Angewandte Chemie最新文献_第5页

Structurally Engineering Multi-Shell Hollow Zeolite Single Crystals via Defect-Directed Oriented-Kinetics Transformation and Their Heterostructures for Hydrodeoxygenation Reaction 多壳中空沸石单晶的缺陷定向动力学转化及其加氢脱氧反应异质结构

Angewandte Chemie Pub Date : 2025-04-14 DOI: 10.1002/ange.202424690

Guangrui Chen, Peihong She, Ji Han, Junyan Li, Ge Tian, Yuanbo Sun, Yanjing Gao, Guoju Yang, Zhenheng Diao, Buyuan Guan, Jihong Yu

{"title":"Structurally Engineering Multi-Shell Hollow Zeolite Single Crystals via Defect-Directed Oriented-Kinetics Transformation and Their Heterostructures for Hydrodeoxygenation Reaction","authors":"Guangrui Chen, Peihong She, Ji Han, Junyan Li, Ge Tian, Yuanbo Sun, Yanjing Gao, Guoju Yang, Zhenheng Diao, Buyuan Guan, Jihong Yu","doi":"10.1002/ange.202424690","DOIUrl":"https://doi.org/10.1002/ange.202424690","url":null,"abstract":"Single-crystalline multi-shell hollow porous materials with high compartment capacity, large active surface area, and superior structural stability are expected to unlock tremendous potential across diverse critical applications. However, their synthetic methodology has not yet been well established. Here, we develop a defect-directed oriented-kinetics transformation approach to prepare multi-shell hollow aluminosilicate ZSM-5 zeolite (MFI) crystals with single-crystalline feature, hierarchical macro-/mesoporosity, controllable shell number, and high structural stability. The methodology lies in the creation of zeolite precursors consisting of multiple inhomogeneous layers with gradient-distributed defects along the [100] and [010] directions and irregularly discrete defects-rich regions along the [001] direction via continuous epitaxial growth. Subsequently, the locations with more defects could be preferentially etched to form voids or mesopores, meanwhile oriented recrystallization interconnects the nanoshells into a unified architecture along the [001] direction. Benefiting from the easily accessible bifunctional metal/acid sites and the capability for reactant accumulation, the resultant multi-shell hollow Ni-loaded zeolite catalysts show significantly enhanced catalytic activity in the hydrodeoxygenation of stearic acid into liquid fuels. The insight gained from this systematic study will facilitate the rational design and synthesis of diverse multi-shell hollow structured single-crystalline porous materials for a broad range of potential applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 24","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thirupathi Ravula Thirupathi Ravula

Angewandte Chemie Pub Date : 2025-04-14 DOI: 10.1002/ange.202507462

Thirupathi Ravula

引用次数: 0

Isolated and Paired Metal Sites in Zeolites Using Solid-State Ion Exchange 固体离子交换在沸石中的分离和配对金属位

Angewandte Chemie Pub Date : 2025-04-12 DOI: 10.1002/ange.202505186

Rio G. Moore, James M. Crawford

引用次数: 0

Integrating Ambient Ionization Mass Spectrometry Imaging and Spatial Transcriptomics on the Same Cancer Tissues to Identify RNA–Metabolite Correlations 整合环境电离质谱成像和空间转录组学在相同的癌症组织中识别rna -代谢物的相关性

Angewandte Chemie Pub Date : 2025-04-11 DOI: 10.1002/ange.202502028

Trevor M. Godfrey, Yasmin Shanneik, Wanqiu Zhang, Thao Tran, Nico Verbeeck, Nathan H. Patterson, Faith E. Jackobs, Chandandeep Nagi, Maheshwari Ramineni, Livia S. Eberlin

{"title":"Integrating Ambient Ionization Mass Spectrometry Imaging and Spatial Transcriptomics on the Same Cancer Tissues to Identify RNA–Metabolite Correlations","authors":"Trevor M. Godfrey, Yasmin Shanneik, Wanqiu Zhang, Thao Tran, Nico Verbeeck, Nathan H. Patterson, Faith E. Jackobs, Chandandeep Nagi, Maheshwari Ramineni, Livia S. Eberlin","doi":"10.1002/ange.202502028","DOIUrl":"https://doi.org/10.1002/ange.202502028","url":null,"abstract":"Innovations in spatial omics technologies applied to human tissues have led to breakthrough discoveries in various diseases, including cancer. Two of these approaches—spatial transcriptomics and spatial metabolomics—have blossomed independently, fueled by technologies such as spatial transcriptomics (ST) and mass spectrometry imaging (MSI). Although powerful, these technologies only offer insights into the spatial distributions of restricted classes of molecules and have not yet been integrated to provide more holistic insights into biological questions. These techniques can be performed on adjacent serial sections from the same sample, but section-to-section variability can convolute data integration. We present a novel method combining desorption electrospray ionization mass spectrometry imaging (DESI-MSI) spatial metabolomics and Visium spatial transcriptomics on the same tissue sections. We show that RNA quality is maintained after performing DESI-MSI on a tissue under ambient conditions and that ST data is unperturbed following DESI-MSI. We demonstrate this workflow on human breast and lung cancer tissues and identify novel correlations between metabolites and mRNA transcripts in cancer-specific tissue regions.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 24","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232418","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Catalytic Asymmetric Synthesis of Chiral Caged Hydrocarbons as Arenes Bioisosteres 催化不对称合成手性笼型芳烃生物同分酯

Angewandte Chemie Pub Date : 2025-04-11 DOI: 10.1002/ange.202505803

Xue-Chun Yang, Ji-Jie Wang, Yuanjiu Xiao, Jian-Jun Feng

{"title":"Catalytic Asymmetric Synthesis of Chiral Caged Hydrocarbons as Arenes Bioisosteres","authors":"Xue-Chun Yang, Ji-Jie Wang, Yuanjiu Xiao, Jian-Jun Feng","doi":"10.1002/ange.202505803","DOIUrl":"https://doi.org/10.1002/ange.202505803","url":null,"abstract":"The utilization of caged hydrocarbons as bioisosteres for arenes, especially the phenyl ring, in bioactive compounds has resulted in significant enhancements in potency, solubility, and metabolic stability. These improvements highlight the potential of C(sp3)-rich polycyclic scaffolds as a promising motif for the development of drug candidates. However, this strategy has also increased the structural complexity of these molecules, posing synthetic challenges in controlling the chirality of caged and highly decorated bioactive scaffolds. Over the past two years, remarkable progress has been achieved in catalytic asymmetric methodologies for the synthesis of caged hydrocarbons, significantly advancing their utility in chiral drug discovery and development. This minireview provides a comprehensive summary of recent breakthroughs in the catalytic asymmetric synthesis of chiral caged hydrocarbons, encompassing bicyclo[n.1.1]alkanes, cubanes, and related three-dimensional scaffolds. Additionally, we highlight the intriguing applications of enantiomerically pure caged hydrocarbons in biological studies. It is anticipated that this minireview will inspire further advancements in the enantioselective synthesis of these pharmaceutically valuable caged hydrocarbons.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 24","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232419","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dandan Gao

Angewandte Chemie Pub Date : 2025-04-10 DOI: 10.1002/ange.202507344

Dandan Gao

引用次数: 0

Chularat Wattanakit Chularat Wattanakit

Angewandte Chemie Pub Date : 2025-04-10 DOI: 10.1002/ange.202507242

Chularat Wattanakit

引用次数: 0

ATP-Assisted Electron and Proton Transfer Boosting Redox Metabolism-Induced Ferroptosis and Apoptosis for Cancer Therapy atp辅助电子和质子转移促进氧化还原代谢诱导的铁下垂和细胞凋亡的癌症治疗

Angewandte Chemie Pub Date : 2025-04-09 DOI: 10.1002/ange.202504542

Shangjie An, Wenyao Zhen, Yue Wang, Xiaodan Jia, Xiue Jiang

{"title":"ATP-Assisted Electron and Proton Transfer Boosting Redox Metabolism-Induced Ferroptosis and Apoptosis for Cancer Therapy","authors":"Shangjie An, Wenyao Zhen, Yue Wang, Xiaodan Jia, Xiue Jiang","doi":"10.1002/ange.202504542","DOIUrl":"https://doi.org/10.1002/ange.202504542","url":null,"abstract":"Compared to the intractability of traditional apoptosis, the vulnerability exposed by cancer cell metabolic reprogramming provides an advantage for ferroptosis treatment. Herein, we developed vanadate and aurintricarboxylic acid coordination nanoparticles (VAP NPs) that synergistically trigger dual cell death pathways. This nanoplatform leveraged dual-Russell mechanisms and Fenton reactions to generate singlet oxygen/hydroxyl radicals in the tumor microenvironment (TME) while depleting glutathione via vanadium redox cycling, thereby silencing glutathione peroxidase 4 and modulating the Kelch-like ECH-associated protein 1 (KEAP1)/nuclear factor erythroid 2-related factor 2 (NRF2)/heme oxygenase 1 (HMOX1) axis. Notably, TME-overexpressed adenosine triphosphate (ATP) acted as a biochemical catalyst, accelerating the transfer of protons and electrons during reactive oxygen species generation to amplify therapeutic efficacy. Therefore, VAP NPs could achieve outstanding efficacy for intrinsically stimulated synergy of ferroptosis and apoptosis in tumor therapy. This study provides reference for revealing the new function of ATP in enhancing the regulation of redox metabolism.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 24","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Oxidative Rearrangements of the Alkaloid Intermediate Geissoschizine 生物碱中间体葛缕荆的氧化重排

Angewandte Chemie Pub Date : 2025-04-09 DOI: 10.1002/ange.202501323

Mohamed O. Kamileen, Benke Hong, Klaus Gase, Maritta Kunert, Lorenzo Caputi, Benjamin R. Lichman, Sarah E. O'Connor

{"title":"Oxidative Rearrangements of the Alkaloid Intermediate Geissoschizine","authors":"Mohamed O. Kamileen, Benke Hong, Klaus Gase, Maritta Kunert, Lorenzo Caputi, Benjamin R. Lichman, Sarah E. O'Connor","doi":"10.1002/ange.202501323","DOIUrl":"https://doi.org/10.1002/ange.202501323","url":null,"abstract":"Plants can generate structural diversity by enzymatic rearrangement of a central intermediate. 19E-geissoschizine is one such chemically versatile intermediate that plays a central role in the biosynthesis of monoterpene indole alkaloids such as strychnine, ibogaine, and vinblastine. Here we report how 19E-geissoschizine undergoes oxidative transformations to generate four distinct alkaloid scaffolds through the action of three biosynthetic enzymes. Using in vitro enzymatic assays and gene silencing, we demonstrate how these three cytochrome P450 enzymes in the medicinal plant Catharanthus roseus transform 19E-geissoschizine into strychnos, sarpagan, akuammiline-type, and mavacurane-type alkaloids. We use mutational analysis to show how minimal changes to the active site of these similar enzymes modulate product specificity. This work highlights how substrate reactivity and enzyme mutations work synergistically to generate chemical diversity.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 24","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202501323","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemical Amination of Aryl Halides with NH3 芳基卤化物的NH3电化学胺化

Angewandte Chemie Pub Date : 2025-04-09 DOI: 10.1002/ange.202504459

Yaowen Liu, Yanfei Sun, Yuan Deng, Youai Qiu

引用次数: 0