for cell activation. Sialic acids can also impact T cell activation by dampening the ligation of the costimulatory receptor CD28 with its ligands. This polypharmacology implicates sialoglycans as a linchpin of tumor immunity that can be targeted to further improve outcomes of PD1 therapies. In this work we conjugated sialidase to anti-PD1 (αPD1-S) to selectively degrade sialic acids on immune cells expressing PD1. Glycan profiling confirmed targeted desialylation, and functional assays demonstrated enhancements to T cell activation and cytotoxic capacity. In a melanoma model, αPD1-S promoted inflammatory macrophage polarization and reduced T cell exhaustion, collectively restricting melanoma growth beyond anti-PD1 (αPD1) alone. By simultaneously blocking PD1 and degrading sialoglycans, αPD1-S provides a novel strategy to enhance T cell-mediated immune responses and improve tumor control in refractory cancers.</p><p >Sialidase conjugated to anti-PD1 degrades inhibitory sialoglycans from PD1+ T cells and tumor cells, enhancing T cell activation and tumor control beyond PD1 blockade alone in refractory cancers.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 8","pages":"1417–1427"},"PeriodicalIF":10.4,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acscentsci.5c00510","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144902058","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Supramolecular Chiral Assembly Films with Dynamic Handedness and Emitting-Color Afterglow","authors":"Xinkun Ma,&nbsp;Wei Yuan,&nbsp;Wangjian Fang,&nbsp;Letian Chen,&nbsp;Zujin Zhao* and Yanli Zhao*,&nbsp;","doi":"10.1021/acscentsci.5c00847","DOIUrl":"10.1021/acscentsci.5c00847","url":null,"abstract":"<p >This work presents a strategy for the fabrication of multicolor-emitting circularly polarized afterglow (CPA) films by assembling achiral phosphorescent donors and fluorescent emitters in a photonic crystal matrix. Achiral positively charged phosphors and fluorophores with good spectral overlap are selected as the donor and sequential receptors, which are then coassembled with poly(vinyl alcohol) and cellulose nanocrystals. CPA can be achieved in the blue to near-infrared (NIR) range with stepwise amplification of the dissymmetry factor (lifetime up to 4.52 s and dissymmetry factor up to −0.038) through synergistic chirality and energy transfer processes. Notably, the handedness of the CPA signal can be amplified or reversed by altering the receptor types or the direction of incident light. With the flexibility in manipulating emission and handedness, these materials show potential applications in multidimensional anticounterfeiting and high-definition noctilucent displays.</p><p >Supramolecular assembly with chiral cellulose nanocrystal template and Förster resonance energy transfer cascade enables direction-switchable circularly polarized afterglow and NIR emission.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 7","pages":"1230–1239"},"PeriodicalIF":10.4,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12291125/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144725833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}