Angewandte Chemie International Edition最新文献

筛选
英文 中文
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
{"title":"Cationic Polyhedral Chalcogenaboranes: Activation without breaking Wade’s Rules","authors":"Josef Holub, Šimon-Petr Náhlík, Zdeňka Růžičková, Maksim Samsonov, Drahomír Hnyk, Josef Cvačka, Jindřich Fanfrlík, Jan Vrána, Aleš Růžička","doi":"10.1002/anie.202419677","DOIUrl":"https://doi.org/10.1002/anie.202419677","url":null,"abstract":"Wade’s rules are a well-established tool for the description of the geometry of inorganic clusters. Among others, they state that a decrease or increase in charge is always accompanied by a change in the number of skeletal electron pairs (SEPs). This work reports the synthesis of the first cationic chalcogenaboranes closo-[12-X-2-IPr-1-EB11H10]BF4 (X = H, I; E = S, Se 3a/b, 4a/b) featuring the same SEP count as their neutral precursors, EB11H11, but bearing a positive charge. This ionisation significantly enhances the activity towards the electrophiles. It unlocks reactivity with very weak bases and offers the control of the regioselectivity towards hard/soft bases by the modulation of LUMO. The localisation of the positive charge within the borane cluster has been confirmed experimentally, spectroscopically and theoretically.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"49 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055538","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
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
Enantioselective Borylcupration/Cyclization of Alkene‐Tethered Oxime Esters
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202420479
Jonathan Bajohr, Shangyu Li, Bijan Mirabi, Colton E. Johnson, Mark Lautens
{"title":"Enantioselective Borylcupration/Cyclization of Alkene‐Tethered Oxime Esters","authors":"Jonathan Bajohr, Shangyu Li, Bijan Mirabi, Colton E. Johnson, Mark Lautens","doi":"10.1002/anie.202420479","DOIUrl":"https://doi.org/10.1002/anie.202420479","url":null,"abstract":"A copper‐catalyzed enantioselective synthesis of borylated 1‐pyrrolines from γ,δ‐unsaturated oxime esters is reported. Twenty‐four novel 1‐pyrroline derivatives are reported in yields ranging from 26% to 96% and enantioselectivities from 74.5:25.5 er to 99:1 er. Examples derived from α‐unsubstituted, non‐fluorinated oxime esters are reported. The hydroxyl group following oxidation of the Bpin moiety acts as a directing group in highly diastereoselective reductions of the pyrrolines to the corresponding prolinol derivatives. Additionally, the Bpin group can be retained in the products following a simplified, chromatography‐free workup procedure. DFT supports a reaction mechanism which proceeds through the formation of an (R)‐benzylic copper intermediate, followed by stereoretentive cyclization with respect to the configuration at the metalated carbon. The conclusions of the computational data are corroborated through control experiments and deuterium‐labelling studies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"39 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143054890","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
Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202423878
Aeli Olson, Briana Schrage, Md Faizul Islam, Lesta Fletcher, Francesca Verich, Morgan Dierolf, Eduardo Aluicio-Sarduy, Kaelyn Becker, Darren Driscoll, Nidhi Girish, Megan Simms, Vilmos Kertesz, Frankie White, Eszter Boros, Alexander Ivanov, Jonathan Engle, Nikki A. Thiele
{"title":"Towards the Stable Chelation of Radioantimony(V) for Targeted Auger Theranostics","authors":"Aeli Olson, Briana Schrage, Md Faizul Islam, Lesta Fletcher, Francesca Verich, Morgan Dierolf, Eduardo Aluicio-Sarduy, Kaelyn Becker, Darren Driscoll, Nidhi Girish, Megan Simms, Vilmos Kertesz, Frankie White, Eszter Boros, Alexander Ivanov, Jonathan Engle, Nikki A. Thiele","doi":"10.1002/anie.202423878","DOIUrl":"https://doi.org/10.1002/anie.202423878","url":null,"abstract":"Antimony-119 (119Sb) is one of the most attractive Auger-electron emitters identified to date, but it remains practically unexplored for targeted radiotherapy because no chelators have been identified to stably bind this metalloid in vivo. In a departure from current studies focused on chelator development for Sb(III), we explore the chelation chemistry of Sb(V) using the tris-catecholate ligand TREN-CAM. Through a combination of radiolabeling, spectroscopic, solid-state, and computational studies, the radiochemistry and structural chemistry of TREN-CAM with 1XX/natSb(V) were established. The resulting [1XXSb]Sb–TREN-CAM complex remained intact for several days in human serum, signifying high stability under biological conditions. Finally, the first in vivo single photon emission computed tomography and positron emission tomography imaging studies were carried out using 117Sb, the diagnostic analogue of 119Sb. These studies revealed marked differences in the uptake/distribution of activity in mice administered unchelated [117Sb]Sb(OH)6– versus [117Sb]Sb–TREN-CAM, suggesting that 117Sb is largely retained by TREN-CAM over the time course of the study. Collectively, these findings demonstrate the most physiologically stable complex of no-carrier-added 1XXSb yet reported, offering new promise for the clinical implementation of radioantimony in nuclear medicine. Our results also establish the feasibility of 117Sb as an elementally matched partner to 119Sb for theranostic applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055537","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
Putting Charge Transfer Degree as a Bridge Connecting Surface-Enhanced Raman Spectroscopy and Photocatalysis
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-01-29 DOI: 10.1002/anie.202424986
Junjie Chen, Mengyuan Li, Xinmeng Wang, Hongye Liu, Wenji Jiang, Bing Zhao, Wei Song
{"title":"Putting Charge Transfer Degree as a Bridge Connecting Surface-Enhanced Raman Spectroscopy and Photocatalysis","authors":"Junjie Chen, Mengyuan Li, Xinmeng Wang, Hongye Liu, Wenji Jiang, Bing Zhao, Wei Song","doi":"10.1002/anie.202424986","DOIUrl":"https://doi.org/10.1002/anie.202424986","url":null,"abstract":"To date, few systematic approach has been established for predicting catalytic performance by analyzing the spectral information of molecules adsorbed on photocatalyst surfaces. Effective charge transfer (CT) between the semiconductor photocatalysts and surface-absorbed molecules is essential for enhancing catalytic activity and optimizing light energy utilization. This study aimed to validate the surface-enhanced Raman spectroscopy (SERS) based on the CT enhancement mechanism in investigating the CT process during semiconductor photocatalytic C–C coupling model reactions. A copper ion doping strategy was employed to simultaneously enhance the SERS effect and catalytic activity of zinc oxide (ZnO) derived from metal-organic framework (MOF). By analyzing molecular fingerprint SERS spectra, we calculated the degree of CT (ρCT), revealing that SERS enhancement is attributed to the CT mechanism. In-situ SERS spectra confirmed a high correlation between the catalytic activity and ρCT of ZnO with varying copper ion doping levels. A range of photoelectric and spectroscopic tests validated the effectiveness of SERS in linking CT to photocatalytic performance, consistent with first-principles density functional theory (DFT) simulations. This finding is also validated in other semiconductor materials and catalytic reactions, demonstrating the broad applicability of ρCT for predicting and evaluating SERS and catalytic activity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"119 1 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055543","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信