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Gas-Releasing Polymer Tubesomes: Boosting Gas Delivery of Nanovehicles via Membrane Stretching
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202421405
Cuiqin Yang, Yulian Zhang, Prof. Dr. Miaomiao Xu, Prof. Dr. Jianfeng Li, Prof. Dr. Qiang Yan
{"title":"Gas-Releasing Polymer Tubesomes: Boosting Gas Delivery of Nanovehicles via Membrane Stretching","authors":"Cuiqin Yang,&nbsp;Yulian Zhang,&nbsp;Prof. Dr. Miaomiao Xu,&nbsp;Prof. Dr. Jianfeng Li,&nbsp;Prof. Dr. Qiang Yan","doi":"10.1002/ange.202421405","DOIUrl":"https://doi.org/10.1002/ange.202421405","url":null,"abstract":"<p>Hydrogen sulfide (H<sub>2</sub>S), one of the three gas signaling molecules, not only plays a vital role in mediating a series of cellular activities but also manifests exciting applications in clinical therapy. However, one main obstacle in using H<sub>2</sub>S as a gaseous therapeutic agent is to realize on-demand storage and delivery of gas, and thus, it is of great importance to develop H<sub>2</sub>S-donating vehicle platforms. Although a variety of polymer-based gas-releasing carriers have been designed, almost all the systems are limited to spherical structures. Here we explore the role of polymer self-assembled morphologies, especially toward those non-spherical nanostructures, on the H<sub>2</sub>S release capacity. A kind of tubular polymersomes (i.e. tubesomes), formed by the membrane stretching of polythionoester-containing block copolymer vesicles, exhibit enhanced cysteine-responsive H<sub>2</sub>S-releasing behavior in contrast to their spherical counterparts. Moreover, we found that the amount and rate of H<sub>2</sub>S release from diverse polymersomes is relied on the extent of membrane elongation, which allows us to regulate the gas releasing kinetics through tailoring the membrane geometries. More importantly, it is demonstrated that the tubesomes as polymer-type H<sub>2</sub>S donors have better anticancer performance than those spherical polymersomes. This would inspire new possibilities to boost gas therapeutic efficacy through shaping the morphology of gas nanovehicles.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143380682","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}
引用次数: 0
Regio- and Enantioselective Rhodium-Catalyzed Allylic Arylation of Racemic Allylic Carbonates with Arylboronic Acids
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202421596
Hu-Chong Wang, Wen-Jie Shen, Prof. Dr. Shu-Li You
{"title":"Regio- and Enantioselective Rhodium-Catalyzed Allylic Arylation of Racemic Allylic Carbonates with Arylboronic Acids","authors":"Hu-Chong Wang,&nbsp;Wen-Jie Shen,&nbsp;Prof. Dr. Shu-Li You","doi":"10.1002/ange.202421596","DOIUrl":"https://doi.org/10.1002/ange.202421596","url":null,"abstract":"<p>Rhodium-catalyzed regio- and enantioselective allylic arylation of racemic alkyl- and aryl- substituted allylic carbonates with arylboronic acids using commercially available BIBOP ligand is reported. This reaction proceeds at room temperature without base or other additive to deliver allylic arylation products in excellent yields, regio- and enantioselectivity (up to 95 % yield, &gt;20 : 1 b/l, &gt;99 % ee). Rh/BIBOP is disclosed as an efficient catalytic system for allylic substitution reaction.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143252434","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}
引用次数: 0
Paweł Borowiecki
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202424488
{"title":"Paweł Borowiecki","authors":"","doi":"10.1002/ange.202424488","DOIUrl":"https://doi.org/10.1002/ange.202424488","url":null,"abstract":"<p><i>“The most exciting thing about my research is exploring the remarkable catalytic potential of enzymes and witnessing the passion and motivation in the eyes of students and young co-workers, as they engage with scientific discovery… My first experiment was developing analog photographs in a darkroom I set up in the basement of my parents’ house…”</i> Find out more about Paweł Borowiecki in his Introducing… Profile.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202424488","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143252435","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pd-Catalyzed Asymmetric Hydrogenolysis Rearrangement of Allylic Esters to Access Axially Chiral Olefins
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202421287
Bing-Ru Shao, Prof. Dr. Wen-Feng Jiang, Prof. Dr. Chen Wang, Prof. Dr. Lei Shi
{"title":"Pd-Catalyzed Asymmetric Hydrogenolysis Rearrangement of Allylic Esters to Access Axially Chiral Olefins","authors":"Bing-Ru Shao,&nbsp;Prof. Dr. Wen-Feng Jiang,&nbsp;Prof. Dr. Chen Wang,&nbsp;Prof. Dr. Lei Shi","doi":"10.1002/ange.202421287","DOIUrl":"https://doi.org/10.1002/ange.202421287","url":null,"abstract":"<p>The Pd-catalyzed asymmetric hydrogenolysis rearrangement of allylic acetates using (<i>s</i>-Bu)<sub>3</sub>BHK has been described, achieving the synthesis of axially chiral alkylidene cycloalkanes with excellent enantioselectivities (up to 99 % ee) and a wide substrate scope (30 examples of cyclohexanes and cyclobutanes). To the best of our knowledge, this is the first time to achieve synthesis of axially chiral olefins via asymmetric hydrogenolysis of allylic acetates. This methodology not only offers a novel synthetic pathway for non-atropisomeric axially chiral structures but also highlights the potential of asymmetric hydrogenolysis as a powerful tool in synthetic organic chemistry.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143380681","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}
引用次数: 0
Anion Transport by Bambusuril-Bile Acid Conjugates: Drastic Effect of the Cholesterol Content
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202424754
Jacopo Torrisi, Matúš Chvojka, Dr. Pia Jurček, Xinxin Zhang, Prof. Dr. Huaqiang Zeng, Prof. Vladimír Šindelář, Dr. Hennie Valkenier
{"title":"Anion Transport by Bambusuril-Bile Acid Conjugates: Drastic Effect of the Cholesterol Content","authors":"Jacopo Torrisi,&nbsp;Matúš Chvojka,&nbsp;Dr. Pia Jurček,&nbsp;Xinxin Zhang,&nbsp;Prof. Dr. Huaqiang Zeng,&nbsp;Prof. Vladimír Šindelář,&nbsp;Dr. Hennie Valkenier","doi":"10.1002/ange.202424754","DOIUrl":"https://doi.org/10.1002/ange.202424754","url":null,"abstract":"<p>Artificial anion transporters offer a potential way to treat deficiencies in cellular anion transport of genetic origins. In contrast to the large variety of mobile anion carriers and self-assembled anion channels reported, unimolecular anion channels are less investigated. Herein, we present a unique example of a unimolecular anion channel based on a bambusuril (BU) macrocycle, a well-established anion receptor. The BU structure was expanded by appending various bile acid residues allowing a single molecule to span the membrane. Chloride transport mediated by BUs through lipid bilayers was investigated in liposomes and these studies revealed a surprisingly high dependence of the anion transport activity on the cholesterol content in the liposomal membrane.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202424754","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Asymmetric Heck Silylation of Unactivated Alkenes
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202421500
Bingcheng Wang, Jiajin Zhao, Jiale Ying, Biao Cheng, Prof. Zhan Lu
{"title":"Asymmetric Heck Silylation of Unactivated Alkenes","authors":"Bingcheng Wang,&nbsp;Jiajin Zhao,&nbsp;Jiale Ying,&nbsp;Biao Cheng,&nbsp;Prof. Zhan Lu","doi":"10.1002/ange.202421500","DOIUrl":"https://doi.org/10.1002/ange.202421500","url":null,"abstract":"<p>Heck silylation of unactivated alkenes is an efficient strategy for the synthesis of useful organosilicon compounds. However, extensive efforts have been dedicated to only achieving achiral molecules. Herein, a highly regio- and enantioselective cobalt-catalyzed Heck silylation of unactivated alkenes with hydrosilanes is reported for the first time, providing access to axially chiral alkenes in good to excellent yields with 87–98 % <i>ee</i>. Aryl and alkyl groups as well as quaternary carbon centers at the 4-position of vinylcyclohexane could be well tolerated, featuring good functional group tolerance. The gram-scale reaction proceeds smoothly under mild conditions even with 0.5 mol % catalyst loading. A possible mechanism has been proposed, in which enantioselectivity is controlled by alkene insertion. A templating strategy that enhances weak bond interaction is employed to control regioselectivity by modifying the substituents on the ligand and silane.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143252436","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}
引用次数: 0
Dongliang Chao
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202424846
{"title":"Dongliang Chao","authors":"","doi":"10.1002/ange.202424846","DOIUrl":"https://doi.org/10.1002/ange.202424846","url":null,"abstract":"<p><i>“The most exciting thing about my research is finding the next safe and reliable battery technology…. I recharge my batteries by fully ‘discharging’ first, i.e., playing badminton….”</i> Find out more about Dongliang Chao in his Introducing… Profile.</p><p>\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202424846","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143379993","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chloride Residues in RuO2 Catalysts Enhance Its Stability and Efficiency for Acidic Oxygen Evolution Reaction
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202420860
Dr. Jiadong Chen, Menghui Qi, Yun Yang, Dr. Xiaofen Xiao, Dr. Ying Li, Prof. Huile Jin, Prof. Yong Wang
{"title":"Chloride Residues in RuO2 Catalysts Enhance Its Stability and Efficiency for Acidic Oxygen Evolution Reaction","authors":"Dr. Jiadong Chen,&nbsp;Menghui Qi,&nbsp;Yun Yang,&nbsp;Dr. Xiaofen Xiao,&nbsp;Dr. Ying Li,&nbsp;Prof. Huile Jin,&nbsp;Prof. Yong Wang","doi":"10.1002/ange.202420860","DOIUrl":"https://doi.org/10.1002/ange.202420860","url":null,"abstract":"<p>. Ruthenium dioxide (RuO<sub>2</sub>) is a benchmark electrocatalyst for proton exchange membrane water electrolyzers (PEMWE), but its stability during the oxygen evolution reaction (OER) is often compromised by lattice oxygen involvement and metal dissolution. Despite that the typical synthesis of RuO<sub>2</sub> produces chloride residues, the underlying function of chloride have not well investigated. In this study, we synthesized chlorine-containing RuO<sub>2</sub> (RuO<sub>2</sub>-Cl) and pure RuO<sub>2</sub> catalysts with similar morphology and crystallinity. RuO<sub>2</sub>-Cl demonstrated superior stability, three times greater than that of pure RuO<sub>2</sub>, and a lower overpotential of 176 mV at 10 mA cm<sup>−2</sup>. Furthermore, the RuO<sub>2</sub>-Cl catalysts that were in situ synthesized on a platinum-coated titanium felt could maintain high performance for up to 1200 hours at 100 mA cm<sup>−2</sup>. Computational and experimental analyses show that chloride stabilizes RuO<sub>2</sub> by substituting the bridging oxygen atoms, which subsequently inhibits lattice oxygen evolution and Ru demetallation. Notably, this substitution also lowers the energy barrier of the rate-determining step by strengthening the binding of *OOH intermediates. These findings offer new insights into the previously unknown role of chloride residues and how to improve RuO<sub>2</sub> stability.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475378","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}
引用次数: 0
Catalytic Asymmetric 1,4-Hydrocarbonation of 1,3-Enynes via Photoredox/Cobalt/Chromium Triple Catalysis
Angewandte Chemie Pub Date : 2025-01-10 DOI: 10.1002/ange.202420563
Ju-Song Yang, Xing-Yu Wang, Yong-Yao Li, Fu-Min Zhang, Xiao-Ming Zhang, Yong-Qiang Tu
{"title":"Catalytic Asymmetric 1,4-Hydrocarbonation of 1,3-Enynes via Photoredox/Cobalt/Chromium Triple Catalysis","authors":"Ju-Song Yang,&nbsp;Xing-Yu Wang,&nbsp;Yong-Yao Li,&nbsp;Fu-Min Zhang,&nbsp;Xiao-Ming Zhang,&nbsp;Yong-Qiang Tu","doi":"10.1002/ange.202420563","DOIUrl":"https://doi.org/10.1002/ange.202420563","url":null,"abstract":"<p>A synergistic photoredox/cobalt/chromium triple catalysis system for regioselective, enantioselective, and diastereoselective 1,4-hydrocarbonation of readily available 1,3-enyne precursors was explored, providing a modular synthetic platform for various trisubstituted axially chiral allenes bearing an extra central chirality. The protocol features a broad substrate scope, good functional group tolerance, excellent selectivity, and mild reaction conditions. Furthermore, a possible reaction mechanism is proposed based on numerous control experiments and density functional theory calculations.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475379","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}
引用次数: 0
Titelbild: Localized Oxidative Catalytic Reactions Triggered by Cavitation Bubbles Confinement on Copper Oxide Microstructured Particles. (Angew. Chem. 6/2025)
Angewandte Chemie Pub Date : 2025-01-09 DOI: 10.1002/ange.202424920
Valarmathi Mahendran, Dr. Quang Thang Trinh, Xie Zhangyue, Dr. Umesh Jonnalagadda, Prof. Tim Gould, Prof. Nam-Trung Nguyen, Prof. James Kwan, Prof. Tej S. Choksi, Prof. Wen Liu, Prof. Sabine Valange, Dr. François Jérôme, Dr. Prince Nana Amaniampong
{"title":"Titelbild: Localized Oxidative Catalytic Reactions Triggered by Cavitation Bubbles Confinement on Copper Oxide Microstructured Particles. (Angew. Chem. 6/2025)","authors":"Valarmathi Mahendran,&nbsp;Dr. Quang Thang Trinh,&nbsp;Xie Zhangyue,&nbsp;Dr. Umesh Jonnalagadda,&nbsp;Prof. Tim Gould,&nbsp;Prof. Nam-Trung Nguyen,&nbsp;Prof. James Kwan,&nbsp;Prof. Tej S. Choksi,&nbsp;Prof. Wen Liu,&nbsp;Prof. Sabine Valange,&nbsp;Dr. François Jérôme,&nbsp;Dr. Prince Nana Amaniampong","doi":"10.1002/ange.202424920","DOIUrl":"https://doi.org/10.1002/ange.202424920","url":null,"abstract":"<p>Cavitation bubbles confinement and collapse on catalyst surfaces facilitates selective and localised acoustic energy transfer directly to the catalyst surface, minimising undesired dissipation of acoustic energy into the bulk liquid solution while demonstrating superior cavitation properties at lower acoustic pressure amplitudes towards catalytic oxidative reactions. The details of this study are reported by Prince Nana Amaniampong in their Research Article (e202416543).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202424920","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143249662","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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