Angewandte Chemie International Edition最新文献_第6页

Unlocking High‐Concentration PET Upcycling via Site‐Decoupled Copper Catalysis 通过位点解耦铜催化解锁高浓度PET升级回收

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516357

Chuan Gang, Jingqing Tian, Bing Ma, Chen Zhao

{"title":"Unlocking High‐Concentration PET Upcycling via Site‐Decoupled Copper Catalysis","authors":"Chuan Gang, Jingqing Tian, Bing Ma, Chen Zhao","doi":"10.1002/anie.202516357","DOIUrl":"https://doi.org/10.1002/anie.202516357","url":null,"abstract":"Upcycling polyethylene terephthalate (PET) plastic waste on islands into valuable fuels represents a promising strategy for carbon resource utilization and circular economy development; however, this approach faces critical challenges, including low processing concentrations (currently CPET < 1.5 wt%) and fast catalyst deactivation under high‐temperature redox conditions. Herein, we report a site‐decoupled copper catalyst (Cu/MgAlGaZnOx) that unlocks quantitative conversion of PET to p‐xylene (PX) at unprecedented concentrations (15.1 wt%), achieving a record PX formation rate of 10.1 −7.8‐fold higher than prior CuNa/SiO2 systems. In situ spectroscopy reveals that ethylene glycol (EG) fragment oxidation during depolymerization reduces Cu+ species in conventional catalysts, triggering rapid deactivation. By contrast, oxygen vacancies (Ov) in the GaZnOx support adsorb methanolysis intermediates, spatially segregating depolymerization (GaZnOx) from hydrodeoxygenation (Cu/MgAlOx). This decoupling stabilizes active Cu⁺/Cu0─Ov sites, enabling sustained operation at high PET concentrations. Our work establishes site decoupling as a general strategy for stabilizing redox catalysts in polymer upcycling under demanding environments.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188635","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

Improving the Conductivity and Stability of Silver Nanowires Through Spontaneous Ligand Exchange for Joule Heating. 焦耳加热下自发配体交换提高银纳米线的导电性和稳定性。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202518337

Junhyeok Kwon,Joon-Young Soh,HyeonOh Shin,Sungjun Lim,So Yeon Yoon,Wang-Hyo Kim,Deok-Ho Roh,Moosung Choi,Sang-Won Park,EunAe Cho,Tae-Hyuk Kwon,Ji Hoon Seo

{"title":"Improving the Conductivity and Stability of Silver Nanowires Through Spontaneous Ligand Exchange for Joule Heating.","authors":"Junhyeok Kwon,Joon-Young Soh,HyeonOh Shin,Sungjun Lim,So Yeon Yoon,Wang-Hyo Kim,Deok-Ho Roh,Moosung Choi,Sang-Won Park,EunAe Cho,Tae-Hyuk Kwon,Ji Hoon Seo","doi":"10.1002/anie.202518337","DOIUrl":"https://doi.org/10.1002/anie.202518337","url":null,"abstract":"Silver nanowires (AgNWs) are promising materials for optoelectronic devices, owing to their high transparency and conductivity. However, their performance is limited by polyvinylpyrrolidone (PVP) as an insulating capping agent that is essential for the synthesis of AgNWs but increases their intrinsic resistance. Herein, we introduce a facile spin-coating ligand exchange strategy that considers the physicochemical properties of ligands, including PVP solubility, viscosity, volatility, and hydrogen-bonding ability, to achieve a stable adsorption and efficient exchange. Among the tested ligands, ethylene glycol (EG) ligand effectively reduces the intrinsic resistance and enhances the optoelectronic properties of AgNWs by spontaneously replacing PVP and forming a stable EG⋯PVP hydrogen-bonded complex, as confirmed by multiple analysis methods. The ligand exchanged AgNWs electrode (AgNWs-EG) improves both in-plane and out-of-plane carrier transport properties as well as stability. Leveraging these properties, AgNWs-EG exhibits a 35% increase in Joule heating performance compared to the pristine AgNWs electrode and remarkable stability at elevated temperatures around 120 °C. Moreover, the performance of AgNWs-EG can be further enhanced through their combination with MXene.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"5 1","pages":"e202518337"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189308","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

Si-H Activation via Dynamic Permutational Isomerism: A Ligand-Directed Route to Dehydrogenative Coupling. Si-H活化通过动态排列异构：一个配体导向的脱氢偶联途径。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202517017

Manuel Kümper,Franz F Westermair,Tobias Götz,Ruth M Gschwind,Jonathan O Bauer

{"title":"Si-H Activation via Dynamic Permutational Isomerism: A Ligand-Directed Route to Dehydrogenative Coupling.","authors":"Manuel Kümper,Franz F Westermair,Tobias Götz,Ruth M Gschwind,Jonathan O Bauer","doi":"10.1002/anie.202517017","DOIUrl":"https://doi.org/10.1002/anie.202517017","url":null,"abstract":"Dehydrogenative coupling (DHC) of hydridosilanes with silanols under metal-free conditions provides a sustainable route to Si─O bond formation. Yet, the mechanistic origin of hydrogen release in such systems has remained unclear. Here, we show that dynamic permutational isomerism of pentacoordinate silicon intermediates is a key prerequisite for Si─H activation and H2 release. Using sterically tailored diaminohydridosilanes, we demonstrate that only ligands enabling access to axial hydride configurations facilitate Si─O coupling with productive H2 elimination. In contrast, N-tert-butyl substitution locks the hydride in the equatorial position and diverts reactivity toward Si─N bond cleavage. Multinuclear variable-temperature NMR spectroscopy, combined with quantum chemical calculations, reveals an equilibrium between equatorial and axial hydride configurations, enabling Berry pseudorotation and hydrogen evolution. These findings provide a mechanistic rationale for H2 release in hydridosilicates and establish ligand-directed isomerism as a general design principle for selective, metal-free Si─H activation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"201 1","pages":"e202517017"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189355","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

Revealing the Active State of a Cu/ZnO:Al Catalyst During Reverse Water-Gas Shift Reaction in an Operando Microwave Absorption Study. 微波吸收研究中Cu/ZnO:Al催化剂在逆向水气转换反应中的活性状态。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202504280

Zohreh Asadi,Clara Patricia Marshall,Annette Trunschke,Thomas Risse

{"title":"Revealing the Active State of a Cu/ZnO:Al Catalyst During Reverse Water-Gas Shift Reaction in an Operando Microwave Absorption Study.","authors":"Zohreh Asadi,Clara Patricia Marshall,Annette Trunschke,Thomas Risse","doi":"10.1002/anie.202504280","DOIUrl":"https://doi.org/10.1002/anie.202504280","url":null,"abstract":"The industrially important Cu/ZnO:Al (CZA) catalyst is known as a dynamic system adapting to reaction conditions, which renders the application of in situ and operando methods key to establish structure function correlations. Herein, a CZA catalyst close to the industrially used compostion was studied using noninvasive and bulk-sensitive in situ/operando microwave cavity perturbation technique and electron paramagnetic resonance spectroscopy during activation and reverse water gas shift reaction. The transient changes of catalytic activity track with the transients of the dielectric properties providing evidence for the importance of bulk properties for catalytic activity. Furthermore, convincing support for the redox reaction mechanism is obtained, and it is shown that H2 and CO2 uptake is not competing kinetically with each other. In addition, the reservoir of H2 and CO2 transiently present in the catalyst during catalysis is determined by the chemical potential of the respective reactant, which is directly coupled to the catalytic activity of the system. The findings fit the model of a Schottky barrier at the Cu/ZnO:Al interface, altered by the gas phase composition which in turn alters the catalytic properties of the system.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"25 1","pages":"e202504280"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189356","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

A Robust Heterometallic Pt2Pd2L8 Double Cage Catenane 一种坚固的异金属Pt2Pd2L8双笼型链烷

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516952

Sudhakar Ganta, Alexander S. Mikherdov, Ananya Baksi, Christoph Drechsler, Guido H. Clever

{"title":"A Robust Heterometallic Pt2Pd2L8 Double Cage Catenane","authors":"Sudhakar Ganta, Alexander S. Mikherdov, Ananya Baksi, Christoph Drechsler, Guido H. Clever","doi":"10.1002/anie.202516952","DOIUrl":"https://doi.org/10.1002/anie.202516952","url":null,"abstract":"The combination of different metal ions in supramolecular structures can lead to the emergence of new features, such as enhanced stability, reduced symmetry, and peculiar reactivity. Mechanically interlocked architectures containing dissimilar metal ions are still scarce. Herein, we report the first example of a heterometallic, quadruply interlocked Pt2Pd2L8 cage catenane, assembled via a combination of metal‐mediated self‐assembly and dynamic covalent chemistry. While direct complexation of the used asymmetric ligand with a mixture of Pt(II) and Pd(II) ions could yield 14 different monomeric and 576 interlocked cage products, the chosen approach allowed us to selectively obtain one PtPdL4 monomeric cage and a single Pt2Pd2L8 double cage isomer as major products, respectively, depending on the reaction conditions. In the obtained interlocked Pt2Pd2L8 structure, the kinetically inert Pt(II) ions are positioned peripherally, while the more labile Pd(II) ions are buried and interlocked within the cage interior, as confirmed by NMR spectroscopy, trapped ion mobility spectrometry (TIMS), and single‐crystal X‐ray diffraction. The resulting catenane structure exhibits an enhanced kinetic stability, resisting disassembly in the presence of excess competitive ligands such as halide anions, unlike previously reported Pd(II) cage catenanes. Furthermore, the Pt2Pd2L8 cage binds halide anions with high affinity, enabling efficient sequestration of halides from organic substrates.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188636","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

Boosting the Ionic Conductivity of Non‐Aqueous Proton Electrolyte for Hybrid Capacitors 提高混合电容器用非水质子电解质的离子电导率

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516992

Mochou Liao, Yuxiao Lin, Yunsong Li, Yongjie Cao, Guodong Li, Dewei Xiao, Ziyue Li, Yi Yang, Fei Wang, Yongyao Xia

{"title":"Boosting the Ionic Conductivity of Non‐Aqueous Proton Electrolyte for Hybrid Capacitors","authors":"Mochou Liao, Yuxiao Lin, Yunsong Li, Yongjie Cao, Guodong Li, Dewei Xiao, Ziyue Li, Yi Yang, Fei Wang, Yongyao Xia","doi":"10.1002/anie.202516992","DOIUrl":"https://doi.org/10.1002/anie.202516992","url":null,"abstract":"Proton batteries have emerged as promising alternatives for energy storage owing to their rapid H⁺ transport kinetics and environmental sustainability. However, state‐of‐art proton batteries using aqueous acid electrolytes suffer from severe hydrogen evolution, electrode dissolution, and narrow electrochemical windows. Non‐aqueous electrolytes could obviate these challenges, while they are typically limited by low ionic conductivity. In this work, a hydrogen‐bond‐mediated proton transport mechanism is revealed in the phosphoric acid/ethyl acetate (H3PO4/EA) electrolytes with various concentrations. The optimized non‐aqueous H3PO4/EA electrolyte (80 m) simultaneously achieves high ionic conductivity (21.8 mS cm−1), wide electrochemical stability window (2.5 V), wide operational temperature range (−80 to 200 °C), and minimal corrosiveness. Using this electrolyte, the MoO3//AC hybrid capacitor demonstrates ultrahigh power density (13292 W kg−1), extended cycling stability (10 000 cycles), and unprecedented temperature adaptability (−50 to 60 °C). Our findings provide fundamental insights into non‐aqueous proton conduction mechanisms and establish new design principles for practical proton energy storage systems.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"100 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188638","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

Hydrogenation of CO2 to Propylene and Butene Over ZnZrOx/SAPO-18. ZnZrOx/SAPO-18上CO2加氢制丙烯和丁烯的研究。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202512845

Siyu Chen,Zhiwei Liang,Zhendong Feng,Zhaochi Feng,Shan Tang,Zelong Li,Jijie Wang,Can Li

{"title":"Hydrogenation of CO2 to Propylene and Butene Over ZnZrOx/SAPO-18.","authors":"Siyu Chen,Zhiwei Liang,Zhendong Feng,Zhaochi Feng,Shan Tang,Zelong Li,Jijie Wang,Can Li","doi":"10.1002/anie.202512845","DOIUrl":"https://doi.org/10.1002/anie.202512845","url":null,"abstract":"Recycling CO2 to light olefins (C2 = ${}^{=} $ - C4 = ${}^{=} $ ) is a promising strategy for long-term carbon storage. However, selective hydrogenation to light olefins while suppressing alkane formation remains a challenge. This work presents an optimized ZnZrOx/SAPO-18 tandem catalyst, which achieves 88.7% light olefins selectivity at 9.5% CO2 conversion with C3 = ${}^{=} $ +C4 = ${}^{=} $ dominating 68.4% of the hydrocarbons. The catalyst exhibits resistance to over hydrogenation, yielding the (C2 = ${}^{=} $ -C4 = ${}^{=} $ )/(C2 0-C4 0) (O/P) ratio of 17.7 and only 1.4% CH4 selectivity. Furthermore, the catalyst shows good stability over 100 h on stream without obvious deactivation, owing to the synergistic effect between ZnZrOx and the reaction conditions, which facilitates the elimination of coke deposition. Hydrothermal treatment brings more Zn─O─Zr active sites and oxygen vacancies (Ov) on ZnZrOx, as well as the modulated Brønsted acid sites (BAS) in SAPO-18 suppresses the over-hydrogenation of olefins, and the AEI-type cage can contain expanded hydrocarbon pool (HCP) intermediates for enhanced C3 = ${}^{=} $ +C4 = ${}^{=} $ formation. This study advances the development of selective CO2-to-olefin conversion technologies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"31 1","pages":"e202512845"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194571","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

Interlocking Organic Nanotubes into a Three-Dimensional Framework: Synthesis, Crystal Structure with Dual-Buckle Configuration, and Application in Stabilizing Lithium Metal Anode. 三维框架的有机纳米管：合成、双扣结构晶体结构及其在稳定锂金属阳极中的应用。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202517238

Zihao Chen,Tuoya Naren,Lei Zhang,Jinglun Yang,Qianfeng Gu,Fangyuan Kang,Libao Chen,Qichun Zhang

{"title":"Interlocking Organic Nanotubes into a Three-Dimensional Framework: Synthesis, Crystal Structure with Dual-Buckle Configuration, and Application in Stabilizing Lithium Metal Anode.","authors":"Zihao Chen,Tuoya Naren,Lei Zhang,Jinglun Yang,Qianfeng Gu,Fangyuan Kang,Libao Chen,Qichun Zhang","doi":"10.1002/anie.202517238","DOIUrl":"https://doi.org/10.1002/anie.202517238","url":null,"abstract":"Single-crystalline organic nanotubes (ONTs) are very important to help us deeply understand the structure-property relationship, however, their preparation remains challenging. In this study, we propose a \"B←N coordination-directed self-locking\" strategy to construct robust single-crystalline ONTs (named as CityU-56). Single crystals of CityU-56 are assembled via the formation of dynamic B←N bonds between 2,2',7,7'-tetra(4-pyridyl)-9,9'-spirobifluorene (SPFPY) and 1,4-bis(benzodioxaborole)benzene (BACT). Single-crystal X-ray diffraction analysis indicates that CityU-56 possesses a well-defined prismatic nanotube structure with highly ordered arrays. Importantly, the dual buckle-tongue-latch interlocking mechanism between adjacent nanotubes stabilizes the ordered arrangement of the nanotubes through synergistic B←N coordination and π-π stacking. Given these advantages, CityU-56 has been demonstrated to serve as an artificial solid electrolyte interphase (ASEI) layer for lithium metal anodes, which significantly enhanced the stability and long-term cycling performance of the as-fabricated batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"69 1","pages":"e202517238"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189305","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

Dynamic Gas-Bridged Chemistry: Breaking Down the Barriers in Building Functional Materials with Gas Molecules. 动态气桥化学：打破用气体分子构建功能材料的障碍。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202519823

Yang-Yang Wang,Nan Yang,Qiang Yan

{"title":"Dynamic Gas-Bridged Chemistry: Breaking Down the Barriers in Building Functional Materials with Gas Molecules.","authors":"Yang-Yang Wang,Nan Yang,Qiang Yan","doi":"10.1002/anie.202519823","DOIUrl":"https://doi.org/10.1002/anie.202519823","url":null,"abstract":"Greenhouse gases like carbon dioxide (CO2), alongside other pollutant gases, pose a significant ecological threat. Harnessing the gaseous species as building blocks to directly participate in the creation of functional assembled materials is a promising strategy for addressing this challenge. Yet, gases as typical polyatomic molecules usually have simple structures and lack effective binding sites, which severely impedes their utility in material assembly. Identifying suitable driving forces or bonding modes that enable gas molecules to be involved in supramolecular construction is imperative. Recently, dynamic gas bridges (DGBs) have emerged as a new class of dynamic covalent bonds that marry gas molecules with complementary Lewis pair components, unlocking impossibilities in fabricating gas-linked molecular assembly systems. This minireview will offer a comprehensive overview of the formation mechanisms and unique dynamic properties of gas-bridged chemistry distinct from other traditional dynamic bonds and highlight their recent advances across three main realms, including how to use dynamic gas bridges to engineer self-assembled materials of different dimensionalities, tailor self-assembly architectures of variable shapes, and prepare soft nanoparticles for sustainable, efficient gas catalysis. Future directions and core challenges for developing smart materials based on dynamic gas-bridged chemistries are outlooked as well.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"11 1","pages":"e202519823"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189352","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

Cell Membrane-Targeted J-Aggregation Strategy for Synergistic Immune Checkpoint Degradation and Immunogenic Pyroptosis to Augment Tumor Immunotherapy. 协同免疫检查点降解和免疫原性焦亡的细胞膜靶向j聚集策略增强肿瘤免疫治疗。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516014

Xiaona Xu,Hao Zhang,Yahui Cao,Weiqing Liu,Zihui Chen,Changhua Li

{"title":"Cell Membrane-Targeted J-Aggregation Strategy for Synergistic Immune Checkpoint Degradation and Immunogenic Pyroptosis to Augment Tumor Immunotherapy.","authors":"Xiaona Xu,Hao Zhang,Yahui Cao,Weiqing Liu,Zihui Chen,Changhua Li","doi":"10.1002/anie.202516014","DOIUrl":"https://doi.org/10.1002/anie.202516014","url":null,"abstract":"While immune checkpoint blockade (ICB) therapy has revolutionized cancer treatment, limitations persist due to factors like PD-L1 recycling, immunosuppressive tumor microenvironments, and off-target effects. Here, we present a novel cell membrane-targeted J-aggregation strategy that synergistically combines immune checkpoint degradation with photo-controlled immune activation within a single-component system. Our platform utilizes a unique PD-L1 ligand-dye conjugate that self-assembles into highly-ordered J-aggregate, maximizing the surface exposure of ligands and imparting remarkable NIR absorption and hypoxia-tolerant type-I photodynamic activities. Surface ligands facilitate multivalent binding to PD-L1 on tumor cell membranes, triggering its lysosomal degradation and leading to a sustained reduction in cellular PD-L1 abundance across diverse cell lines. NIR light irradiation then drives potent immunogenic pyroptosis even under extremely hypoxic conditions (down to 0.1% O2), due to the organelle-targeted type-I photodynamic effect on cell membrane and lysosomes. This targeting arises from the initial PD-L1-mediated membrane binding and subsequent trafficking to lysosomes. Moreover, our platform enables drug self-delivery, coupled with the EPR effect and active targeting of tumor PD-L1, resulting in excellent tumor-selective accumulation (up to 9.8%ID/g). In vivo studies validate a synergistic antitumor immune response. This versatile strategy, applicable to various membrane proteins, represents a significant advance in immunotherapy, opening new avenues for more effective tumor immunotherapies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"104 1","pages":"e202516014"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189362","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