Visible Light-Driven Radical-Mediated C-C Bond Cleavage/Functionalization in Organic Synthesis
作者：
Yu, Xiao-Ye;Chen, Jia-Rong* ;Xiao, Wen-Jing*
期刊：
CHEMICAL REVIEWS ,2021年121(1):506-561 ISSN：0009-2665
通讯作者：
Chen, Jia-Rong;Xiao, Wen-Jing
作者机构：
[Chen, Jia-Rong; Xiao, WJ; Xiao, Wen-Jing; Yu, Xiao-Ye] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Chen, JR; Xiao, WJ] C;Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Thermal C-C bond cleavage reactions allow the construction of structurally diverse molecular skeletons via predictable and efficient bond reorganizations. Visible light photoredox-catalyzed radical-mediated C-C bond cleavage reactions have recently emerged as a powerful alternative method for overcoming the thermodynamic and kinetic barrier of C-C bond cleavage in diverse molecular scaffolds. In recent years, a plethora of elegant and useful reactions have been invented, and the products are sometimes otherwise inaccessible by classic thermal reactions. Considering the great influence and synthetic potential of these reactions, we provide a summary of the state of art visible light-driven radical-mediated C-C bond cleavage/functionalization strategies with a specific emphasis on the working models. We hoped that this review will be useful for medicinal and synthetic organic chemists and will inspire further reaction development in this interesting area. © 2021 American Chemical Society. All rights reserved.
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英文
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Guidelines for the use and interpretation of assays for monitoring autophagy (4th edition)1
作者：
Klionsky, Daniel J.* ;Abdel-Aziz, Amal Kamal;Abdelfatah, Sara;Abdellatif, Mahmoud;Abdoli, Asghar;...
期刊：
Autophagy ,2021年17(1):1-382 ISSN：1554-8627
通讯作者：
Klionsky, Daniel J.
作者机构：
[Huang, Yuxiang Jack; Hawkins, Wayne D.; Zhang, Zhihai; Lei, Yuchen; Lahiri, Vikramjit; Klionsky, Daniel J.; Ariosa, Aileen R.; Yin, Zhangyuan; Wen, Xin; Yang, Ying; Gatica, Damian; Lin, Jiandie D.; Delorme-Axford, Elizabeth; Metur, Shree Padma; Popelka, Hana] Univ Michigan, Life Sci Inst, Ann Arbor, MI 48109 USA.;[Huang, Yuxiang Jack; Hawkins, Wayne D.; Xu, Haoxing; Zhang, Zhihai; Lei, Yuchen; Zhang, Xiaoyan; Lahiri, Vikramjit; Klionsky, Daniel J.; Li, Ming; Yin, Zhangyuan; Wen, Xin; Yang, Ying; Gatica, Damian; Metur, Shree Padma; Wang, Yanzhuang] Univ Michigan, Dept Mol Cellular & Dev Biol, Ann Arbor, MI 48109 USA.;[Abdel-Aziz, Amal Kamal] Ain Shams Univ, Fac Pharm, Dept Pharmacol & Toxicol, Cairo, Egypt.;[Chiocca, Susanna; Abdel-Aziz, Amal Kamal] European Inst Oncol IRCCS, Dept Expt Oncol, IEO, Milan, Italy.;[Efferth, Thomas; Abdelfatah, Sara] Johannes Gutenberg Univ Mainz, Inst Pharmaceut & Biomed Sci, Dept Pharmaceut Biol, Mainz, Germany.
通讯机构：
[Klionsky, Daniel J.] U;Univ Michigan, Dept Mol Cellular & Dev Biol, Ann Arbor, MI 48109 USA.
关键词：
Autophagosome;cancer;flux;LC3;lysosome;macroautophagy;neurodegeneration;phagophore;stress;vacuole
摘要：
In 2008, we published the first set of guidelines for standardizing research in autophagy. Since then, this topic has received increasing attention, and many scientists have entered the field. Our knowledge base and relevant new technologies have also been expanding. Thus, it is important to formulate on a regular basis updated guidelines for monitoring autophagy in different organisms. Despite numerous reviews, there continues to be confusion regarding acceptable methods to evaluate autophagy, especially in multicellular eukaryotes. Here, we present a set of guidelines for investigators to select and interpret methods to examine autophagy and related processes, and for reviewers to provide realistic and reasonable critiques of reports that are focused on these processes. These guidelines are not meant to be a dogmatic set of rules, because the appropriateness of any assay largely depends on the question being asked and the system being used. Moreover, no individual assay is perfect for every situation, calling for the use of multiple techniques to properly monitor autophagy in each experimental setting. Finally, several core components of the autophagy machinery have been implicated in distinct autophagic processes (canonical and noncanonical autophagy), implying that genetic approaches to block autophagy should rely on targeting two or more autophagy-related genes that ideally participate in distinct steps of the pathway. Along similar lines, because multiple proteins involved in autophagy also regulate other cellular pathways including apoptosis, not all of them can be used as a specific marker for bona fide autophagic responses. Here, we critically discuss current methods of assessing autophagy and the information they can, or cannot, provide. Our ultimate goal is to encourage intellectual and technical innovation in the field. © 2020 Informa UK Limited, trading as Taylor & Francis Group.
语种：
英文
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When Nanozymes Meet Single-Atom Catalysis
作者：
Jiao, Lei;Yan, Hongye;Wu, Yu;Gu, Wenling;Zhu, Chengzhou* ;...
期刊：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2020年59(7):2565-2576 ISSN：1433-7851
通讯作者：
Zhu, Chengzhou;Lin, Yuehe
作者机构：
[Zhu, Chengzhou; Yan, Hongye; Wu, Yu; Jiao, Lei; Gu, Wenling] Cent China Normal Univ Wuhan, Key Lab Pesticide & Chem Biol, Int Joint Res Ctr Intelligent Biosensing Technol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构：
[Zhu, Chengzhou] C;[Lin, Yuehe] W;Cent China Normal Univ Wuhan, Key Lab Pesticide & Chem Biol, Int Joint Res Ctr Intelligent Biosensing Technol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
关键词：
biosensors;nanozymes;organic pollutant degradation;SAzymes;therapeutic drugs
摘要：
Nanomaterials with enzyme-like activities, coined nanozymes, have been researched widely as they offer unparalleled advantages in terms of low cost, superior activity, and high stability. The complex structure and composition of nanozymes has led to extensive investigation of their catalytic sites at an atomic scale, and to an in-depth understanding of the biocatalysis occurring. Single-atom catalysts (SACs), characterized by atomically dispersed active sites, have provided opportunities for mimicking metalloprotease and for bridging the gap between natural enzymes and nanozymes. In this Minireview, we illustrate the unique properties of nanozymes and we discuss recent advances in the synthesis, characterization, and applications of SACs. Subsequently, we outline the impressive progress made in single-atom nanozymes and we discuss their applications in sensing, degradation of organic pollutants, and in therapeutic roles. Finally, we present the major challenges and opportunities remaining for a successful marriage of nanozymes and SACs. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
语种：
英文
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When Light Meets Nitrogen-Centered Radicals: From Reagents to Catalysts
作者：
Yu, Xiao-Ye;Zhao, Quan-Qing;Chen, Jun;Xiao, Wen-Jing;Chen, Jia-Rong*
期刊：
ACCOUNTS OF CHEMICAL RESEARCH ,2020年53(5):1066-1083 ISSN：0001-4842
通讯作者：
Chen, Jia-Rong
作者机构：
[Zhao, Quan-Qing; Xiao, Wen-Jing; Chen, Jun; Chen, Jia-Rong; Yu, Xiao-Ye] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Chen, Jia-Rong] C;Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
ConspectusNitrogen-centered radicals (NCRs) are a versatile class of highly reactive species that have a longer history than the classical carbon-based radicals in synthetic chemistry. Depending on the N-hybridization and substitution patterns, NCRs can serve as electrophiles or nucleophiles to undergo various radical transformations. Despite their power, progress in nitrogen-radical chemistry is still slow compared with the popularity of carbon radicals, and their considerable synthetic potential has been largely underexplored, which is, as concluded by Zard, mainly hampered by "a dearth of convenient access to these species and a lack of awareness pertaining to their reactivity".Over the past decade, visible-light photoredox catalysis has been established as a powerful toolbox that synthetic chemists can use to generate a diverse range of radical intermediates from native organic functional groups via a single electron transfer process or energy transfer under mild reaction conditions. This catalytic strategy typically obviates the need for external stoichiometric activation reagents or toxic initiators and often enables traditionally inaccessible ionic chemical reactions. On the basis of our long-standing interest in nitrogen chemistry and catalysis, we have emphasized the use of visible-light photoredox catalysis as a tactic to discover and develop novel methods for generating NCRs in a controlled fashion and synthetic applications. In this Account, we describe our recent advances in the development of visible-light-driven photoredox-catalyzed generation of NCRs and their synthetic applications.Inspired by the natural biological proton-coupled electron transfer (PCET) process, we first developed a strategy of visible-light-driven photoredox-catalyzed oxidative deprotonation electron transfer to activate the N-H bonds of hydrazones, benzamides, and sulfonamides to give the corresponding NCRs under mild reaction conditions. With these reactive species, we then achieved a range of 5-exo and 6-endo radical cyclizations as well as cascade reactions in a highly regioselective manner, providing access to a variety of potentially useful nitrogen heterocycles. To further expand the repertoire of possible reactions of NCRs, we also revealed that iminyl radicals, derived from O-acyl cycloalkanone oxime esters, can undergo facile ring-opening C-C bond cleavage to give cyanoalkyl radicals. These newly formed radical species can further undergo a variety of C-C bond-forming reactions to allow the synthesis of diverse distally functionalized alkyl nitriles. Stimulated by these studies, we further developed a wide variety of visible-light-driven copper-catalyzed radical cross-coupling reactions of cyanoalkyl radicals. Because of their inherent highly reactive and transient properties, the strategy of heteroatom-centered radical catalysis is still largely underexplored in organic synthesis. Building on our understanding of the fundamental chemistry of NCRs, we also developed for the first time the concept of NCR covalent catalysis, which involves the use of in situ-photogenerated NCRs to activate allyl sulfones, vinylcyclopropanes, and N-tosyl vinylaziridines. This catalytic strategy has thus enabled efficient difunctionalization of various alkenes and late-stage modification of complex biologically active molecules.In this Account, we describe a panoramic picture of our recent contributions since 2014 to the development and application of the visible-light-driven photoredox systems in the field of NCR chemistry. These studies provide not only efficient methods for the synthesis of functionally rich molecules but also some insight into the exploration of new reactivity or reaction modes of NCRs. © 2020 American Chemical Society.
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英文
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Coupling coordination degree measurement and spatiotemporal heterogeneity between economic development and ecological environment ----Empirical evidence from tropical and subtropical regions of China
作者：
Shi, Tao;Yang, Shenyan* ;Zhang, Wei;Zhou, Qian
期刊：
Journal of Cleaner Production ,2020年244:118739 ISSN：0959-6526
通讯作者：
Yang, Shenyan
作者机构：
[Shi, Tao] Chinese Acad Governance, Party Sch Cent Comm CPC, Sch Econ Teaching & Res, Beijing, Peoples R China.;[Yang, Shenyan] Hubei Univ Econ, Sch Finance, Wuhan, Hubei, Peoples R China.;[Zhang, Wei] Cent China Normal Univ, Sch Publ Policy & Management, Wuhan, Hubei, Peoples R China.;[Yang, Shenyan] Hubei Financial Dev & Financial Secur Res Ctr, Wuhan, Hubei, Peoples R China.;[Zhou, Qian] Shanghai Univ Finance & Econ, Sch Shanghai Dev, Shanghai, Peoples R China.
通讯机构：
[Yang, Shenyan] H;Hubei Univ Econ, Sch Finance, Wuhan, Hubei, Peoples R China.
关键词：
Economic development;Ecological environment;Geographically and temporally weighted regression;Tropical and subtropical regions;China
摘要：
Along with the rapid economic development, China's ecological environment is becoming an increasingly severe issue with strong negative externalities accelerating the spatial spillover. This paper uses Geographically and Temporally Weighted Regression (GTWR) to measure and analyze the coupling coordination and spatiotemporal heterogeneity between economic development and ecological environment of 17 tropical and subtropical regions in China from 2003 to 2016. The results show that: First, there is a significant spatiotemporal heterogeneity between economic development and ecological environment; Second, economic development and ecological environment are in an intermediate coupling coordination stage, relative more regions belonged to economic lag type; Third, the ecological lag type mainly lies in developed areas in the east, while the economic lag type is mainly in the central and western regions. Fourth, the spatial relationship and agglomeration effect of economic development are both positive, and the spatial relationship of ecological environment also tends to be positive. Fifth, the interaction relationship between economic development and ecological environment tends to converge. The negative interaction effect of the economic development and ecological environment tends to concentrate in central and eastern developed area, while the positive interaction effect tends to concentrate in central and western developing area. Finally, the paper puts forward corresponding policy recommendations. (C) 2019 Elsevier Ltd. All rights reserved.
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英文
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Non-noble metal-nitride based electrocatalysts for high-performance alkaline seawater electrolysis
作者：
Yu, Luo;Zhu, Qing;Song, Shaowei;McElhenny, Brian;Wang, Dezhi;...
期刊：
Nature Communications ,2019年10(1):5106 ISSN：2041-1723
通讯作者：
Yu, Ying;Chen, Shuo;Ren, Zhifeng
作者机构：
[Yu, Ying; Yu, Luo] Cent China Normal Univ, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China.;[McElhenny, Brian; Chen, Shuo; Yu, Luo; Song, Shaowei; Wang, Dezhi; Ren, Zhifeng; Zhu, Qing] Univ Houston, Dept Phys, Houston, TX 77204 USA.;[McElhenny, Brian; Chen, Shuo; Yu, Luo; Song, Shaowei; Wang, Dezhi; Ren, Zhifeng; Zhu, Qing] Univ Houston, TcSUH, Houston, TX 77204 USA.;[Song, Shaowei; Zhu, Qing] Univ Houston, Mat Sci & Engn Program, Houston, TX 77204 USA.;[Qin, Zhaojun; Bao, Jiming; Wu, Chunzheng] Univ Houston, Dept Elect & Comp Engn, Houston, TX 77204 USA.
通讯机构：
[Yu, Ying] C;[Chen, S; Ren, ZF] U;Cent China Normal Univ, Coll Phys Sci & Technol, Wuhan 430079, Hubei, Peoples R China.;Univ Houston, Dept Phys, Houston, TX 77204 USA.;Univ Houston, TcSUH, Houston, TX 77204 USA.
摘要：
Seawater is one of the most abundant natural resources on our planet. Electrolysis of seawater is not only a promising approach to produce clean hydrogen energy, but also of great significance to seawater desalination. The implementation of seawater electrolysis requires robust and efficient electrocatalysts that can sustain seawater splitting without chloride corrosion, especially for the anode. Here we report a three-dimensional core-shell metal-nitride catalyst consisting of NiFeN nanoparticles uniformly decorated on NiMoN nanorods supported on Ni foam, which serves as an eminently active and durable oxygen evolution reaction catalyst for alkaline seawater electrolysis. Combined with an efficient hydrogen evolution reaction catalyst of NiMoN nanorods, we have achieved the industrially required current densities of 500 and 1000 mA cm−2 at record low voltages of 1.608 and 1.709 V, respectively, for overall alkaline seawater splitting at 60 °C. This discovery significantly advances the development of seawater electrolysis for large-scale hydrogen production. © 2019, The Author(s).
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英文
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