Angewandte Chemie International Edition最新文献_第8页

Pd─N4 Sites in MOFs Modulate Oxygen Reduction Pathways for 100% Selective Photocatalytic CO2-to-CH4 Conversion from Oxygenated Flue Gas. MOFs中的Pd─N4位点调节氧化烟气中100%选择性光催化co2到ch4转化的氧还原途径

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202513157

Wei-Hao Bai,Qi Shao,Ye-Kun Ji,Hao Dong,Xue-Yu Hu,Hao-Ran Xiao,Chao Long

{"title":"Pd─N4 Sites in MOFs Modulate Oxygen Reduction Pathways for 100% Selective Photocatalytic CO2-to-CH4 Conversion from Oxygenated Flue Gas.","authors":"Wei-Hao Bai,Qi Shao,Ye-Kun Ji,Hao Dong,Xue-Yu Hu,Hao-Ran Xiao,Chao Long","doi":"10.1002/anie.202513157","DOIUrl":"https://doi.org/10.1002/anie.202513157","url":null,"abstract":"Direct photocatalytic CO2 reduction in flue gas is significantly challenged by the thermodynamically favored oxygen reduction reaction. While conventional approaches showed promise, the inherent O2 affinity of transition and noble metals prevented full suppression of O2 adsorption and activation, severely constraining the multi-step proton-coupled electron transfers required for the CO2-to-CH4 pathway. We therefore envisioned a CO-mediated oxygen scavenging mechanism by modulating oxygen reduction pathways. Via Pd─N4 site engineering, the resulting Pd/Cu3(HITP)2/TiO2 composite effectively suppressed competitive oxygen reduction reaction, enabling selective CO2-to-CH4 conversion under aerobic conditions. Control experiments and density functional theory calculations revealed that the Pd─N4 sites steered oxygen reduction toward CO-mediated pathways-thermodynamically and kinetically favored over conventional oxygen reduction reaction, thereby mitigating competitive effects and simultaneously purifying the product. Consequently, such composite exhibited complete CH4 selectivity at 6.7 µmol g-1 h-1 under simulated industrial flue gas conditions (15 vol% CO2, 3 vol% O2, 5 vol% H2O, balanced N2). Our work highlights catalytic site modulation and advances a new strategy for photocatalytic CO2 reduction in oxygenated flue gas via pathway-selective oxygen reduction.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"59 1","pages":"e202513157"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331963","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

Mechanochemically Induced Circularly Polarized Luminescence from Polymers. 聚合物机械化学诱导圆极化发光。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202517113

Yuan Yu,Titi Xie,Junyu Li,Yuchuan Tian,Feng Wang,Qi Wang,Laiwei Gao,Yuan Yuan,Yulan Chen

{"title":"Mechanochemically Induced Circularly Polarized Luminescence from Polymers.","authors":"Yuan Yu,Titi Xie,Junyu Li,Yuchuan Tian,Feng Wang,Qi Wang,Laiwei Gao,Yuan Yuan,Yulan Chen","doi":"10.1002/anie.202517113","DOIUrl":"https://doi.org/10.1002/anie.202517113","url":null,"abstract":"Achieving diversified optical signals in polymer mechanochemistry remains a significant challenge, particularly within the area of light polarization. This work pioneers the development of mechanochemically induced circularly polarized luminescence (MICPL) in polymers. We have designed crosslinked polymer networks by photopolymerizing achiral mechanophores (Diels-Alder adducts of maleimide and anthracene derivatives) with the chiral monomer L(-)-bornyl acrylate (LBA). Mechanical compression triggers the retro-Diels-Alder reaction of the mechanophores, releasing fluorophores. Crucially, the applied force simultaneously promotes the aggregation of these released fluorophores and transfers the nonreciprocal chirality inherent in the compressed chiral polymer matrix (PLBA) to these aggregates, resulting in bright, force-dependent CPL emission with a high luminescence dissymmetry factor of up to 10-2. The versatility of this strategy was demonstrated with a series of mechanophores with varying electronic structures and copolymer matrix, enabling tunable CPL colors spanning from blue-violet to green to yellow-orange, and a ternary system achieving white CPL. The MICPL property was retained in copolymer systems (e.g., copolymers with achiral monomer methyl acrylate), demonstrating its potential as a macromolecular chiral optical probe for multimodal stress reporting. These findings resolve questions about mechanical force-regulated chirality and offer a platform for on-demand CPL materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":"e202517113"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331621","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

Closing Electron Transfer Loop to Boost Electrocatalytic Urea Synthesis. 闭合电子传递环促进电催化尿素合成。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202517450

Ruping Miao,Xupeng Qin,Yujie Wang,Siqing Wang,Kaizhi Gu,Yangyang Zhou,Dawei Chen,Dafeng Yan,Wenqi Gao,Qinghua Liu,Chen Chen,Shuangyin Wang

{"title":"Closing Electron Transfer Loop to Boost Electrocatalytic Urea Synthesis.","authors":"Ruping Miao,Xupeng Qin,Yujie Wang,Siqing Wang,Kaizhi Gu,Yangyang Zhou,Dawei Chen,Dafeng Yan,Wenqi Gao,Qinghua Liu,Chen Chen,Shuangyin Wang","doi":"10.1002/anie.202517450","DOIUrl":"https://doi.org/10.1002/anie.202517450","url":null,"abstract":"The electrocatalytic C─N coupling of carbon dioxide and nitrate presents a promising approach for environmentally friendly urea synthesis. In this work, we propose a strategy to boost efficient and durable urea synthesis by coupling the electrochemical and chemical steps. Utilizing fullerene (C60) as a redox-active electron mediator during the electrochemical reduction process, we effectively inhibit the irreversible reduction deactivation of positively charged copper (Cuδ+) active sites. The electron-accepting fullerene form ions (C60 n-) that engage in a spontaneous chemical redox reaction with nitrate ions, producing nitrite ions and regenerating neutral C60 (C60 n- + NO3 - → C60 + NO2 -). This recycling mechanism closes the electron transfer loop while optimizing the overall reaction pathway. The urea yield rate is dramatically increased to 385.9 mmol h-1 g-1, accompanied by long-term durability. Our findings provide a valuable framework for designing highly efficient electrocatalyst for coupling reactions, advancing the field of sustainable urea synthesis.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"28 1","pages":"e202517450"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331662","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 Oxygen Electroreduction Efficiency of Porous Silicon-based Catalysts via Atomic Iron Site-Induced Lattice Expansion. 通过原子铁位诱导晶格膨胀提高多孔硅基催化剂的氧电还原效率。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202516529

Man Wang,Jianming Liu,Xiangju Zhou,Changhao Liu,Jun Gu,Junfeng Zhang,Zhaosheng Li,Zhen-Tao Yu

{"title":"Improving Oxygen Electroreduction Efficiency of Porous Silicon-based Catalysts via Atomic Iron Site-Induced Lattice Expansion.","authors":"Man Wang,Jianming Liu,Xiangju Zhou,Changhao Liu,Jun Gu,Junfeng Zhang,Zhaosheng Li,Zhen-Tao Yu","doi":"10.1002/anie.202516529","DOIUrl":"https://doi.org/10.1002/anie.202516529","url":null,"abstract":"Developing non-noble metal-based catalysts as alternatives to precious metals for the 4 electron oxygen reduction reaction (ORR) in acidic conditions is crucial in advancing practical proton-exchange membrane fuel cells (PEMFCs) technology. A significant challenge in designing these electrocatalysts is to suppress metal leaching and optimize the adsorption and dissociation free energy of oxygen intermediates during the reaction. Herein, a carbon-encapsulated porous silicon (Si) featuring single iron (Fe) sites was developed as an effective ORR catalyst through a one-step thermal reduction process using silica nanoparticles as precursors. This catalyst exhibited both impressive activity with half-wave potentials (E1/2) of 0.88 V and 0.95 V, alongside robust stability showing minimal decay of 7 and 4 mV after 40,000 potential cycles under acidic and alkaline conditions, respectively. Additionally, as a cathode catalyst in PEMFCs, it reached a peak power density of 0.63 W cm-2 in a 1.0 bar H2-O2 condition, while maintaining notable durability at a constant potential of 0.5 V over a duration of 100 h. Spectroscopic characterizations and theoretical calculations demonstrated that iron atoms were effectively integrated into the crystal lattice of porous Si, resulting in the formation of stable Si─Fe bonds that inhibited the leaching of Fe and the formation of *OOH intermediates, thereby enhancing the ORR performance. This approach facilitates the design of efficient and stable ORR catalysts, which hold significant implications for the advancement of next-generation PEMFCs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"2 1","pages":"e202516529"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331746","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

Enantioselective Synthesis of Inherently Chiral Calix[4]arenes via Catalytic Asymmetric Lower-Rim Functionalization. 催化不对称下环功能化对映选择性合成固有手性杯杯芳烃。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202518659

Lei Peng,Yu Chang,Shujun Tong,Wenling Qin,Gianpiero Cera,Hailong Yan

{"title":"Enantioselective Synthesis of Inherently Chiral Calix[4]arenes via Catalytic Asymmetric Lower-Rim Functionalization.","authors":"Lei Peng,Yu Chang,Shujun Tong,Wenling Qin,Gianpiero Cera,Hailong Yan","doi":"10.1002/anie.202518659","DOIUrl":"https://doi.org/10.1002/anie.202518659","url":null,"abstract":"We report herein an efficient approach for the enantioselective synthesis of inherently chiral calix[4]arenes (ICCs) via chiral phosphoric acid (CPA)-catalyzed lower-rim asymmetric functionalization. With vinylidene ortho-quinone methides (VQMs) as the key intermediates, a stepwise asymmetric halo-cyclization strategy was applied to construct diverse inherently chiral calix[4]arenes bearing multiple C─C axially stereogenic elements with high enantio- and diastereoselectivities (up to 96% ee, all d.r. > 20:1). The obtained lower-rim functionalized products underwent further photocatalytic transformations to access novel inherently chiral naphthofuran-based calix[4]arene architectures. Further synthetic modifications and analysis of their photophysical/chiroptical properties demonstrated their potential in optoelectronic materials and related fields. Mechanistic studies reveal that the reaction proceeds via a stepwise process, with the stereoselectivity-determining step occurring in the first VQMs-mediated cyclization, and the second step constituting a chiral transfer process.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202518659"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331664","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

Asymmetric Structure-Induced d-Orbital Splitting Boosts Highly Active and Stable Li-CO2 Batteries. 非对称结构诱导的d轨道分裂促进高活性和稳定的锂-二氧化碳电池。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202516978

Jinghan Qiu,Min Wang,Yingqi Liu,Yanze Song,Zhilong Yang,Yanli Chen,Bingyi Lu,Xin Tao,Jinlong Yang,Guangmin Zhou

{"title":"Asymmetric Structure-Induced d-Orbital Splitting Boosts Highly Active and Stable Li-CO2 Batteries.","authors":"Jinghan Qiu,Min Wang,Yingqi Liu,Yanze Song,Zhilong Yang,Yanli Chen,Bingyi Lu,Xin Tao,Jinlong Yang,Guangmin Zhou","doi":"10.1002/anie.202516978","DOIUrl":"https://doi.org/10.1002/anie.202516978","url":null,"abstract":"Lithium-carbon dioxide (Li-CO2) batteries provide an extremely feasible strategy for sustainable development and carbon neutrality. However, due to the sluggish kinetics and complex interfacial reactions, Li-CO2 batteries are limited by low output voltage and poor cycling stability. Developing efficient and durable catalysts remains an urgent challenge. Transition metal oxides have gained significant attention owing to their availability and stability for electrocatalytic reactions, but their catalytic activity remains unsatisfactory toward Li-CO2 batteries. Herein, this work proposes an asymmetric Fe/Cu-incorporated Co3O4 tactic system to tune charge distribution for motivating efficient electrocatalysis and decipher the mechanism of asymmetric structure modulation on the promotion of catalytic activity and stability. It is unraveled that d-orbital spin splitting induces the modification of nondegenerate state, which enhances catalyst durability, while simultaneously increasing electron occupancy in dxz / yz orbitals. This higher electron occupancy facilitates the hybridization with the p orbitals of reactants and intermediates via π bonding, thereby strengthening the adsorption activity. In consequence, the Li-CO2 battery with Cu-Co3O4 cathode demonstrates a low overpotential of 0.73 V and high Coulombic efficiency of 96%, outperforming batteries with Co3O4 and Fe-Co3O4. This work offers a unique insight for electronic structure regulation strategy and displays a high-performance catalyst for Li-CO2 batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"68 1","pages":"e202516978"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331710","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 Picolyl-Based Cys Caging/Uncaging Strategy Facilitates Protein Synthesis. 基于picolyl的Cys笼/解笼策略促进蛋白质合成。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202518002

Farong Ye,Hanxi Bai,Xinliang Liu,Peng Xu,Guoping Ding,Ping Huang,Xiaheng Zhang,Biao Yu,Ping Wang

{"title":"A Picolyl-Based Cys Caging/Uncaging Strategy Facilitates Protein Synthesis.","authors":"Farong Ye,Hanxi Bai,Xinliang Liu,Peng Xu,Guoping Ding,Ping Huang,Xiaheng Zhang,Biao Yu,Ping Wang","doi":"10.1002/anie.202518002","DOIUrl":"https://doi.org/10.1002/anie.202518002","url":null,"abstract":"Endowed with a reactive thiol group, cysteine (Cys) provides a versatile handle for site-specific bioconjugation and serves as a cornerstone of chemical protein synthesis, particularly in native chemical ligation (NCL). Extensions such as expressed protein ligation (EPL)-desulfurization have significantly broadened access to challenging proteins. However, they require orthogonal caging/uncaging protecting groups to enable selective desulfurization in the presence of native cysteines, a process that is crucial for synthetic applications. Photolabile protecting groups (PPGs), which are cleaved via irradiation, offer a simpler and less disruptive approach to protein assembly compared to traditional thiol protecting groups. However, current commercially available PPGs are not compatible with orthogonal protection and EPL-desulfurization. To address this challenge, we developed a novel and simple picolyl-based PPG for Cys caging/uncaging, which enables rapid orthogonal caging of thiols and their subsequent uncaging via pH and wavelength control. Notably, the picolyl group undergoes photoorthogonal activation in the presence of a nitrobenzyl group. The efficient synthesis of interleukin-4 (IL-4) via one-pot iterative ligation and tumor necrosis factor-alpha (TNF-α) via EPL-desulfurization further highlights how this strategy significantly advances the synthesis of complex proteins.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"25 1","pages":"e202518002"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331794","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

Precise Kinetic Separation of Hexane Isomers via Morphology Engineering of Metal-Organic Frameworks with Diffusion-Selective Pore Structure. 具有扩散选择性孔结构的金属-有机骨架的形态工程对己烷异构体的精确动力学分离。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202521313

Qingju Wang,Zhenglu Yang,Zhensong Qiu,Lifeng Yang,Xian Suo,Xili Cui,Huabin Xing

{"title":"Precise Kinetic Separation of Hexane Isomers via Morphology Engineering of Metal-Organic Frameworks with Diffusion-Selective Pore Structure.","authors":"Qingju Wang,Zhenglu Yang,Zhensong Qiu,Lifeng Yang,Xian Suo,Xili Cui,Huabin Xing","doi":"10.1002/anie.202521313","DOIUrl":"https://doi.org/10.1002/anie.202521313","url":null,"abstract":"Hexane isomer separation is critical to advancing sustainable and high-value refining in the petrochemical industry. However, precise separation of multi-component hexane mixtures with similar molecular structures remains a bottleneck. Herein, we report a novel metal-organic framework (Cu-3,3-bipyridine-SIFSIX, termed as ZU-621) featuring a tailored diffusion-selective pore structure, synergistically integrated with crystal size engineering, that enables precise and efficient separation of hexane isomers. Owing to the uniquely engineered dumbbell-shaped, misaligned electronegative pore environment, ZU-621 exhibits intrinsic kinetic discrimination among hexane isomers based on the alkyl spatial distribution. Complementary crystal morphology engineering further fine-tunes the adsorption-diffusion behavior, affording precise kinetic separation across linear, mono-branched, and di-branched isomer pairs. As a result, this kinetic-morphology synergistic approach achieved benchmark separation performance as evidenced by record gasoline productivity (research octane numbers, RON > 95, 49.8 L kg-1) along with precise, multi-objective separation across five hexane isomers.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"2 1","pages":"e202521313"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331712","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 Novel Antimalarial Agent that Inhibits Protein Synthesis in Plasmodium falciparum. 一种抑制恶性疟原虫蛋白合成的新型抗疟药。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202514085

Patricia Bravo,Eleonora Diamanti,Mostafa M Hamed,Lorenzo Bizzarri,Natalie Wiedemar,Armin Passecker,Nicolas M B Brancucci,Anna Albisetti,Christin Gumpp,Boris Illarionov,Markus Fischer,Matthias Witschel,Tobias Schehl,Hannes Hahne,Pascal Mäser,Matthias Rottmann,Anna K H Hirsch

{"title":"A Novel Antimalarial Agent that Inhibits Protein Synthesis in Plasmodium falciparum.","authors":"Patricia Bravo,Eleonora Diamanti,Mostafa M Hamed,Lorenzo Bizzarri,Natalie Wiedemar,Armin Passecker,Nicolas M B Brancucci,Anna Albisetti,Christin Gumpp,Boris Illarionov,Markus Fischer,Matthias Witschel,Tobias Schehl,Hannes Hahne,Pascal Mäser,Matthias Rottmann,Anna K H Hirsch","doi":"10.1002/anie.202514085","DOIUrl":"https://doi.org/10.1002/anie.202514085","url":null,"abstract":"The emergence of drug resistance to nearly all antimalarials following their rollout underscores the need for novel chemotypes with novel modes of action to replenish the antimalarial drug-development pipeline. We identified a novel class of compounds in the antimalarial armory. Compound 31, characterized by a 2-hydroxyphenyl benzamide scaffold, displays potent activity against blood-stage and mature sexual stages of Plasmodium falciparum and no toxicity in human cells. Resistance selection studies with 31 identified a previously unknown point mutation in the P. falciparum multidrug-resistance protein 1 (pfmdr1) gene, for which we confirmed causality by CRISPR/Cas9-based gene editing as the primary mediator of resistance. No cross-resistance toward first-line antimalarials was identified in compound 31-resistant parasites. Proteomics studies indicated that the primary mode of action of 31 is through direct binding to cytosolic ribosomal subunits, thereby inhibiting protein synthesis in the parasite. Taken together, compound 31 is a promising starting point for the development of a next-generation antimalarial.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202514085"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331726","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

Zinc-Coordinated Lipids: Facilitators for Enhanced mRNA Delivery Efficacy. 锌协调脂质：增强mRNA传递效率的促进剂。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-10-20 DOI: 10.1002/anie.202515406

Yiran Zhang,Kexin Su,Lu Shi,Shiqi Wu,Xinxin Yan,Yifan Zhang,Zichuan Wang,Wei Wang,Tengfei Xu,Shuai Liu

{"title":"Zinc-Coordinated Lipids: Facilitators for Enhanced mRNA Delivery Efficacy.","authors":"Yiran Zhang,Kexin Su,Lu Shi,Shiqi Wu,Xinxin Yan,Yifan Zhang,Zichuan Wang,Wei Wang,Tengfei Xu,Shuai Liu","doi":"10.1002/anie.202515406","DOIUrl":"https://doi.org/10.1002/anie.202515406","url":null,"abstract":"The advancement of mRNA therapeutics necessitates more efficient delivery systems. Current clinically advanced lipid nanoparticles (LNPs) primarily bind mRNA through electrostatic interactions, with limited exploration of other intermolecular forces that can benefit multiple delivery processes. Here, we design zinc-coordinated lipids (Zn-CL) to formulate LNPs, enabling high mRNA delivery efficacy in vivo. The zinc-coordinated moieties in ionizable lipids show strong affinity toward phosphate groups, yielding tight yet reversible mRNA encapsulation. In addition, due to the abundance of phosphate groups in biological membranes, Zn-CL lipids engage them to boost enhanced cellular uptake. Once inside endosomes, competitive binding of zinc-coordinated moieties to the membranes strengthens endosomal destabilization and weakens Zn‑CL/mRNA interactions, enabling efficient endosomal escape as well as rapid cytosolic mRNA release and resolving the long‑standing paradox between stable encapsulation and efficient release. As a result, zinc coordination introduction simultaneously solves multiple mRNA delivery obstacles, ultimately leading to 29-fold higher mRNA translation than FDA-approved SM-102 LNPs in vivo. Notably, this coordination strategy is extendable to other metal ions, with cobalt-coordinated lipids facilitating spleen-targeted mRNA delivery. These findings highlight the substantial potential of metal-coordinated lipids as a versatile platform for enhancing mRNA therapeutic delivery.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"58 1","pages":"e202515406"},"PeriodicalIF":16.6,"publicationDate":"2025-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145331619","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