IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.031

Stefan Ilic , Sydney N. Lavan , Justin G. Connell

引用次数: 0

The tension-activated carbon–carbon bond 张力激活的碳-碳键

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.05.012

引用次数: 0

A light-driven chloride anion transporter 光驱动的氯阴离子转运体

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.09.012

Chenxin Ou , Jinze Lv , Aaron J. Lim , Qing-Hui Guo , Yuanning Feng

引用次数: 0

Modifying commodity-relevant unsaturated polymers via Co-catalyzed MHAT 通过共催化 MHAT 改性与商品相关的不饱和聚合物

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.05.021

{"title":"Modifying commodity-relevant unsaturated polymers via Co-catalyzed MHAT","authors":"","doi":"10.1016/j.chempr.2024.05.021","DOIUrl":"10.1016/j.chempr.2024.05.021","url":null,"abstract":"<div><div><span>The past 2 decades have witnessed the rapid development of CoSalen-catalyzed hydrofunctionalization reactions, mostly on terminal and conjugation-activated olefins. However, the use of 1,2-dialkyl-substituted alkenes continues to pose challenges. In this study, we revisit this substrate class in the context of Carreira-type hydrofunctionalization reactions and introduce a simple yet effective modification (over a 250-fold-increase in </span>turnover number<span><span> [TON]). Near-quantitative yields can be achieved at a low catalyst loading, typically 0.05 mol %. The key lies in inhibiting the degradation of the salen<span> backbone using molecular sieves<span>. This protocol facilitates a study on the metal hydride </span></span></span>hydrogen atom<span><span> transfer (MHAT) regioselectivity of this type of alkene. We found that allylic electron-negative groups and </span>hyperconjugation have profound effects, yielding regioisomeric ratios ranging from 6.5:1 to < 1:20. The high TONs, mild conditions, and versatility of this method further enable its application in the post-polymerization modification of several olefin-rich, commodity-relevant polymers, demonstrating the rich potential of MHAT hydrofunctionalization in macromolecular settings.</span></span></div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 3088-3099"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141425340","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

Recent progress in energy-saving hydrogen production by coupling with value-added anodic reactions 通过与增值阳极反应耦合实现节能制氢的最新进展

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.08.009

Jing Li , Haohong Duan

引用次数: 0

Chiral stacks of a curved nanographene 弯曲纳米石墨的手性叠层

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.008

Zhongbo Zhang , Dániel Csókás , Israel Fernández , Mihaiela C. Stuparu

{"title":"Chiral stacks of a curved nanographene","authors":"Zhongbo Zhang , Dániel Csókás , Israel Fernández , Mihaiela C. Stuparu","doi":"10.1016/j.chempr.2024.07.008","DOIUrl":"10.1016/j.chempr.2024.07.008","url":null,"abstract":"<div><div>Despite enormous advances in the edge extension chemistry of nanographenes, examples of <em>peri</em>-annulations and the knowledge of their effect on molecular properties remain scarce. Here, we show the synthesis of a curved C<sub>60</sub>S<sub>5</sub> nanographene comprising quintuple [5]thiahelicenes arranged in a <em>C</em><sub>5</sub>-symmetric fashion on the zigzag edge (<em>L</em>-region) of a bowl-shaped corannulene core. The synthesis is achieved with the help of Stille coupling, alkynyl thiolation, sulfide/aryne cyclization, and direct arylation reactions. The prepared bowl-helix chiral structure absorbs and emits in the visible and near-IR regions. It assembles into persistent molecular bilayer graphene stacks in solution, solid state, and gas phase. The concave cavities of the supramolecular dimers can recognize the convex surfaces of fullerene C<sub>60</sub> through shape complementarity and π-π stacking interactions in the solid state. A properties comparison with <em>ortho</em>-annulated analogs and archetypical nanographenes indicates the superiority of <em>peri</em>-annulations in the design of molecular graphenes.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 3199-3211"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141918669","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}

引用次数: 0

Transition metal-free difunctionalization of unactivated alkenes: Arylation/azidation, arylation/chlorination, and arylation/cyanation 未活化烯烃的无过渡金属双官能化：芳基化/唑化、芳基化/氯化和芳基化/氰化

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.036

Li Li , Viresh H. Rawal

引用次数: 0

Ribosomal peptides with polycyclic isoprenoid moieties 具有多环异戊二烯分子的核糖体肽

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.07.026

Florian Hubrich , Sanath K. Kandy , Clara Chepkirui , Chandrashekhar Padhi , Silja Mordhorst , Philipp Moosmann , Tao Zhu , Muriel Gugger , Jonathan R. Chekan , Jörn Piel

{"title":"Ribosomal peptides with polycyclic isoprenoid moieties","authors":"Florian Hubrich , Sanath K. Kandy , Clara Chepkirui , Chandrashekhar Padhi , Silja Mordhorst , Philipp Moosmann , Tao Zhu , Muriel Gugger , Jonathan R. Chekan , Jörn Piel","doi":"10.1016/j.chempr.2024.07.026","DOIUrl":"10.1016/j.chempr.2024.07.026","url":null,"abstract":"<div><div>Isoprenoid modifications of proteins and peptides serve fundamental biological functions and are of therapeutic interest. While C<sub>15</sub> (farnesyl) and C<sub>20</sub> (geranylgeranyl) moieties are prevalent among proteins, known ribosomal peptide prenylations involve shorter-chain units not exceeding farnesyl in size. To our knowledge, cyclized terpene moieties have not been reported from either biomolecule class. Here, we used targeted genome mining and heterologous pathway reconstitution to identify ribosomally synthesized and post-translationally modified peptides (RiPPs) with elaborate, cyclized geranylgeranyl modifications. The installing maturases commonly feature fused prenyltransferase-terpene cyclase architectures. We characterized two bifunctional maturases with distinct prenyltransferase folds and identified the terminal product of a cyanobacterial proteusin as an exceptionally complex pseudosteroid-annelated polycyclic peptide. Bioassays suggest modest anti-cyanobacterial activity with the modification being crucial for activity. Genome data predict cyclic isoprenoid units for various RiPP families, including proteusin, Nif11, and lasso peptides, and thus the broader natural and biotechnological compatibility of the maturase system.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 3224-3242"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142142934","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

Hierarchical porous covalent organic framework nanosheets with adjustable large mesopores 具有可调大介孔的分层多孔共价有机框架纳米片

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.05.022

{"title":"Hierarchical porous covalent organic framework nanosheets with adjustable large mesopores","authors":"","doi":"10.1016/j.chempr.2024.05.022","DOIUrl":"10.1016/j.chempr.2024.05.022","url":null,"abstract":"<div><div><span>Synchronous manipulation of meso-structure and architecture of covalent organic frameworks<span><span><span> (COFs) is vital for customized applications but still remains challenging. Here, we develop a polymerization-induced co-assembly approach to construct hierarchical porous COF-based </span>nanosheets with adjustable large </span>mesopores (7–40 nm), intrinsic micropores (∼1.2 nm), ultra-thin thickness (∼24 nm), and a crystalline wall. Furthermore, density functional theory calculations and adsorption experiments indicated that the complementarity of the two-dimensional architecture and intrinsic micropores of COFs can effectively confine iodine molecules. Meanwhile, the exposed nitrogen-containing active sites created by the unique mesoporous structure can strongly anchor iodine species, thereby greatly inhibiting their dissolution and shuttling. Therefore, as a cathode for zinc-iodine battery, they delivered an outstanding rate capability (191.2 mAh g</span></span><sup>−1</sup> at 0.5 A g<sup>−1</sup>) and stable long-term cyclability (154.8 mAh g<sup>−1</sup> at 3 A g<sup>−1</sup> after 20,000 cycles). This approach sheds light on the precise fabrication of crystalline porous materials for diverse applications.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 3100-3113"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453193","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

Terpenoid-based high-performance polyester with tacticity-independent crystallinity and chemical circularity 萜类高性能聚酯，具有与触觉无关的结晶性和化学循环性

IF 19.1 1区化学

Chem Pub Date : 2024-10-10 DOI: 10.1016/j.chempr.2024.05.024

{"title":"Terpenoid-based high-performance polyester with tacticity-independent crystallinity and chemical circularity","authors":"","doi":"10.1016/j.chempr.2024.05.024","DOIUrl":"10.1016/j.chempr.2024.05.024","url":null,"abstract":"<div><div>The development of chemically circular, bio-based polymers is an urgently needed solution to combat the plastic waste crisis. However, the most prominent, commercially implemented bio-based aliphatic polyester, poly(lactic acid) (PLA), is brittle, therefore largely limiting its broad applications. Herein, we introduce a class of aliphatic polyesters produced through the ring-opening polymerization (ROP) of (1<em>R</em>,5<em>S</em>)-8,8-dimethyl-3-oxabicyclo[3.2.1]octan-2-one (D-CamL) and the racemic mixture (<em>rac</em>-CamL), which exhibit superior material properties relative to PLA. A metal-based or organic catalyst was used for the modulation of polymer tacticity. Notably, regardless of tacticity, poly(CamL) exhibits intrinsic crystallinity, resulting in polyesters with high yield stress (24–39 MPa), high Young’s modulus (1.36–2.00 GPa), tunable fracture strains (6%–218%), and high melting temperatures (161°C–225°C). Importantly, poly(CamL) can be chemically recycled to monomer in high yield, and virgin-quality poly(CamL) is obtained after repolymerization. Overall, poly(CamL) represents a new class of bio-derived and chemically circular high-performance polyesters.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 10","pages":"Pages 3040-3054"},"PeriodicalIF":19.1,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453205","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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