Angewandte Chemie International Edition最新文献_第4页

Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations.

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-30 DOI: 10.1002/anie.202425551

Dexi Yu, Junhua Zou, Lingdong Zeng, Yidong Hou, Wei Lin, Ling Wu, Masakazu Anpo, Jimmy C Yu, Jinshui Zhang, Xinchen Wang

{"title":"Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations.","authors":"Dexi Yu, Junhua Zou, Lingdong Zeng, Yidong Hou, Wei Lin, Ling Wu, Masakazu Anpo, Jimmy C Yu, Jinshui Zhang, Xinchen Wang","doi":"10.1002/anie.202425551","DOIUrl":"https://doi.org/10.1002/anie.202425551","url":null,"abstract":"<p><p>Photocatalytic chemical transformations for green organic synthesis has attracted much interest. However, their development is greatly hampered by the lack of sufficient reactive sites on the photocatalyst surface for the adsorption and activation of substrate molecules. Herein, we demonstrate that the introduction of well-defined Lewis and Brønsted acid sites coexisting on the surface of TiO2 (SO42-/N-TiO2) creates abundant active adsorption sites for photoredox reactions. The electron-deficient Lewis acid sites supply coordinatively unsaturated surface sites to adsorb molecular oxygen, and the Brønsted acid sites are liable to donate protons to form hydrogen bonds with the OH groups of alcohols like benzyl alcohol (BA). These coexistent acid sites result in a strong synergistic effect in photocatalytic aerobic oxidation of BA. For example, the conversion of BA to benzaldehyde was found to be 88.6%, being much higher than those of pristine TiO2 (14.7%), N-doped TiO2 (N-TiO2, 24.6%), sulfated TiO2 (SO42-/ TiO2, 35.4%), and even their sum. The apparent quantum efficiency (AQE) was determined to be 58.1% at 365 nm and 12.9% at 420 nm over SO42-/N-TiO2. This strategy to create effective synergistic Lewis and Brønsted acids on the catalyst surfaces enables us to apply it to other semiconducting photocatalytic organic transformations.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202425551"},"PeriodicalIF":16.1,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062718","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

Taming the Ion-Dipole Interaction via Rational Diluent Selection for Low-Temperature Li-Metal Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-30 DOI: 10.1002/anie.202423940

Zhenglu Zhu, Yan Li, Jie Ji, Xiaoqun Qi, Junqing Pan, Jiwei Ma, Long Qie, Yunhui Huang

{"title":"Taming the Ion-Dipole Interaction via Rational Diluent Selection for Low-Temperature Li-Metal Batteries","authors":"Zhenglu Zhu, Yan Li, Jie Ji, Xiaoqun Qi, Junqing Pan, Jiwei Ma, Long Qie, Yunhui Huang","doi":"10.1002/anie.202423940","DOIUrl":"https://doi.org/10.1002/anie.202423940","url":null,"abstract":"Developing advanced electrolytes with high Li affinity is crucial for achieving long-cycling lithium metal batteries (LMBs). However, the strong Li+-solvent interactions in conventional electrolytes often induce difficult Li+ desolvation especially under low-temperature conditions, resulting in the formation of fragile electrode interfaces involving solvents, and thus dissatisfactory cycling stability of LMBs. Herein, by introducing various diluents into the lithium hexafluorophosphate in 1, 2-dimethoxyethane electrolyte, we reveal that Li+ desolvation is influenced by not only the diluent-solvent interaction but also the diluent-anion interaction. Based on these findings, a diluent selection parameter (DSP), which is calculated based on the product of interaction energies of diluent-solvent/diluent-Li+ and diluent-anion/diluent-Li+, is proposed for diluent selection. A diluent with a larger DSP is more favorable for promoting Li+ desolvation and improving the low-temperature performance of LMBs. With the rationally selected 1, 2-dichloroethane diluent (DSP=3.95), Li||Cu cell enables high Li reversibility (98.5% after 300 cycles). Li||LiFePO4 cell barely loses capacity at −20 °C for 300 cycles. The Li||LiNi0.8Co0.1Mn0.1O2 cell with the anode-to-cathode capacity ratio of 2.7 retains 87% capacity retention after 100 cycles. This work not only provides new insights into taming strong Li-solvent interactions but also offers a new paradigm for advanced electrolyte design.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"13 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057304","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

Inhibiting Interfacial Electron Leakage via An Artificial Rectified Layer for Longevous Zinc Metal Anodes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-30 DOI: 10.1002/anie.202423244

Xian-Xiang Zeng, Guang-Yuan Yin, Hong-Rui Wang, Min-Yang Zhou, Tao Long, Meng-Sha Ding, Bin Xie, Xiong-Wei Wu, Jiabao Li, Wei Ling, Jiayu Dai

{"title":"Inhibiting Interfacial Electron Leakage via An Artificial Rectified Layer for Longevous Zinc Metal Anodes","authors":"Xian-Xiang Zeng, Guang-Yuan Yin, Hong-Rui Wang, Min-Yang Zhou, Tao Long, Meng-Sha Ding, Bin Xie, Xiong-Wei Wu, Jiabao Li, Wei Ling, Jiayu Dai","doi":"10.1002/anie.202423244","DOIUrl":"https://doi.org/10.1002/anie.202423244","url":null,"abstract":"Dendrites and water-induced side reactions impose greatly challenge on the implementation of aqueous zinc ion batteries. To tackle these problems, an artificial rectified layer (ARL) with hydrophobic, zincophilic and insulating features was in-situ synthesized on Zn surface rapidly to prevent the electron leakage from Zn anode to aqueous electrolyte, which is the underlying logic for uneven Zn deposition and parasitic side reactions. The ARL also displays a high Zn2+ transference number of 0.71 and can build fast Zn2+ transport channels to homogenize the interfacial ion flux and electric field according to the calculated work function and multi-physics phase simulation results. Therefore, the Zn anode with ARL shows preferred plating along with (002) crystal facet and an admirable Coulombic efficiency of 99.86% over 3200 cycles. Zn symmetric cells can withstand large current density up to 40 mA cm-2 and operate stably at 44.2% depth of discharge for 250 hours, surpassing most of published reports. The ARL also enables the Zn||MnO2 full batteries to circulate over 2600 cycles with a high-capacity retention of 80.1% and low self-discharge at 1 A g-1. This work provides a different perspective to comprehend and design satisfactory solid electrolyte interphase for Zn metal anodes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"207 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057306","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

Rational Design of Cobalt-Based Prussian Blue Analogues via 3d Transition Metals Incorporation for Superior Na-Ion Storage

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-30 DOI: 10.1002/anie.202423356

Zhongxin Jing, Muhammad Mamoor, Lingtong Kong, Lu Wang, Bin Wang, Ming Chen, Fengbo Wang, Guangmeng Qu, Yueyue Kong, Dedong Wang, Xiyu He, Chang Wang, Xintong Zhang, Yufei Zhang, Gang Wang, Liqiang Xu

{"title":"Rational Design of Cobalt-Based Prussian Blue Analogues via 3d Transition Metals Incorporation for Superior Na-Ion Storage","authors":"Zhongxin Jing, Muhammad Mamoor, Lingtong Kong, Lu Wang, Bin Wang, Ming Chen, Fengbo Wang, Guangmeng Qu, Yueyue Kong, Dedong Wang, Xiyu He, Chang Wang, Xintong Zhang, Yufei Zhang, Gang Wang, Liqiang Xu","doi":"10.1002/anie.202423356","DOIUrl":"https://doi.org/10.1002/anie.202423356","url":null,"abstract":"Understanding the relationship between structure regulation and electrochemical performance is key to developing efficient and sustainable sodium-ion batteries (SIBs) materials. Herein, seven Cobalt-M-based (M=V, Mn, Fe, Co, Ni, Cu, Zn) Prussian blue analogues (CoM-PBAs) are designed as anodes for SIBs via a universal low-energy co-precipitation approach with the strategic inclusion of 3d transition metals. Density Functional Theory (DFT) simulation and experimental validation reveal that a moderate p-band center of cyanide linkages (-CN-) is more favorable for Na+ intercalation and diffusion, while the d-band center of metal cations is linearly related to electrode stability. Among seven CoM-based PBAs, CoV-PBAs possess the best sodium-ion adsorption/diffusion kinetics and overall cycling performance, including high specific capacity (565 mAh/g at 0.1 A/g), cycling stability (over 15000 cycles with 97.7% capacity retention), and superior rate capability (174.7 mAh/g at 30 A/g). In-situ/ex-situ techniques further demonstrate that the π-electron regulation by V introduction enhances the reversibility and kinetics of redox reactions. Moreover, the study identified the \"p-band center\" and \"d-band center\" may serve as key descriptors for quantifying the capability and stability of other-type bimetal Co-based anodes (oxides, phosphides, sulfides, and selenides) with similar theoretical capacity, offering a potentially transformative approach for selecting practical SIB electrode materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"56 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057309","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

SN2-Reaction-Driven Bonding-Heterointerface Strengthens Buried Adhesion and Orientation for Advanced Perovskite Solar Cells SN2 反应驱动的键合-异质界面增强了先进过氧化物太阳能电池的埋入式粘附力和定向力

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202424046

Naimin Liu, Jialong Duan, Chenlong Zhang, Jinyue Zhang, Yueyang Bi, Linzheng Ma, Dongmei Xu, Jun Gao, Xingxing Duan, Jie Dou, Qiyao Guo, Benlin He, Yuanyuan Zhao, Qunwei Tang

{"title":"SN2-Reaction-Driven Bonding-Heterointerface Strengthens Buried Adhesion and Orientation for Advanced Perovskite Solar Cells","authors":"Naimin Liu, Jialong Duan, Chenlong Zhang, Jinyue Zhang, Yueyang Bi, Linzheng Ma, Dongmei Xu, Jun Gao, Xingxing Duan, Jie Dou, Qiyao Guo, Benlin He, Yuanyuan Zhao, Qunwei Tang","doi":"10.1002/anie.202424046","DOIUrl":"https://doi.org/10.1002/anie.202424046","url":null,"abstract":"Traditionally weak buried interaction without customized chemical bonding always goes against the formation of high-quality perovskite film that highly determines the efficiency and stability of perovskite solar cells. To address this issue, herein, we propose a bimolecular nucleophilic substitution reaction (SN2) driving strategy to idealize the robust buried interface by simultaneously decorating underlying substrate and functionalizing [PbX6]4- octahedral framework with iodoacetamide and thiol molecules, respectively. Theoretical and experimental results demonstrate that a strong SN2 reaction between exposed halogen and thiol group in two molecules occurs, which not only benefits the reinforcement of buried adhesion, but also triggers target-point-oriented crystallization, synergistically upgrading the upper perovskite film quality and accelerating interfacial charge extraction-transfer behavior. Benefiting from the suppressed nonradiative recombination, as a result, an all-air-processed carbon-based all-inorganic CsPbI2Br device achieves an enhanced efficiency of 15.14%, more importantly, with significantly prolonged long-term stability under harsh conditions. This unique reaction-driven buried interface provides a new path for manipulating perovskite growth and obtaining advanced perovskite photovoltaics.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"35 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055536","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

Bias‐Induced Ga‐O‐Ir Interface Breaks the Limits of Adsorption‐Energy Scaling Relationships for High‐Performing Proton Exchange Membrane Electrolyzers

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202419352

Yinnan Qian, Yirun Guo, Zijie Yang, zhaoyan luo, Lei Zhang, Qianling Zhang, Chuanxin He, Hao Zhang, Xueliang Sun, Xiangzhong Ren

{"title":"Bias‐Induced Ga‐O‐Ir Interface Breaks the Limits of Adsorption‐Energy Scaling Relationships for High‐Performing Proton Exchange Membrane Electrolyzers","authors":"Yinnan Qian, Yirun Guo, Zijie Yang, zhaoyan luo, Lei Zhang, Qianling Zhang, Chuanxin He, Hao Zhang, Xueliang Sun, Xiangzhong Ren","doi":"10.1002/anie.202419352","DOIUrl":"https://doi.org/10.1002/anie.202419352","url":null,"abstract":"Rationally manipulating the in‐situ formed catalytically active surface of catalysts remains a significant challenge for achieving highly efficient water electrolysis. Herein, we present a bias‐induced activation strategy to modulate in‐situ Ga leaching and trigger the dynamic surface restructuring of lamellar Ir@Ga2O3 for the electrochemical oxygen evolution reaction. The in‐situ reconstructed Ga‐O‐Ir interface sustains high water oxidation rates at OER overpotentials. We found that OER at the Ga‐O‐Ir interface follows a bi‐nuclear adsorbate evolution mechanism with unsaturated IrOx as the active sites, while GaOx atoms play an indirect role in promoting water dissociation to form OH* and transferring OH* to Ir sites. This breaks the scaling relationship of the adsorption energies between OH* and OOH*, significantly lowering the energy barrier of the rate‐limiting step and greatly increasing reactivity. The Ir@Ga2O3 catalyst achieves lower overpotentials, a current density of 2 A cm‐2 at 1.76 V, and stable operation up to 1 A cm‐2 in scalable PEM electrolyzers at 1.63 V, maintaining stable operation at 1 A cm‐2 over 1000 hours with a degradation rate of 11.5 μV h−1. This work prompted us to jointly address substrate‐catalyst interactions and catalyst reconstruction, an underexplored path, to improve activity and stability in Ir PEMWE anodes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"28 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143054889","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

An Oxidative Stress Nanoamplifier to Enhance the Efficacy of Cisplatin in Head and Neck Cancer

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202421481

Zhenzhen Li, Qiaolin Liu, Guorong Wang, Ru Bai, Shengmin Li, Tao Liu, Qingzhen Wang, Yufeng Peng, Fei Teng, Huige Zhou, Junfang Xian, Chunying Chen

{"title":"An Oxidative Stress Nanoamplifier to Enhance the Efficacy of Cisplatin in Head and Neck Cancer","authors":"Zhenzhen Li, Qiaolin Liu, Guorong Wang, Ru Bai, Shengmin Li, Tao Liu, Qingzhen Wang, Yufeng Peng, Fei Teng, Huige Zhou, Junfang Xian, Chunying Chen","doi":"10.1002/anie.202421481","DOIUrl":"https://doi.org/10.1002/anie.202421481","url":null,"abstract":"Cisplatin (CP) is a first-line platinum-based drug used for the treatment of head and neck cancer. However, tumor cells can diminish the therapeutic effects of CP through the detoxification system mediated by glutathione (GSH) and the nucleotide excision repair (NER) pathway. Herein, we present a light-activable and pH-responsive oxidative stress nanoamplifier (FPLC@IR OSNA), comprising an amphiphilic compound (FPLC) with Fmoc-lysine acting as a connector between a nitroimidazole derivative and a pH-responsive cinnamaldehyde (CA) derivative, loaded with photosensitizer IR780. The acidic microenvironment of lysosome can trigger the release of CA to produce H2O2, which breaks down into oxygen, further improving the phototherapy efficacy mediated by IR780 irradiation. The consumption of oxygen during the phototherapy process induces hypoxia, prompting the reduction of nitroimidazole to aminoimidazole and leading to reduced GSH synthesis, enhancing tumor cell death induced by CP. Meanwhile, the accumulation of intracellular reactive oxygen species (ROS) during phototherapy attenuates the nuclear NER pathway, further augmenting the therapy effect of CP. This strategy, by combining FPLC@IR OSNA with laser and CP, significantly promotes the therapeutic effect in vitro, and notably inhibits tumor growth in both Cal27 cell line-derived xenograft models and patient-derived xenograft models.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"121 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055540","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

Cationic Polyhedral Chalcogenaboranes: Activation without breaking Wade’s Rules

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202419677

Josef Holub, Šimon-Petr Náhlík, Zdeňka Růžičková, Maksim Samsonov, Drahomír Hnyk, Josef Cvačka, Jindřich Fanfrlík, Jan Vrána, Aleš Růžička

引用次数: 0

Regulating Interphase Chemistry by Targeted Functionalization of Hard Carbon Anode in Ester-based Electrolytes for High-Performance Sodium-Ion Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202424028

Guangxiang Zhang, Chuankai Fu, Shuyang Gao, Haoquan Zhao, Chi Ma, Ziwei Liu, Shuai Li, Zhijin Ju, Hua Huo, Pengjian Zuo, Geping Yin, Tiefeng Liu, Yulin Ma

{"title":"Regulating Interphase Chemistry by Targeted Functionalization of Hard Carbon Anode in Ester-based Electrolytes for High-Performance Sodium-Ion Batteries","authors":"Guangxiang Zhang, Chuankai Fu, Shuyang Gao, Haoquan Zhao, Chi Ma, Ziwei Liu, Shuai Li, Zhijin Ju, Hua Huo, Pengjian Zuo, Geping Yin, Tiefeng Liu, Yulin Ma","doi":"10.1002/anie.202424028","DOIUrl":"https://doi.org/10.1002/anie.202424028","url":null,"abstract":"Commercial hard carbon (HC) anode suffers from unexpected interphase chemistry rooted in the parasitic reactions between surface oxygen-functional groups and ester-based electrolytes. Herein, an innovative strategy is proposed to regulate interphase chemistry by tailoring targeted functional groups on the HC surface, where highly active undesirable oxygen-functional groups are skillfully converted into a Si-O-Si molecular layer favorable for anchoring anions. Then, an inorganic/organic hybrid solid electrolyte interphase with low interfacial charge transfer resistance and enhanced cycling durability is constructed successfully. Consequently, the modified HC anode delivers an excellent rate capability of 206.2 mAh g−1 at 0.5 A g−1 and a remarkable capacity retention of 92.5% after 1000 cycles at 1.0 A g−1. Moreover, the coin-type full-cell equipped with Na2Fe[Fe(CN)6] cathode exhibits an exceptional capacity retention ratio of 80.9% after 800 cycles at 1C. The present simple and effective interfacial modification strategy offers a promising and alternative avenue for promoting the development and practicability of HC anode in ester-based electrolytes for sodium-ion batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"53 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055541","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

Ultrasound-Enhanced Spleen-Targeted mRNA Delivery via Fluorinated PEGylated Lipid Nanoparticles for Immunotherapy

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202500878

Minglong Chen, Jie Cen, Qiangqiang Shi, Bing Shao, Jiajia Tan, Xianjun Ye, Zhihua He, Yang Liu, Guoying Zhang, Jinming Hu, Jianqiang Bao, Shiyong Liu

{"title":"Ultrasound-Enhanced Spleen-Targeted mRNA Delivery via Fluorinated PEGylated Lipid Nanoparticles for Immunotherapy","authors":"Minglong Chen, Jie Cen, Qiangqiang Shi, Bing Shao, Jiajia Tan, Xianjun Ye, Zhihua He, Yang Liu, Guoying Zhang, Jinming Hu, Jianqiang Bao, Shiyong Liu","doi":"10.1002/anie.202500878","DOIUrl":"https://doi.org/10.1002/anie.202500878","url":null,"abstract":"Lipid nanoparticles (LNPs) based messenger RNA (mRNA) therapeutics hold immense promise for treating a wide array of diseases, while their nonhepatic organs targeting and insufficient endosomal escape efficiency remain challenges. For LNPs, polyethylene glycol (PEG) lipids have a crucial role in stabilizing them in aqueous medium, but they severely hinder cellular uptake and reduce transfection efficiency. In this study, we designed ultrasound (US)-assisted fluorinated PEGylated LNPs (F-LNPs) to enhance spleen-targeted mRNA delivery and transfection. Through liquid-to-gas phase transition, we enabled the controlled shedding of fluorinated PEG lipids from F-LNPs, facilitating cellular uptake, membrane fusion, and mRNA release. In vivo results demonstrated that US-assisted F-LNPs increased mRNA transfection approximately 4.0-fold in the spleen following intravenous administration. Notably, the F-LNPs achieved effective mRNA delivery to antigen-presenting cell subsets, such as dendritic cells, macrophages, and B cells. The targeted delivery of full-length ovalbumin-encoding mRNA vaccine induced significant CD8+ T cell response and exhibited excellent therapeutic effect against the ovalbumin-transduced B16F10 tumor model. These findings establish a novel strategy for spleen-specific mRNA delivery through the combination of fluorinated PEG lipids and US treatment, which holds substantial promise for enhancing the efficacy of immunotherapy, potentially broadening the scope of clinical applications for mRNA-based therapy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"20 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055545","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