Angewandte Chemie International Edition最新文献_第5页

Aptamer as a molecular tethering agent induces PrPC aggregation and degradation to inhibit melanoma proliferation 适配体作为分子系带剂诱导PrPC聚集和降解抑制黑色素瘤增殖

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202425051

Tiantian Xie, Yibin Zhang, Neng Ling, Yijun Yuan, Weibin Liu, Junxiao Guo, Xianhua Wei, Tianhuan Peng, Zhiyan Wang, Jing Dai, Wenjing Chen, Ming Yan, Xiaoqiu Wu, Wencan Wu, Mao Ye, Weihong Tan

{"title":"Aptamer as a molecular tethering agent induces PrPC aggregation and degradation to inhibit melanoma proliferation","authors":"Tiantian Xie, Yibin Zhang, Neng Ling, Yijun Yuan, Weibin Liu, Junxiao Guo, Xianhua Wei, Tianhuan Peng, Zhiyan Wang, Jing Dai, Wenjing Chen, Ming Yan, Xiaoqiu Wu, Wencan Wu, Mao Ye, Weihong Tan","doi":"10.1002/anie.202425051","DOIUrl":"https://doi.org/10.1002/anie.202425051","url":null,"abstract":"Melanoma, a malignant tumor originating from melanocytes, is the most aggressive and deadly form of skin cancer. Previous studies have revealed that the cellular prion protein (PrPC) is frequently overexpressed in melanoma, contributing to tumor progression. This study presents the first proof-of-concept evidence that nucleic acid aptamers can be used to construct a molecular tethering agent that regulates PrPC protein levels by inducing membrane-bound PrPC aggregation for anti-melanoma therapy. Using a screening strategy combining cell-SELEX and cell-internalization SELEX, we obtained an ssDNA aptamer, TT-1e, specifically binding to melanoma cells and tissues. We identified that the binding site of TT-1e is located at the octapeptide repeat region of glycosylated PrPC. Based on the binding characteristics of TT-1e, we engineered an aptamer-based molecular tethering agent TTe-TTe. We found that TTe-TTe induces aggregation of cell surface PrPC, promoting its internalization and facilitating its lysosomal degradation. This process resulted in the inhibition of AKT pathway activation. Importantly, in vivo studies confirmed the ability of TTe-TTe to target melanoma xenografts and suppress tumor growth through this unique mechanism. Our study presents a promising strategy for targeted melanoma therapy and introduces a paradigm-shifting approach for manipulating protein levels using aptamers as molecular tethering agents.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889511","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

Preparation of Cyclic Olefin Polymers via Group Transfer Radical Cyclopolymerization for High Performance in Anode-Free Batteries 基团转移自由基环聚合法制备高性能无阳极电池用环烯烃聚合物

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202507557

Yasu Chen, Shuo Wang, Tongkun Wang, Xianjin Wang, Hao Sun, Chen Zhu

{"title":"Preparation of Cyclic Olefin Polymers via Group Transfer Radical Cyclopolymerization for High Performance in Anode-Free Batteries","authors":"Yasu Chen, Shuo Wang, Tongkun Wang, Xianjin Wang, Hao Sun, Chen Zhu","doi":"10.1002/anie.202507557","DOIUrl":"https://doi.org/10.1002/anie.202507557","url":null,"abstract":"Cyclic olefin polymers (COPs) are of high importance in optical and medical materials. These materials are typically synthesized via ring-opening metathesis polymerization (ROMP) of norbornene derivatives, using metallocene catalysts, followed by high-pressure hydrogenation catalyzed by noble metals. However, the complex synthetic processes, the continuous use of expensive catalysts, and the need to remove metal residues remain substantial barriers in COP production. In contrast, radical cyclopolymerization of dienes, which eliminates the need for metal catalysis and hydrogenation, offers a promising alternative for COP synthesis. Nevertheless, chain transfer reactions hinder the radical polymerization of non-conjugated dienes. To address these challenges, we present a novel strategy, group transfer radical cyclopolymerization (GTRCP), which effectively suppresses chain transfer and enables radical polymerization of dienes to yield COPs. This approach allows for the production of a broad range of sequenceregulated COPs with high molecular weights and low dispersity. Density functional theory (DFT) calculations support the proposed GTRCP mechanism, highlighting its efficiency and selectivity, driven by substantial thermodynamic forces. The resulting COPs demonstrate great potentials as the interphase layer materials in anode-free lithium metal batteries, significantly enhancing the cycling performance towards practical energy storage applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889517","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

Thrombus Boring Microrobot Prepared by an Integrated Phase Separation and Interfacial Self-Assembly Process towards Thrombolysis 基于相分离和界面自组装的溶栓微机器人

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202503221

Han Bao, Sen Zhang, Jing Luo, Jingxin Meng, Shutao Wang

{"title":"Thrombus Boring Microrobot Prepared by an Integrated Phase Separation and Interfacial Self-Assembly Process towards Thrombolysis","authors":"Han Bao, Sen Zhang, Jing Luo, Jingxin Meng, Shutao Wang","doi":"10.1002/anie.202503221","DOIUrl":"https://doi.org/10.1002/anie.202503221","url":null,"abstract":"The pathological formation of thrombi is the primary etiological factor of acute cardiovascular and cerebrovascular diseases, accounting for one-quarter of global fatalities. Traditional thrombolytic drugs are constrained by short half-life, low utilization, and severe complications. Inspired by the tunnel boring machine to excavate strata into small rocks, we reported urokinase plasminogen activator (uPA)-modified thrombus boring microrobots (uTBMs), prepared by a one-step integrated phase separation and interfacial self-assembly process, for effective thrombolysis. The uTBMs are composed of microspheres capped with dual-layered structures of magnetic nanoparticles (MNPs) and cilia nanostructures. In situ observation reveals the integrated phase separation and interfacial self-assembly process of the uTBMs within an emulsion droplet. The capped layer of MNPs allows for controllable motion and rotation behavior under the manipulation of a remote magnetic field. The uPA-modified cilia nanostructures grasp and degrade the fibrin network, synergizing with the uTBMs rotation to mechanically excavate blood cells from thrombus individually, achieving ~8.5-fold higher thrombolytic efficacy than uPA alone. This research demonstrates the feasibility of controllably fabricating and modifying complex-structured microrobots via the simple process towards the potential thrombus therapy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"102 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889519","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

Production of H2O2 via Energy Transfer Photocatalysis by Coupling with Furfuryl Alcohol Conversion over an Amide-Functionalized Heptazine Framework 酰胺功能化七嗪骨架上糠醛转化的能量转移光催化生产H2O2

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202504635

Liangpang Xu, Ka Shuen Yeung, Lejing Li, Xixian Nan, Oleksandr Savateev, Zhuofeng Hu, Jimmy C. Yu

{"title":"Production of H2O2 via Energy Transfer Photocatalysis by Coupling with Furfuryl Alcohol Conversion over an Amide-Functionalized Heptazine Framework","authors":"Liangpang Xu, Ka Shuen Yeung, Lejing Li, Xixian Nan, Oleksandr Savateev, Zhuofeng Hu, Jimmy C. Yu","doi":"10.1002/anie.202504635","DOIUrl":"https://doi.org/10.1002/anie.202504635","url":null,"abstract":"Photocatalytic oxygen reduction provides a sustainable approach for hydrogen peroxide (H2O2) synthesis, but the charge carrier-based pathway is severely limited by inefficient charge separation and redox decomposition of the produced H2O2. Energy transfer photocatalysis (EnTP) is an alternative charge-carrier-free route for H2O2 synthesis. Herein, we propose a strategy of killing two birds with one stone to simultaneously realize the synthesis of H2O2 and conversion of a biomass derivative by coupling EnTP with the Achmatowicz reaction. Results show efficient production of H2O2 at a rate of 14.6 mmol gcat-1 h−1 and an apparent quantum yield of 44.1% at 420 nm, coupled with the conversion of biomass-derived furfuryl alcohol (FFA) to hydroxy-2H-pyran-3(6H)-one with a high selectivity of 85.9%. Such a performance was attributed to the efficient EnTP over the amide-functionalized heptazine framework photocatalyst for singlet oxygen generation, which induces the FFA conversion and concurrently produces H2O2. A systematic study of the photoexcitation process of the catalysts reveals that the amide-functionalization significantly improves the intersystem crossing efficiency, as the structural modification optimizes the electronic structure and thus tunes the composition and distribution of energy bands.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"140 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889535","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

Iridium-Catalyzed Asymmetric β-Selective Hydroamination of Enamides for the Synthesis of 1,2-Diamines 铱催化的不对称β选择性胺化反应合成1,2-二胺

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202507200

Yu-Wen Sun, Hao-Tian Tan, Sheng-Nan Sun, Bi-Jie Li

引用次数: 0

Guideline for Analysis and Prevention of Contamination Catalysis 污染催化分析和预防指南

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202424425

János Daru, Zsombor Gonda, Zoltán May, Zoltán Novák, Gergely L. Tolnai

引用次数: 0

Red-Light-Mediated Generation of Radicals: Applications in Organic Synthesis, Small-Molecule Activation, Polymerization, and Bio-Related Fields 红光介导自由基的产生：在有机合成、小分子活化、聚合和生物相关领域的应用

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202501194

Tong Zhang, Suman Pradhan, Shoubhik Das

引用次数: 0

Biomass-derived Functional Polyacetals via Controlled Cascade Enyne Metathesis Polymerization: Tunable Degradability, Post-Polymerization Modification, and Self-assembly 通过控制级联炔复分解聚合的生物质衍生功能聚缩醛：可调降解性、聚合后修饰和自组装

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202503022

Liangbing Fu, Yuan Tao, Bixia Xie, Jingrong Liu, Changquan Lin, Yanli Feng, Jiazhou Jiang, Yuhan Peng, Lijun Liu, Junpeng Zhao

{"title":"Biomass-derived Functional Polyacetals via Controlled Cascade Enyne Metathesis Polymerization: Tunable Degradability, Post-Polymerization Modification, and Self-assembly","authors":"Liangbing Fu, Yuan Tao, Bixia Xie, Jingrong Liu, Changquan Lin, Yanli Feng, Jiazhou Jiang, Yuhan Peng, Lijun Liu, Junpeng Zhao","doi":"10.1002/anie.202503022","DOIUrl":"https://doi.org/10.1002/anie.202503022","url":null,"abstract":"We present a versatile platform for the synthesis of functional polyacetals from sugar and furfuryl alcohol derivatives using controlled cascade enyne metathesis polymerization. A range of monomers with defined stereochemistry were explored that featured broad functional group tolerance. The polymerization showed living character and permitted preparation of functionalized polyacetals with targetable molecular weights and more complex architectures. In addition, by harnessing the chiral nature of starting materials, the method granted facile access to chiral polyacetals. Modulation of regiochemical and substituent factors around the acetal motif conferred tunable hydrolysis rate, as well as photodegradability when installed with an ortho-nitrobenzyl group. The polymer structure was further elaborated by post-polymerization modification via leveraging the reactivity of suitable pendent groups and preparation of fully degradable bottlebrush polymers via graft-through polymerization. Further utilities of the method were showcased by the preparation of amphiphilic copolymers with complete degradability that exhibited self-assembly behaviors through copolymerization.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"29 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889542","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

Introducing Photochemical Action Plots as a Tool for Unlocking On-Off Switchable Behavior in a Polymeric Eosin Y Photocatalyst 介绍光化学作用图作为解锁聚合伊红Y光催化剂的开关行为的工具

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202502890

Sebastian Gillhuber, Alicia K. Finch, Joshua O. Holloway, Hendrik Frisch, Florian Weigend, Christopher Barner-Kowollik, Peter Werner Roesky

{"title":"Introducing Photochemical Action Plots as a Tool for Unlocking On-Off Switchable Behavior in a Polymeric Eosin Y Photocatalyst","authors":"Sebastian Gillhuber, Alicia K. Finch, Joshua O. Holloway, Hendrik Frisch, Florian Weigend, Christopher Barner-Kowollik, Peter Werner Roesky","doi":"10.1002/anie.202502890","DOIUrl":"https://doi.org/10.1002/anie.202502890","url":null,"abstract":"Photochemical action plots are a powerful tool for investigating the wavelength-dependent efficiency of photochemical processes. Herein, we apply the photochemical action plot methodology developed by the Barner-Kowollik team to a photocatalytic reaction, resulting in the first examples of photocatalytic action plots, paving the way for future in-depth explorations of the wavelength dependence of similar reactions. Specifically, we investigate the wavelength dependence of the catalytic oxidation capabilities of an Eosin Y functionalized polymer photocatalyst (P1) as well as a small molecule representative of the polymer bound Eosin Y moieties (EY) for the oxidation of triphenylphosphine. Introduction of zinc(II) ions into the system proved to drastically influence the optical absorption properties of both catalysts, accompanied by a pronounced influence on their wavelength-dependent reactivity profiles which is not predictable based on the absorption spectra. For P1, these changes can be reversed by metal-mediated single-chain nanoparticle (SCNP) formation upon base addition, giving access to a stimuli-responsive polymeric photocatalyst. Detailed analysis of the photocatalytic action plots enabled the identification of a suitable wavelength for the realization of an on-off switchable polymeric photocatalytic system.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"88 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143889512","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

Chiral Spirobipyridine Synthesis by Cobalt-Catalyzed Enantioselective Double [2+2+2] Cycloaddition 钴催化对映选择性双[2+2+2]环加成合成手性螺联吡啶

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-04-30 DOI: 10.1002/anie.202504831

Ke Li, Danyang Zhu, Luyu Cao, Changkun Li

引用次数: 0