ACS Combinatorial Science最新文献

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Ultra-Narrowband Circularly Polarized Luminescence from Multiple 1,4-Azaborine-Embedded Helical Nanographenes 多重 1,4-氮杂硼烷嵌入螺旋纳米石墨的超窄带圆极化发光
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-22 DOI: 10.1021/jacs.4c1140410.1021/jacs.4c11404
Fangyuan Zhang, Vincenzo Brancaccio, Fridolin Saal, Upasana Deori, Krzysztof Radacki, Holger Braunschweig, Pachaiyappan Rajamalli and Prince Ravat*, 
{"title":"Ultra-Narrowband Circularly Polarized Luminescence from Multiple 1,4-Azaborine-Embedded Helical Nanographenes","authors":"Fangyuan Zhang,&nbsp;Vincenzo Brancaccio,&nbsp;Fridolin Saal,&nbsp;Upasana Deori,&nbsp;Krzysztof Radacki,&nbsp;Holger Braunschweig,&nbsp;Pachaiyappan Rajamalli and Prince Ravat*,&nbsp;","doi":"10.1021/jacs.4c1140410.1021/jacs.4c11404","DOIUrl":"https://doi.org/10.1021/jacs.4c11404https://doi.org/10.1021/jacs.4c11404","url":null,"abstract":"<p >In this manuscript we present a strategy to achieve ultranarrowband circularly polarized luminescence (CPL) from multiple 1,4-azaborine-embedded helical nanographenes. The impact of number and position of boron and nitrogen atoms in the rigid core of the molecule on optical properties─including absorption and emission maxima, photoluminescence quantum yield, Stokes shift, excited singlet–triplet energy gap and full width at half-maximum (fwhm) for CPL and fluorescence─was investigated. The molecules reported here exhibits ultranarrowband fluorescence (fwhm 16–17.5 nm in toluene) and CPL (fwhm 18–19 nm in toluene). To the best of our knowledge, this is among the narrowest CPL for any organic molecule reported to date. Quantum chemical calculations, including computed CPL spectra involving vibronic contributions, provide valuable insights for future molecular design aimed at achieving narrowband CPL.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 43","pages":"29782–29791 29782–29791"},"PeriodicalIF":14.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient Aerial Water Harvesting with Self-Sensing Dynamic Janus Crystals 利用自感应动态 Janus 晶体实现高效空中集水
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-22 DOI: 10.1021/jacs.4c1168910.1021/jacs.4c11689
Linfeng Lan, Liang Li, Chenguang Wang, Panče Naumov* and Hongyu Zhang*, 
{"title":"Efficient Aerial Water Harvesting with Self-Sensing Dynamic Janus Crystals","authors":"Linfeng Lan,&nbsp;Liang Li,&nbsp;Chenguang Wang,&nbsp;Panče Naumov* and Hongyu Zhang*,&nbsp;","doi":"10.1021/jacs.4c1168910.1021/jacs.4c11689","DOIUrl":"https://doi.org/10.1021/jacs.4c11689https://doi.org/10.1021/jacs.4c11689","url":null,"abstract":"<p >Water scarcity is one of the most pressing issues of contemporary societal development that requires innovative technologies where the material not only harvests water but also plays an active role in the process. Here, we demonstrate a highly efficient optical self-sensing approach to humidity capture from the air, where both humidity-harvesting and water-transduction functionalities are imparted on slender organic crystals by partial silanization via layer-by-layer hybridization. We report that due to the integration of the harvesting of aerial moisture and the collection of the condensed water, the ensuing Janus-type crystals capture humidity with the highest-to-date water collection efficiency of 15.96 ± 0.63 g cm<sup>–2</sup> h<sup>–1</sup>. The water-collecting elements are also capable of delivering the water by reversible and periodic elastic deformation, and their high optical transparency allows real-time monitoring of the periodic fog collection process by deformational modulation of passively or actively transduced light that outcouples at the crystal-droplet interface. The results could inspire sophisticated approaches to humidity harvesting where optically transparent crystals combine fog capture with self-sensing capabilities for continuous and optimized operation to maximize the cost-gain balance of aerial fog capture.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30529–30538 30529–30538"},"PeriodicalIF":14.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c11689","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Long-Lived Charge Carrier Photogeneration in a Cooperative Supramolecular Double-Cable Polymer 合作型超分子双缆聚合物中的长寿命电荷载流子光生成
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-22 DOI: 10.1021/jacs.4c0963710.1021/jacs.4c09637
Jan Joseph, José Augusto Berrocal, Nicolás M. Casellas, Dirk M. Guldi*, Tomás Torres* and Miguel García-Iglesias*, 
{"title":"Long-Lived Charge Carrier Photogeneration in a Cooperative Supramolecular Double-Cable Polymer","authors":"Jan Joseph,&nbsp;José Augusto Berrocal,&nbsp;Nicolás M. Casellas,&nbsp;Dirk M. Guldi*,&nbsp;Tomás Torres* and Miguel García-Iglesias*,&nbsp;","doi":"10.1021/jacs.4c0963710.1021/jacs.4c09637","DOIUrl":"https://doi.org/10.1021/jacs.4c09637https://doi.org/10.1021/jacs.4c09637","url":null,"abstract":"<p >A newly designed C<sub>3</sub>-symmetric disc-shaped chromophore, <b>BTT(NDI)<sub>3</sub></b>, features electron accepting naphthalene diimides linked to an electron donor BTT core. <b>BTT(NDI)<sub>3</sub></b> self-assembles in apolar solvents into highly ordered, chiral supramolecular fibers through π–π and 3-fold hydrogen-bonding interactions. This leads to a cooperative formation of plane-to-plane stacking of BTTs and J-aggregation of the outer NDIs. Such a structure ensures high charge mobility. Only photoexcitation of BTT in the <b>BTT(NDI)<sub>3</sub></b> polymers triggers a unidirectional electron transfer from BTT to NDI and results in (BTT<sup>•+</sup>-NDI<sup>•–</sup>) lifetimes that are by up to 3 orders of magnitude longer compared to (NDI<sup>•+</sup>-NDI<sup>•–</sup>) that is formed upon NDI photoexcitation. A multiphasic decay implies ambipolar pathways for charge carriers, that is, electron and hole delocalization along the respective BTT and NDI stacks. Our supramolecular approach offers potential for developing functional supramolecular polymers with continuous pathways for electrons and holes and, in turn, minimizing charge recombination losses in organic photovoltaic devices.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30272–30280 30272–30280"},"PeriodicalIF":14.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c09637","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585648","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interwoven Trimeric Cage-Catenanes with Topological Chirality 具有拓扑手性的交织三元笼-烯烷
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-22 DOI: 10.1021/jacs.4c1010410.1021/jacs.4c10104
Lihua Chen, Zhenghong Chen, Weihao Wang, Chenhao Chen, Yoshiaki Kuboi, Chi Zhang, Chenfei Li and Shaodong Zhang*, 
{"title":"Interwoven Trimeric Cage-Catenanes with Topological Chirality","authors":"Lihua Chen,&nbsp;Zhenghong Chen,&nbsp;Weihao Wang,&nbsp;Chenhao Chen,&nbsp;Yoshiaki Kuboi,&nbsp;Chi Zhang,&nbsp;Chenfei Li and Shaodong Zhang*,&nbsp;","doi":"10.1021/jacs.4c1010410.1021/jacs.4c10104","DOIUrl":"https://doi.org/10.1021/jacs.4c10104https://doi.org/10.1021/jacs.4c10104","url":null,"abstract":"<p >Catenanes have gained increasing attention for their unique features such as topological chirality. To date, the majority of works have focused on catenanes comprising monocyclic rings. Due to the lack of efficient synthetic strategy, catenanes of multiannulated monomers remain scarce. Here, we report the one-pot synthesis of an interwoven trimeric cage-catenane in high yield by dynamic imine condensation between diamine linkers of suitable length and trialdehyde panels in stoichiometry. The formation of cage-catenane is driven by the efficient 6-fold π–π stacking of panels. The monomeric cage and trimeric cage-catenane are interconvertible with reversible imine chemistry, with the latter thermodynamically being more favored. Using a topology-based statistical model, we first reveal that the formation probability of the interwoven catenane surpasses that of its chain-like isomer by 20%. When this pure mathematical model is refined by taking into account the strong template effect provided by the π–π stacking of aromatic panels, it shows that the interwoven structure emerges as the dominant species, almost ruling out the formation of the latter. Although composed of achiral cage monomers, the topological chirality of the interwoven trimeric catenane is unraveled by chiral-high-performance liquid chromatography (HPLC) and circular dichroism (CD) spectroscopy, and single-crystal X-ray diffraction (XRD) analysis of the interwoven cage-catenane also reveals a pair of two topological enantiomers. Our probability analysis-aided rationale would provide a design rationale for guiding the efficient synthesis of topologically sophisticated structures.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30303–30313 30303–30313"},"PeriodicalIF":14.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Photoresponsive Organic Cages─Computationally Inspired Discovery of Azobenzene-Derived Organic Cages 光致伸缩有机笼--受计算启发发现偶氮苯衍生有机笼
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-22 DOI: 10.1021/jacs.4c1021710.1021/jacs.4c10217
Michael C. Brand, Hamish G. Trowell, James T. Pegg, Jake L. Greenfield, Magdalena Odaybat, Marc A. Little, Peter R. Haycock, Gokay Avci, Nicola Rankin, Matthew J. Fuchter, Kim E. Jelfs, Andrew I. Cooper and Rebecca L. Greenaway*, 
{"title":"Photoresponsive Organic Cages─Computationally Inspired Discovery of Azobenzene-Derived Organic Cages","authors":"Michael C. Brand,&nbsp;Hamish G. Trowell,&nbsp;James T. Pegg,&nbsp;Jake L. Greenfield,&nbsp;Magdalena Odaybat,&nbsp;Marc A. Little,&nbsp;Peter R. Haycock,&nbsp;Gokay Avci,&nbsp;Nicola Rankin,&nbsp;Matthew J. Fuchter,&nbsp;Kim E. Jelfs,&nbsp;Andrew I. Cooper and Rebecca L. Greenaway*,&nbsp;","doi":"10.1021/jacs.4c1021710.1021/jacs.4c10217","DOIUrl":"https://doi.org/10.1021/jacs.4c10217https://doi.org/10.1021/jacs.4c10217","url":null,"abstract":"<p >The incorporation of photoresponsive groups into porous materials is attractive as it offers potential advantages in controlling the pore size and selectivity to guest molecules. A combination of computational modeling and experiment resulted in the synthesis of two azobenzene-derived organic cages based on building blocks identified in a computational screen. Both cages incorporate three azobenzene moieties, and are therefore capable of 3-fold isomerization, using either ditopic or tetratopic aldehydes containing diazene functionality. The ditopic aldehyde forms a <b>Tri</b><sup><b>2</b></sup><b>Di</b><sup><b>3</b></sup> cage via a 6-fold imine condensation and the tritopic aldehyde forms a <b>Tet</b><sup><b>3</b></sup><b>Di</b><sup><b>6</b></sup> cage via a 12-fold imine condensation. The relative energies and corresponding intrinsic cavities of each isomeric state were computed, and the photoswitching behavior of both cages was studied by UV–Vis and <sup>1</sup>H NMR spectroscopy, including a detailed kinetic analysis of the thermal isomerization for each of the <i>EEZ</i>, <i>EZZ</i> and <i>ZZZ</i> metastable isomers of the <b>Tet</b><sup><b>3</b></sup><b>Di</b><sup><b>6</b></sup> cage. Both cages underwent photoisomerization, where a photostationary state of up to 77% of the <i>cis</i>-isomer and overall thermal half-life of 110 h was identified for the <b>Tet</b><sup><b>3</b></sup><b>Di</b><sup><b>6</b></sup> species. Overall, this work demonstrates the potential of computational modeling to inform the design of photoresponsive materials and highlights the contrasting effects on the photoswitching properties of the azobenzene moieties on incorporation into the different cage species.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30332–30339 30332–30339"},"PeriodicalIF":14.4,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c10217","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585713","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tetraphenylethene-Based Molecular Cage with Coenzyme FAD: Conformationally Isomeric Complexation toward Photocatalysis-Assisted Photodynamic Therapy 含有辅酶 FAD 的四苯基乙烯基分子笼:面向光催化辅助光动力疗法的同构异构复合物
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-21 DOI: 10.1021/jacs.4c0950810.1021/jacs.4c09508
Qingfang Li, Chaochao Yan, Peijuan Zhang, Pingxia Wang, Kaige Wang, Wanni Yang, Lin Cheng, Dongfeng Dang and Liping Cao*, 
{"title":"Tetraphenylethene-Based Molecular Cage with Coenzyme FAD: Conformationally Isomeric Complexation toward Photocatalysis-Assisted Photodynamic Therapy","authors":"Qingfang Li,&nbsp;Chaochao Yan,&nbsp;Peijuan Zhang,&nbsp;Pingxia Wang,&nbsp;Kaige Wang,&nbsp;Wanni Yang,&nbsp;Lin Cheng,&nbsp;Dongfeng Dang and Liping Cao*,&nbsp;","doi":"10.1021/jacs.4c0950810.1021/jacs.4c09508","DOIUrl":"https://doi.org/10.1021/jacs.4c09508https://doi.org/10.1021/jacs.4c09508","url":null,"abstract":"<p >Flavin adenine dinucleotide (FAD), serving as a light-absorbing coenzyme factor, can undergo conformationally isomeric complexation within different enzymes to form various enzyme–coenzyme complexes, which exhibit photocatalytic functions that play a crucial role in physiological processes. Constructing an artificial photofunctional system using FAD or its derivatives can not only develop biocompatible photocatalytic systems with excellent activities but also further enhance our understanding of the role of FAD in biological systems. Here, we demonstrate a supramolecular approach for constructing an artificial enzyme–coenzyme-type host–guest complex with photoinduced catalytic function in water. First, we have designed and synthesized a water-soluble tetraphenylethene (TPE)-based octacationic molecular cage (<b>1</b>) with a large and flexible cavity, which can adaptively encapsulate with two FAD molecules with “U-shaped” conformation (<i>u</i>FAD) to form a 1:2 host–guest complex (<b>1</b>⊃<i>u</i>FAD<sub>2</sub>) in water. Second, based on the conformationally isomeric complexation of FAD within <b>1</b>, the <b>1</b>⊃<i>u</i>FAD<sub>2</sub> complex facilitates electron and energy transfers to molecular oxygen upon the white-light illumination, efficiently producing reactive oxygen species (ROS) such as superoxide radical (O<sub>2</sub><sup>•–</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>). To our knowledge, the <b>1</b>⊃<i>u</i>FAD<sub>2</sub> complex acts as a photocatalyst to achieve the highest turnover frequency (TOF) of 35.6 min<sup>–1</sup> for the photocatalytic oxidation reaction of NADH via a photoinduced superoxide radical catalysis mechanism in an aqueous medium. At last, combining the cytotoxic effects of ROS and the disruption of the intracellular redox balance involving NADH, <b>1</b>⊃<i>u</i>FAD<sub>2</sub> as a supramolecular photosensitizer displays an excellent oxygen-independent photocatalysis-assisted photodynamic therapy in hypoxic tumors.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 45","pages":"30933–30946 30933–30946"},"PeriodicalIF":14.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Supramolecular Catalyzed Cascade Reduction of Azaarenes Interrogated via Data Science 通过数据科学探究氮杂烯烃的超分子催化级联还原反应
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-21 DOI: 10.1021/jacs.4c1148210.1021/jacs.4c11482
Sean M. Treacy, Andrew L. Smith, Robert G. Bergman, Kenneth N. Raymond and F. Dean Toste*, 
{"title":"Supramolecular Catalyzed Cascade Reduction of Azaarenes Interrogated via Data Science","authors":"Sean M. Treacy,&nbsp;Andrew L. Smith,&nbsp;Robert G. Bergman,&nbsp;Kenneth N. Raymond and F. Dean Toste*,&nbsp;","doi":"10.1021/jacs.4c1148210.1021/jacs.4c11482","DOIUrl":"https://doi.org/10.1021/jacs.4c11482https://doi.org/10.1021/jacs.4c11482","url":null,"abstract":"<p >Catalysis of multicomponent transformations requires controlled assembly of reactants within the active site. Supramolecular scaffolds possess synthetic microenvironments that enable precise modulation over noncovalent interactions (NCIs) engaged by reactive, encapsulated species. While molecular properties that describe the behavior of single guests in host cavities have been studied extensively, multicomponent transformations remain challenging to design and deploy. Here, simple univariate regression and threshold analyses are employed to model reactivity in a cascade reduction of azaarenes catalyzed by water-soluble metal organic cages. Yield and stereoselectivity models help deduce unknown mechanisms of reactivity by the multicomponent, host–guest complexes. Furthermore, a comprehensive model is established for NCIs driving stereoselectivity in the reported host–guest adducts.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 43","pages":"29792–29800 29792–29800"},"PeriodicalIF":14.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c11482","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551258","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective pH-Responsive Conjugation between a Pair of De Novo Discovered Peptides 一对新发现的多肽之间的选择性 pH 响应共轭作用
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-21 DOI: 10.1021/jacs.4c0852010.1021/jacs.4c08520
Yuto Ohno, Alexander A. Vinogradov* and Hiroaki Suga*, 
{"title":"Selective pH-Responsive Conjugation between a Pair of De Novo Discovered Peptides","authors":"Yuto Ohno,&nbsp;Alexander A. Vinogradov* and Hiroaki Suga*,&nbsp;","doi":"10.1021/jacs.4c0852010.1021/jacs.4c08520","DOIUrl":"https://doi.org/10.1021/jacs.4c08520https://doi.org/10.1021/jacs.4c08520","url":null,"abstract":"<p >There is a demand for site-selective peptide/protein conjugation chemistry that is fully reversible in a stimulus-responsive manner. The contemporary methods for site-selective protein modification enable the preparation of homogeneous protein–small molecule conjugates, which are indispensable for drug delivery and chemical biology purposes, but such chemistries are usually irreversible. In contrast, the existing reversible protein labeling techniques are generally not site-selective. Here, we report an mRNA display-enabled <i>de novo</i> discovery of a pair of peptides which selectively react with each other to form a conjugate that is stable under neutral conditions (pH 7.5) but rapidly dissociates into the constituents at pH 10. A Cys thiol of peptide CP1 rapidly reacts (<i>k</i><sub>1</sub> = 340 M<sup>–1</sup>·s<sup>–1</sup>) with the isothiocyanate moiety in partner ITC6 to furnish a stable dithiocarbamate (<i>t</i><sub>1/2</sub> = 6 h at pH 7.5). We show that the pH-responsive nature of the reaction (conjugate’s <i>t</i><sub>1/2</sub> = 5 min at pH 10) can be leveraged to utilize ITC6 (1) as a pull-down handle to selectively isolate CP1 from cell lysates and (2) as a temporary protecting group to protect CP1 from nonspecific Cys labeling reagents such as iodoacetamide. Altogether, the chemistry developed here complements the existing approaches and is applicable in a variety of chemical biology settings where selective reversible reactions are needed.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 43","pages":"29429–29440 29429–29440"},"PeriodicalIF":14.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142551422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Development of Ribityllumazine Analogue as Mucosal-Associated Invariant T Cell Ligands 开发作为粘膜相关不变 T 细胞配体的利比替嗪类似物
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-21 DOI: 10.1021/jacs.4c1299710.1021/jacs.4c12997
Ryosuke Takasaki, Emi Ito, Masamichi Nagae, Yuki Takahashi, Takuro Matsuoka, Wakana Yasue, Norihito Arichi, Hiroaki Ohno*, Sho Yamasaki* and Shinsuke Inuki*, 
{"title":"Development of Ribityllumazine Analogue as Mucosal-Associated Invariant T Cell Ligands","authors":"Ryosuke Takasaki,&nbsp;Emi Ito,&nbsp;Masamichi Nagae,&nbsp;Yuki Takahashi,&nbsp;Takuro Matsuoka,&nbsp;Wakana Yasue,&nbsp;Norihito Arichi,&nbsp;Hiroaki Ohno*,&nbsp;Sho Yamasaki* and Shinsuke Inuki*,&nbsp;","doi":"10.1021/jacs.4c1299710.1021/jacs.4c12997","DOIUrl":"https://doi.org/10.1021/jacs.4c12997https://doi.org/10.1021/jacs.4c12997","url":null,"abstract":"<p >Mucosal-associated invariant T (MAIT) cells are a subset of innate-like T cells abundant in human tissues that play a significant role in defense against bacterial and viral infections and in tissue repair. MAIT cells are activated by recognizing microbial-derived small-molecule ligands presented by the MHC class I related-1 protein. Although several MAIT cell modulators have been identified in the past decade, potent and chemically stable ligands remain limited. Herein, we carried out a structure–activity relationship study of ribityllumazine derivatives and found a chemically stable MAIT cell ligand with a pteridine core and a 2-oxopropyl group as the Lys-reactive group. The ligand showed high potency in a cocultivation assay using model cell lines of antigen-presenting cells and MAIT cells. The X-ray crystallographic analysis revealed the binding mode of the ligand to MR1 and the T cell receptor, indicating that it forms a covalent bond with MR1 via Schiff base formation. Furthermore, we found that the ligand stimulated proliferation of human MAIT cells in human peripheral blood mononuclear cells and showed an adjuvant effect in mice. Our developed ligand is one of the most potent among chemically stable MAIT cell ligands, contributing to accelerating therapeutic applications of MAIT cells.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 43","pages":"29964–29976 29964–29976"},"PeriodicalIF":14.4,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142550208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective Reduction of Nitroarenes via Noncontact Hydrogenation 通过非接触氢化选择性还原硝基烯烃
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-21 DOI: 10.1021/jacs.4c0601110.1021/jacs.4c06011
Hua An, Yani Ding, Philippe Sautet, Geng Sun* and Ning Yan*, 
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