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Efficient flow synthesis of a Star of David [2]catenane and a pentafoil knot 大卫星[2]烯烷和五叶结的高效流动合成
IF 23.5 1区 化学
Chem Pub Date : 2024-10-21 DOI: 10.1016/j.chempr.2024.09.027
Chenchen Du, Alex C. Padgham, Anna G. Slater, Liang Zhang
{"title":"Efficient flow synthesis of a Star of David [2]catenane and a pentafoil knot","authors":"Chenchen Du, Alex C. Padgham, Anna G. Slater, Liang Zhang","doi":"10.1016/j.chempr.2024.09.027","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.027","url":null,"abstract":"The development of flow processes for metal-ligand self-assembly and ring-closing metathesis has facilitated the efficient and scalable preparation of iron(II) pentafoil knot and Star of David [2]catenane. Use of a flow reactor also enables the formation of the otherwise inaccessible coordinatively labile zinc(II) pentameric helicate, leading to an efficient two-step synthesis of the zinc(II) pentafoil knot. As the first example of topology-synthesis in flow, our work demonstrates that the metal-ligand self-assembly can be readily adapted to flow techniques, even for labile complexes that are difficult to prepare in batches. The method is well-positioned for expansion to other topological complexes made from the metal template approach. Transitioning from laboratory batch synthesis to efficient large-scale production using continuous flow reactors not only paves the way for new applications of flow synthesis in chemical topology but also enhances the accessibility of these “hard-to-make” entangled moieties, thereby opening avenues for exploring their applications in various fields.","PeriodicalId":268,"journal":{"name":"Chem","volume":"12 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452037","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}
引用次数: 0
Borohydride oxidation-water reduction fuel cells advanced by local hydroxyl enrichment-inhibited borohydride hydrolysis on Cu(0) sites 通过局部羟基富集抑制铜（0）位上的硼氢化物水解推进硼氢化物氧化-水还原燃料电池的发展
IF 23.5 1区 化学
Chem Pub Date : 2024-10-21 DOI: 10.1016/j.chempr.2024.09.030
Libo Zhu, Chang Chen, Tiantian Wu, Xu Yu, Han Tian, Fantao Kong, Ziwei Chang, Wenshu Luo, Xiangzhi Cui, Jianlin Shi
{"title":"Borohydride oxidation-water reduction fuel cells advanced by local hydroxyl enrichment-inhibited borohydride hydrolysis on Cu(0) sites","authors":"Libo Zhu, Chang Chen, Tiantian Wu, Xu Yu, Han Tian, Fantao Kong, Ziwei Chang, Wenshu Luo, Xiangzhi Cui, Jianlin Shi","doi":"10.1016/j.chempr.2024.09.030","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.030","url":null,"abstract":"A promising fuel cell using the acidic hydrogen evolution reaction (HER) instead of kinetically sluggish oxygen reduction reaction to couple with the borohydride oxidation reaction (BOR) has been established. This BOR-HER fuel cell (BHFC) has achieved the concurrent electricity generation and hydrogen production. To catalyze HER/BOR, a copper (Cu)-doped cobalt phosphide nanosheet grown on Cu foam (Cu–CoP/CF) was developed, which exhibits significantly inhibited competitive NaBH<sub>4</sub> hydrolysis during BOR, along with excellent HER performance and stability over 700 h. Specifically, the Cu(0), <em>in situ</em> formed on the surface of Cu–CoP/CF, plays a decisive role in creating an OH<sup>−</sup>-enriched local environment, resulting in significantly inhibited borohydride hydrolysis but greatly enhanced BOR selectivity of up to 85%, as well as the reduced thermodynamic barrier of BOR. The assembled BHFC equipped with Cu–CoP/CF is capable of generating a high power density of 114 mW cm<sup>−2</sup> and concurrently producing hydrogen at a rate of at least 40 mol h<sup>−1</sup> m<sup>−2</sup> at cathode.","PeriodicalId":268,"journal":{"name":"Chem","volume":"24 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452039","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}
引用次数: 0
Tetralactam-based anion transporters 基于四内酰胺的阴离子转运体
IF 23.5 1区 化学
Chem Pub Date : 2024-10-21 DOI: 10.1016/j.chempr.2024.09.028
Alexander M. Gilchrist, Daniel A. McNaughton, Mohamed Fares, Xin Wu, Bryson A. Hawkins, Stephen J. Butler, David E. Hibbs, Philip A. Gale
{"title":"Tetralactam-based anion transporters","authors":"Alexander M. Gilchrist, Daniel A. McNaughton, Mohamed Fares, Xin Wu, Bryson A. Hawkins, Stephen J. Butler, David E. Hibbs, Philip A. Gale","doi":"10.1016/j.chempr.2024.09.028","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.028","url":null,"abstract":"Synthetic anion transporters provide a promising avenue to treat diseases such as cystic fibrosis and cancer. Anion binding site preorganization is one aspect of transporter design that can be manipulated to enhance binding. Macrocycles possess preorganized binding cavities, enabling more selective and efficient anion binding and transport. In this study, we build on a macrocyclic tetralactam scaffold by preparing a series of fluorinated and non-fluorinated tetralactam anion transporters. Anion binding and transport assays were used to analyze the substituent effects on scaffold lipophilicity, selectivity, solubility, binding strength, and transport rates. The series was analyzed for the ability to bind and transport Cl<sup>−</sup> and F<sup>−</sup> anions across lipid bilayers. Some highly fluorinated tetralactams display extremely high levels of Cl<sup>−</sup> and F<sup>−</sup> transport activity, showing record activities in 8-hydroxypyrene-1,3,6-trisulfonic acid (HPTS) assays and a Eu(III) probe-based F<sup>−</sup> transport assay.","PeriodicalId":268,"journal":{"name":"Chem","volume":"20 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452042","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}
引用次数: 0
Engineering a photoenzyme to use red light 利用红光改造光酵素
IF 23.5 1区 化学
Chem Pub Date : 2024-10-16 DOI: 10.1016/j.chempr.2024.09.017
Jose M. Carceller, Bhumika Jayee, Claire G. Page, Daniel G. Oblinsky, Gustavo Mondragón-Solórzano, Nithin Chintala, Jingzhe Cao, Zayed Alassad, Zheyu Zhang, Nathaniel White, Danny J. Diaz, Andrew D. Ellington, Gregory D. Scholes, Sijia S. Dong, Todd K. Hyster
{"title":"Engineering a photoenzyme to use red light","authors":"Jose M. Carceller, Bhumika Jayee, Claire G. Page, Daniel G. Oblinsky, Gustavo Mondragón-Solórzano, Nithin Chintala, Jingzhe Cao, Zayed Alassad, Zheyu Zhang, Nathaniel White, Danny J. Diaz, Andrew D. Ellington, Gregory D. Scholes, Sijia S. Dong, Todd K. Hyster","doi":"10.1016/j.chempr.2024.09.017","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.017","url":null,"abstract":"Photoenzymatic reactions involving flavin-dependent “ene”-reductases (EREDs) rely on protein-templated charge transfer (CT) complexes between the cofactor and substrate for radical initiation. These complexes typically absorb in the blue region of the electromagnetic spectrum. Here, we engineered an ERED to form CT complexes that absorb red light. Mechanistic studies indicate that red-light activity is due to the growth of a red-absorbing shoulder off the previously identified cyan absorption feature. Molecular dynamics simulations, docking, and excited-state calculations suggest that the cyan feature involves a π→π∗ transition on flavin, whereas the red-light absorption is a π→π∗ transition between flavin and the substrate. Differences in the electronic transition are due to changes in the substrate-binding conformation and allosteric tuning of the electronic structure of the cofactor-substrate complex. Microenvironment tuning of the CT complex for red-light activity is observed with other engineered photoenzymatic reactions, highlighting this effect’s generality.","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439790","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}
引用次数: 0
Exerting control of self-assembly pathways via morphological switching and patterning in amino-acid-based benzene-1,3,5-tricarboxamide conjugates 通过氨基酸基苯-1,3,5-三甲酰胺共轭物的形态切换和图案化控制自组装途径
IF 23.5 1区 化学
Chem Pub Date : 2024-10-16 DOI: 10.1016/j.chempr.2024.09.020
Aramballi J. Savyasachi, Oxana Kotova, Ena T. Luis, Amy D. Lynes, Shaun Mills, Sandra A. Bright, Gavin J. McManus, Matthias E. Möbius, D. Clive Williams, Robert Pal, John J. Boland, Thorfinnur Gunnlaugsson
{"title":"Exerting control of self-assembly pathways via morphological switching and patterning in amino-acid-based benzene-1,3,5-tricarboxamide conjugates","authors":"Aramballi J. Savyasachi, Oxana Kotova, Ena T. Luis, Amy D. Lynes, Shaun Mills, Sandra A. Bright, Gavin J. McManus, Matthias E. Möbius, D. Clive Williams, Robert Pal, John J. Boland, Thorfinnur Gunnlaugsson","doi":"10.1016/j.chempr.2024.09.020","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.020","url":null,"abstract":"Small structural changes to benzene-1,3,5-tricarboxamide (BTA) dictate its self-assembly behavior and morphological outcome. Functionalization with an α-amino acid close to the BTA core, which also possesses a terminal terpyridine (tpy) unit, led to a robust gel in the case of glycine, whereas monodisperse, solid microspheres formed in the case of alanine, phenylalanine, and leucine. The self-assembly pathways of the chiral and achiral BTAs are orthogonal and both microspheres and gel fibers independently assemble in the same medium. Further hierarchical self-assembly results upon addition of lanthanide ions (i.e., Eu(III) and Tb(III) that emit at long wavelengths with long excited-state lifetimes) that crosslink the microspheres through coordination, whereas coordination within the gel led to a change in morphology toward microspheres, as well as the formation of hierarchical superstructures. The chirality of the BTA influences helicity of the assembly and the resulting enantiomeric conformation around the lanthanides, evidenced by circularly polarized luminescence.","PeriodicalId":268,"journal":{"name":"Chem","volume":"11 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439928","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}
引用次数: 0
Dearomative dimerization of quinolines and their skeletal rearrangement to indoles triggered by single-electron transfer 单电子转移引发的喹啉二聚化及其骨架重排为吲哚的过程
IF 23.5 1区 化学
Chem Pub Date : 2024-10-16 DOI: 10.1016/j.chempr.2024.09.016
Eugene Yew Kun Tan, Alireza Dehdari, Amirah S. Mat Lani, Derek A. Pratt, Shunsuke Chiba
{"title":"Dearomative dimerization of quinolines and their skeletal rearrangement to indoles triggered by single-electron transfer","authors":"Eugene Yew Kun Tan, Alireza Dehdari, Amirah S. Mat Lani, Derek A. Pratt, Shunsuke Chiba","doi":"10.1016/j.chempr.2024.09.016","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.016","url":null,"abstract":"Dearomatization of two-dimensional planar aromatic feedstocks is an attractive strategy for the introduction of three-dimensional vectors into chemical scaffolds to expand chemical space for drug discovery. Here, we demonstrate the dearomative dimerization and skeletal rearrangement of quinolines under polysulfide anion photocatalysis, in which the additive dictates the reaction courses. In the presence of formate, dearomative dimerization of quinolines is followed by cyclization to form an sp<sup>3</sup>-rich polyheterocyclic hybrid of a 2,5-methanobenzo[<em>b</em>]azepine and a tetrahydroquinoline in a net-reductive manner. On the other hand, in the presence of triethylamine instead of formate, sequential dimerization and skeletal rearrangement occurs to afford 4-(3-indolylmethyl)quinolines in a redox-neutral manner. These observations enabled the design of a net-reductive skeletal rearrangement of 4-arylquinolines to 3-(arylmethyl)indoles. Detailed mechanistic investigations revealed that this umpolung transformation from electron-deficient quinolines to electron-rich indoles is mediated via a 1,2-aryl migration/ring-contraction sequence, as opposed to the more commonly invoked neophyl-like rearrangement.","PeriodicalId":268,"journal":{"name":"Chem","volume":"18 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439965","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}
引用次数: 0
The cyclotriborate trianion 环三硼酸盐三阴离子
IF 23.5 1区 化学
Chem Pub Date : 2024-10-16 DOI: 10.1016/j.chempr.2024.09.002
Manjur O. Akram, Caleb D. Martin
{"title":"The cyclotriborate trianion","authors":"Manjur O. Akram, Caleb D. Martin","doi":"10.1016/j.chempr.2024.09.002","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.002","url":null,"abstract":"In this issue of <em>Chem</em>, Kinjo and Feng report the synthesis of a cyclotriborate trianion (B<sub>3</sub>R<sub>6</sub><sup>3−</sup>), a highly charged boron ring system with discrete two-center two-electron bonds. With three contiguous borates, the B<sub>3</sub><sup>3−</sup> core of the feature compound defies Coulomb’s law and represents the first homocyclic boron analog of the ubiquitous cyclopropane. The remarkable stability enabled full characterization and opens new vistas in the field of multiply charged boron ions.","PeriodicalId":268,"journal":{"name":"Chem","volume":"94 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439926","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}
引用次数: 0
Globally aromatic odd-electron π-magnetic macrocycle 全芳香奇电子π-磁性大环
IF 23.5 1区 化学
Chem Pub Date : 2024-10-15 DOI: 10.1016/j.chempr.2024.09.015
Federico Villalobos, Jan Berger, Adam Matěj, Reed Nieman, Ana Sánchez-Grande, Diego Soler, Andrés Pinar Solé, Hans Lischka, Mikuláš Matoušek, Jiri Brabec, Libor Veis, Alba Millan, Carlos Sánchez-Sánchez, Araceli G. Campaña, Juan M. Cuerva, Pavel Jelínek
{"title":"Globally aromatic odd-electron π-magnetic macrocycle","authors":"Federico Villalobos, Jan Berger, Adam Matěj, Reed Nieman, Ana Sánchez-Grande, Diego Soler, Andrés Pinar Solé, Hans Lischka, Mikuláš Matoušek, Jiri Brabec, Libor Veis, Alba Millan, Carlos Sánchez-Sánchez, Araceli G. Campaña, Juan M. Cuerva, Pavel Jelínek","doi":"10.1016/j.chempr.2024.09.015","DOIUrl":"https://doi.org/10.1016/j.chempr.2024.09.015","url":null,"abstract":"Molecular π-magnets based on single organic molecules have attracted increasing attention for their potential applications in optoelectronics and spintronics. Global aromaticity in conjugated macrocyclic polyradicaloids is still an open question that has only been tackled in molecules with an even number of electrons. Here, we report the on-surface synthesis of a cyclopenta-ring-fused oligo(<em>m</em>-phenylene) macrocycle, <strong>9MC</strong>, with an odd number of electrons. The generated polyradicaloid undergoes a surface-induced distortion to a <em>D</em><sub><em>3</em>h</sub> symmetry with a fully delocalized doublet ground state. Interestingly, <strong>9MC</strong> exhibits two aromatic annulene-within-an-annulene (AWA) ring currents in the inner and outer rings.","PeriodicalId":268,"journal":{"name":"Chem","volume":"56 1","pages":""},"PeriodicalIF":23.5,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436152","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}
引用次数: 0
Stimuli-responsive actuation enabled by selective host-guest recognition of urea cage 通过对尿素笼的主客体选择性识别实现刺激响应式驱动
IF 19.1 1区 化学
Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.013
Zhuo Huang , Xinxing Zhang
{"title":"Stimuli-responsive actuation enabled by selective host-guest recognition of urea cage","authors":"Zhuo Huang ,&nbsp;Xinxing Zhang","doi":"10.1016/j.chempr.2024.09.013","DOIUrl":"10.1016/j.chempr.2024.09.013","url":null,"abstract":"<div><div>Organic cages, featuring the selective stimuli response and reversible encapsulation of guest molecules, demonstrate a huge potential in guest-triggered actuation. In this issue of <em>Chem</em>, Khashab and co-workers exploited host-guest recognition of organic urea cages with three-dimensional structures to integrate multiple mechanical actuations into a single material for the first time.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 2943-2945"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398308","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}
引用次数: 0
Arylative difunctionalization of olefins using easily accessed organobismuth (V) reagents 使用易于获取的有机铋 (V) 试剂对烯烃进行芳基化反官能度处理
IF 19.1 1区 化学
Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.014
Nicholas D. Chiappini
{"title":"Arylative difunctionalization of olefins using easily accessed organobismuth (V) reagents","authors":"Nicholas D. Chiappini","doi":"10.1016/j.chempr.2024.09.014","DOIUrl":"10.1016/j.chempr.2024.09.014","url":null,"abstract":"<div><div>In this issue of <em>Chem</em>, Li and Rawal present an exciting new application of Ar<sub>3</sub>BiCl<sub>2</sub> as convenient reagents for arylative difunctionalization of alkenes using visible or near-visible light. Unburdened by air and moisture sensitivity, the method affords rapid and facile azido-, cyano-, and chloro-arylation of a bevy of functionalized alkenes.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 2945-2947"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398309","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}
引用次数: 0
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