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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Enantioselective Radical Carbocyanation of 1,3-Dienes via Photocatalytic Generation of Allylcopper Complexes
作者：
Lu, Fu-Dong;Lu, Liang-Qiu;He, Gui-Feng;Bai, Jun-Chuan;Xiao, Wen-Jing
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2021年143(11):4168-4173 ISSN：0002-7863
通讯作者：
Wen-Jing Xiao
作者机构：
[Lu, Fu-Dong; Lu, Liang-Qiu; Bai, Jun-Chuan; Xiao, Wen-Jing; He, Gui-Feng] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Lu, Liang-Qiu] Chinese Acad Sci, Lanzhou Inst Chem Phys LICP, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China.;[Xiao, Wen-Jing] Chinese Acad Sci, Shanghai Inst Organ Chem, State Key Lab Organometall Chem, Shanghai 200032, Peoples R China.
通讯机构：
[Xiao, W.-J.] C;CCNU-uOttawa Joint Research Centre, 152 Luoyu Road, China
摘要：
1,3-Dienes are readily available feedstocks that are widely used in the laboratory and industry. However, the potential of converting 1,3-dienes into value-added products, especially chiral products, has not yet been fully exploited. By synergetic photoredox/copper catalysis, we achieve the first visible-light-induced, enantioselective carbocyanation of 1,3-dienes by using carboxylic acid derivatives and trimethylsilyl cyanide. Under mild and neutral conditions, a diverse range of chiral allyl cyanides are produced in generally good efficiency and with high enantioselectivity from bench-stable and user-safe chemicals. Moreover, preliminary results also confirm that this success can be expanded to 1,3-enynes and the four-component carbonylative carbocyanation of 1,3-dienes and 1,3-enynes.
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英文
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Single-Atom catalysts boost signal amplification for biosensing
作者：
Jiao, Lei;Xu, Weiqing;Wu, Yu;Yan, Hongye;Gu, Wenling;...
期刊：
CHEMICAL SOCIETY REVIEWS ,2021年50(2):750-765 ISSN：0306-0012
通讯作者：
Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn)
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Yan, Hongye; Wu, Yu; Jiao, Lei; Gu, Wenling] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Du, Dan; Lin, Yuehe] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构：
[Jiao, Lei] K;[Du, Dan] S;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan, 430079, P. R. China.;School of Mechanical and Materials Engineering, Washington State University, Pullman, WA 99164, USA. yuehe.
摘要：
Development of highly sensitive biosensors has received ever-increasing attention over the years. Due to the unique physicochemical properties, the functional nanomaterial-enabled signal amplification strategy has made some great breakthroughs in biosensing. However, the sensitivity and selectivity still need further improvement. Single-Atom catalysts (SACs) containing atomically dispersed metal active sites demonstrate distinctive advantages in catalytic activity and selectivity for various catalytic reactions. As a consequence, the SAC-enabled signal amplification strategy holds great promise in biosensors, demonstrating satisfactory sensitivity and selectivity with the assistance of tunable metal-support interactions, coordination environments and geometric/electronic structures of active sites. In this tutorial review, we briefly discuss the structural advantages of SACs. Then, the catalytic mechanism at the atomic scale and signal amplification effects of SACs in the colorimetric, electrochemical, chemiluminescence, electrochemiluminescence, and photoelectrochemical biosensing applications are highlighted in detail. Finally, opportunities and challenges to be faced in the future development of the SAC-enabled signal amplification strategy for biosensing are discussed and outlooked. © The Royal Society of Chemistry.
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Reactive oxygen species, thiols and enzymes activable AIEgens from single fluorescence imaging to multifunctional theranostics
作者：
Li, Jun;Zhang, Yi;Wang, Pengzhan;Yu, Le;An, Jusung;...
期刊：
Coordination Chemistry Reviews ,2021年427:213559 ISSN：0010-8545
通讯作者：
Deng, Ganzhen;Sun, Yao;Kim, Jong Seung
作者机构：
[Li, Jun] Huazhong Agr Univ, Coll Sci, Dept Chem, Wuhan 430070, Peoples R China.;[Deng, Ganzhen] Huazhong Agr Univ, Coll Anim Sci & Vet Med, State Key Lab Agr Microbiol, Wuhan 430070, Peoples R China.;[Zhang, Yi; Sun, Yao] Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[An, Jusung; Kim, Jong Seung; Yu, Le] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Wang, Pengzhan] Hubei Univ, Key Lab Synth & Applicat Organ, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Minist Educ,Funct Mol, Wuhan 430062, Peoples R China.
通讯机构：
[Deng, Ganzhen] H;[Sun, Yao] C;[Kim, Jong Seung] K;Huazhong Agr Univ, Coll Anim Sci & Vet Med, State Key Lab Agr Microbiol, Wuhan 430070, Peoples R China.;Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
关键词：
Activable AIEgens;Aggregation-induced emission;Fluorescence Imaging;Small-molecule dye;Theranostics
摘要：
Reactive oxygen species (ROS), thiols and enzymes are regarded as important biomarkers in the physiological process. The abnormal levels of the above species are associated with many diseases, developing a fluorescence detection method for biomarkers is of great significance for diseases early diagnosis and therapy. Compared with traditional fluorescent dyes, aggregation-induced emission (ALE) based fluorescent emitters display excellent photostability with minimum aggregation caused quenching (ACQ) effect. Thus, the biomarker-activable AIEgens have attracted much attentions in biomedical research. In addition, many AIE emitters not only act as fluorescent dyes, but serve as promising theranostic agents. The AIE based image-guided multifunctional theranostics under the activation of biomarkers are vital to the precise biomedicine. This view focuses on the recent development of ROS, thiols, and enzymes activable AIEgens from single fluorescence imaging to multifunctional theranostics. (C) 2020 Elsevier B.V. All rights reserved.
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Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters
作者：
Li, Jie;Zhan, Guangming;Yang, Jianhua;Quan, Fengjiao;Mao, Chengliang;...
期刊：
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY ,2020年142(15):7036-7046 ISSN：0002-7863
通讯作者：
Zhang, Lizhi;Yu, Jimmy C.
作者机构：
[Xu, Liangpang; Lei, Fengcai; Chan, Alice W. M.; Li, Lejing; Liu, Yang; Yu, Jimmy C.; Li, Jie] Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China.;[Quan, Fengjiao; Zhang, Lizhi; Shi, Yanbiao; Mao, Chengliang; Zhan, Guangming] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Wang, Jianfang; Yang, Jianhua] Chinese Univ Hong Kong, Dept Phys, Shatin, Hong Kong, Peoples R China.;[Wong, Po Keung; Wang, Bo] Chinese Univ Hong Kong, Sch Life Sci, Shatin, Hong Kong, Peoples R China.;[Du, Yi; Dou, Shi-Xue] Univ Wollongong, AIIM, ISEM, Wollongong, NSW 2500, Australia.
通讯机构：
[Zhang, Lizhi; Yu, Jimmy C.] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Minist Educ,Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;Chinese Univ Hong Kong, Dept Chem, Shatin, Hong Kong, Peoples R China.
摘要：
The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N-2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol g(cat)(-1) h(-1)), a small partial current density (<1 mA cm(-2)), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 g(cat)(-1) h(-1)) than the Haber- Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm(-2) current densities for 100 h due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis.
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英文
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A drug-likeness toolbox facilitates ADMET study in drug discovery
作者：
Jia, Chen-Yang
* ;Li, Jing-Yi;Hao, Ge-Fei;Yang, Guang-Fu
（ 期刊：
Drug Discovery Today ,2020年25(1):248-258 ISSN：1359-6446
通讯作者：
Jia, Chen-Yang
作者机构：
[Yang, Guang-Fu; Li, Jing-Yi; Jia, Chen-Yang; Hao, Ge-Fei] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Yang, Guang-Fu; Hao, Ge-Fei] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Peoples R China.;[Hao, Ge-Fei] Guizhou Univ, State Key Lab Breeding Base Green Pesticide & Agr, Key Lab Green Pesticide & Agr Bioengn, Minist Educ,Res & Dev Ctr Fine Chem, Guiyang 550025, Peoples R China.;[Yang, Guang-Fu] Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300072, Peoples R China.
通讯机构：
[Jia, Chen-Yang] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.
摘要：
Undesirable pharmacokinetic (PK) properties or unacceptable toxicity are the main causes of the failure of drug candidates at the clinical trial stage. Since the concept of drug-likeness was first proposed, it has become an important consideration in the selection of compounds with desirable bioavailability during the early phases of drug discovery. Over the past decade, online resources have effectively facilitated drug-likeness studies in an economical and time-efficient manner. Here, we provide a comprehensive summary and comparison of current accessible online resources, in terms of their key features, application fields, and performance for in silico drug-likeness studies. We hope that the assembled toolbox will provide useful guidance to facilitate future in silico drug-likeness research.
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英文
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Cascade Reaction System Integrating Single-Atom Nanozymes with Abundant Cu Sites for Enhanced Biosensing
作者：
Wu, Yu;Wu, Jiabin;Jiao, Lei;Xu, Weiqing;Wang, Hengjia;...
期刊：
Analytical Chemistry ,2020年92(4):3373-3379 ISSN：0003-2700
通讯作者：
Huang, Liang;Zhu, Chengzhou
作者机构：
[Zhu, Chengzhou; Jiao, Lei; Gu, Wenling; Xu, Weiqing; Wu, Yu; Wei, Xiaoqian; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticides & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Huang, Liang; Wu, Jiabin] Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Peoples R China.;[Zhang, Nian; Ren, Guoxi] Chinese Acad Sci, SIMIT, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China.;[Zhang, Qinghua; Gu, Lin] Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China.;[Zhang, Qinghua; Gu, Lin] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China.
通讯机构：
[Huang, Liang] H;[Zhu, Chengzhou] C;Huazhong Univ Sci & Technol, Wuhan Natl Lab Optoelect, Wuhan 430074, Peoples R China.;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticides & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
摘要：
Single-atom nanozymes (SAzymes), as novel nanozymes with atomically dispersed active sites, are of great importance in the development of nanozymes for their high catalytic activities, the maximum utilization efficiency of metal atoms, and the simple model of active sites. Herein, the peroxidase-like SAzymes with high-concentration Cu sites on carbon nanosheets (Cu-N-C) were synthesized through a salt-template strategy. With the densely distributed active Cu atoms (â¼5.1 wt %), the Cu-N-C SAzymes exhibit remarkable activity to mimic natural peroxidase. Integrating Cu-N-C SAzymes with natural acetylcholinesterase and choline oxidase, three-enzyme-based cascade reaction system was constructed for the colorimetric detection of acetylcholine and organophosphorus pesticides. This work not only provides a strategy to synthesize SAzymes with abundant active sites but also gives some new insights for robust nanozyme biosensing systems. Copyright © 2020 American Chemical Society.
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英文
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Recent advances in the development of NIR-II organic emitters for biomedicine
作者：
Li, Jun;Liu, Yi;Xu, Yuling;Li, Lin* ;Sun, Yao* ;...
期刊：
Coordination Chemistry Reviews ,2020年415:213318 ISSN：0010-8545
通讯作者：
Sun, Yao;Li, Lin
作者机构：
[Li, Jun; Xu, Yuling; Sun, Yao] Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Li, Lin; Liu, Yi; Huang, Wei] Nanjing Tech Univ, Key Lab Flexible Elect, Nanjing 211816, Peoples R China.;[Li, Lin; Liu, Yi; Huang, Wei] Nanjing Tech Univ, IAM, Nanjing 211816, Peoples R China.;[Li, Jun] Huazhong Agr Univ, Coll Sci, Dept Chem, Wuhan 430070, Peoples R China.;[Huang, Wei] Northwestern Polytech Univ, SIFE, Xian 710072, Peoples R China.
通讯机构：
[Sun, Yao] C;[Li, Lin] N;Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;Nanjing Tech Univ, Key Lab Flexible Elect, Nanjing 211816, Peoples R China.;Nanjing Tech Univ, IAM, Nanjing 211816, Peoples R China.
关键词：
Fluorescence imaging;Multifunctionality;Near-infrared II;Organic emitters
摘要：
Fluorescence imaging with deep penetration and low auto-fluorescence in the second near-infrared biochannel (NIR-II, 1000–1700 nm) was developed rapidly during the past decades. Organic materials such as organic small molecules and polymers are promising candidates for various biomedical studies owing to their low toxicity and facile chemical modification. Recently, scaffold-structural diversity and multifunctional utilization of NIR-II fluorophores attracted a lot of attentions as the gradually revealing shortcomings of first generation NIR-I organic fluorophores and unbalanced demand between single fluorescence imaging and clinical practice. In this review, organic emitters including NIR-II organic small molecules and polymers are discussed which focus on their multifunctional applications in biomedicine. Furthermore, we raised the current challenges and perspectives of NIR-II organic emitters. © 2020 Elsevier B.V.
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英文
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Single-Atom Iron Boosts Electrochemiluminescence
作者：
Gu, Wenling;Wang, Hengjia;Jiao, Lei;Wu, Yu;Chen, Yuxin;...
期刊：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION ,2020年59(9):3534-3538 ISSN：1433-7851
通讯作者：
Zhu, Chengzhou;Hu, Liuyong
作者机构：
[Zhu, Chengzhou; Chen, Yuxin; Gong, Jingming; Wu, Yu; Jiao, Lei; Gu, Wenling; Wang, Hengjia] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Sch Mat Sci & Engn, Wuhan 430205, Peoples R China.;[Du, Dan] Washington State Univ, Sch Mech & Mat Engn, Pullman, WA 99164 USA.
通讯机构：
[Zhu, Chengzhou] C;[Hu, Liuyong] W;Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China.;Wuhan Inst Technol, Sch Mat Sci & Engn, Wuhan 430205, Peoples R China.
关键词：
antioxidant capacity;electrochemiluminescence;Fe-N-C catalysts;luminol;single-atom catalysts
摘要：
The traditional luminol–H2O2 electrochemiluminescence (ECL) sensing platform suffers from self-decomposition of H2O2 at room temperature, hampering its application for quantitative analysis. In this work, for the first time we employ iron single-atom catalysts (Fe-N-C SACs) as an advanced co-reactant accelerator to directly reduce the dissolved oxygen (O2) to reactive oxygen species (ROS). Owing to the unique electronic structure and catalytic activity of Fe-N-C SACs, large amounts of ROS are efficiently produced, which then react with the luminol anion radical and significantly amplify the luminol ECL emission. Under the optimum conditions, a Fe-N-C SACs–luminol ECL sensor for antioxidant capacity measurement was developed with a good linear range from 0.8 μm to 1.0 mm of Trolox. © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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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
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英文
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Formation and stabilization of colloidal ultra-small palladium nanoparticles on diamine-modified Cr-MIL-101: Synergic boost to hydrogen production from formic acid
作者：
Alamgholiloo, Hassan;Rostamnia, Sadegh* ;Hassankhani, Asadollah* ;Liu, Xiao* ;Eftekhari, Aziz;...
期刊：
Journal of Colloid and Interface Science ,2020年567:126-135 ISSN：0021-9797
通讯作者：
Rostamnia, Sadegh;Hassankhani, Asadollah;Liu, Xiao;Hasanzadeh, Amir;Shokouhimehr, Mohammadreza;Khaksar, Samad;Varma, Rajender S.
作者机构：
[Rostamnia, Sadegh; Alamgholiloo, Hassan] Univ Maragheh, Fac Sci, Dept Chem, Organ & Nano Grp ONG, POB 55181-83111, Maragheh, Iran.;[Hassankhani, Asadollah] Grad Univ Adv Technol, Inst Sci & High Technol & Environm Sci, Dept New Mat, Kerman, Iran.;[Liu, Xiao] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Eftekhari, Aziz; Hasanzadeh, Amir] Maragheh Univ Med Sci, POB 78151-55158, Maragheh, Iran.;[Zhang, Kaiqiang; Shokouhimehr, Mohammadreza] Seoul Natl Univ, Res Inst Adv Mat, Dept Mat Sci & Engn, Seoul 08826, South Korea.
通讯机构：
[Rostamnia, Sadegh; Khaksar, Samad] U;[Hassankhani, Asadollah] G;[Liu, Xiao] C;[Hasanzadeh, Amir] M;[Shokouhimehr, Mohammadreza] S
关键词：
Formic acid dehydrogenation;Metal-organic frameworks;Open metal site MOFs;[email protected]
摘要：
Ultra-small nano-sized palladium particles were successfully stabilized within the pores of diamine groups grafted open metal site metal-organic frameworks of Cr-MIL-101; coordinated diamine groups of ethylene diamine (ED) and propyl diamine (PD) on the active site of chromium units of Cr-MIL-101. The physiochemical properties of the [email protected] were investigated using FTIR, XRD, SEM/EDX mapping, TEM, BET, and AAS. The Cr-MIL-101 stabilized ultra-small Pd nanoparticles, [email protected](ethylene diamine)/Cr-MIL-101, and [email protected](propyl diamine)/Cr-MIL-101, displayed catalytic activity for clean dehydrogenation of formic acid and generation of hydrogen at room temperature. The resultant [email protected]/Cr-MIL-101 catalyst indicates high catalytic activity with turnover frequency (TOF) of 583 h−1 at 328 K, which is superior to most of the reported catalysts, including [email protected]/Cr-MIL-101 with TOF 532 h−1. Our studies open up a new method to the design of an ultra-small metal nanoparticle for the catalytic dehydrogenation of HCOOH. © 2020 Elsevier Inc.
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英文
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An overview of spirooxindole as a promising scaffold for novel drug discovery
作者：
Zhou, Li-Ming;Qu, Ren-Yu;Yang, Guang-Fu
* （ 期刊：
Expert Opinion on Drug Discovery ,2020年15(5):603-625 ISSN：1746-0441
通讯作者：
Yang, Guang-Fu
（ 作者机构：
[Yang, Guang-Fu; Qu, Ren-Yu; Zhou, Li-Ming] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan, Peoples R China.
通讯机构：
[Yang, Guang-Fu] C;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan, Peoples R China.
关键词：
Spirooxindole;natural products;bioactivity;anticancer;antimicrobial;structure-activity relationship
摘要：
Introduction: Spirooxindole, a unique and versatile scaffold, has been widely studied in some fields such as pharmaceutical chemistry and synthetic chemistry. Especially in the application of medicine, quite a few compounds featuring spirooxindole motif have displayed excellent and broad pharmacological activities. Many identified candidate molecules have been used in clinical trials, showing promising prospects. Areas covered: This article offers an overview of different applications and developments of spirooxindoles (including the related natural products and their derivatives) in the process of drug innovation, including such as in anticancer, antimicrobial, anti–inflammatory, analgesic, antioxidant, antimalarial, and antiviral activities. Furthermore, the crucial structure-activity relationships, molecular mechanisms, pharmacokinetic properties, and main synthetic methods of spirooxindoles-based derivatives are also reviewed. Expert opinion: Recent progress in the biological activity profiles of spirooxindole derivatives have demonstrated their significant position in present-day drug discovery. Furthermore, we believe that the multidirectional development of novel drugs containing this core scaffold will continue to be the research hotspot in medicinal chemistry in the future. © 2020, © 2020 Informa UK Limited, trading as Taylor & Francis Group.
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英文
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Electrochemically self-doped WO3/TiO2 nanotubes for photocatalytic degradation of volatile organic compounds
作者：
Wang, Xiaoguang;Sun, Minghui;Murugananthan, Muthu;Zhang, Yanrong* ;Zhang, Lizhi*
期刊：
Applied Catalysis B: Environmental ,2020年260:118205 ISSN：0926-3373
通讯作者：
Zhang, Yanrong;Zhang, Lizhi
作者机构：
[Wang, Xiaoguang; Sun, Minghui; Zhang, Yanrong] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China.;[Murugananthan, Muthu] PSG Coll Technol, Dept Chem, Coimbatore 641004, Tamil Nadu, India.;[Zhang, Lizhi] Cent China Normal Univ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Zhang, Yanrong] H;[Zhang, Lizhi] C;Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China.;Cent China Normal Univ, Inst Environm Chem, Wuhan 430079, Hubei, Peoples R China.
关键词：
Electrochemical self-doping;Oxygen vacancy;Photocatalysis;VOC degradation;WO3/TiO2 nanotubes
摘要：
In this study, an electrochemically self-doped WO3/TiO2 nanotubes (R-WO3/TNTs) composite film was developed for the photocatalytic degradation of waste gas. The doping of oxygen vacancies (OVs) into the heterojunction of WO3/TNTs was conducted by a simple electrochemical approach, by which the quantity and distribution of OVs on surface as well as bulk were tailored with respect to the applied cathodic potential and the duration of the treatment. With an increase of applied cathodic potential as well as the duration, the quantity of OVs on WO3/TNTs was observed to be consistently raised, while those presented in the surface were raised initially and further showed a plateau trend as the duration extended at a fixed potential. The incorporation of OVs into WO3/TNTs enhanced the charge-transport resistance and reduced the electron-hole recombination, thereby showed an enhanced photocatalytic performance. The R-WO3/TNTs prepared by the electrochemical polarization process at −1.4 V (vs SCE) exhibited a 12 times higher photo-current density and obviously, an enhanced efficiency in the photocatalytic degradation of VOCs with a prolonging photostability compared to that of the pristine WO3/TNTs, under a simulated solar light irradiation. The single-time purification trial demonstrated the effectiveness of the R-WO3/TNTs composite in treating the VOCs for the practical application. © 2019 Elsevier B.V.
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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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Visible light-promoted ring-opening functionalization of three-membered carbo- And heterocycles
作者：
Xuan, Jun* ;He, Xiang-Kui;Xiao, Wen-Jing*
期刊：
CHEMICAL SOCIETY REVIEWS ,2020年49(9):2546-2556 ISSN：0306-0012
通讯作者：
Xuan, Jun;Xiao, Wen-Jing
作者机构：
[Xuan, Jun; He, Xiang-Kui] Anhui Univ, Anhui Prov Key Lab Chem Inorgan Organ Hybrid Func, Coll Chem & Chem Engn, Hefei 230601, Anhui, Peoples R China.;[Xuan, Jun] Anhui Univ, Key Lab Struct & Funct Regulat Hybrid Mat, Minist Educ, Hefei 230601, Peoples R China.;[Xiao, Wen-Jing] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Xuan, Jun] A;[Xiao, Wen-Jing] C;Anhui Univ, Anhui Prov Key Lab Chem Inorgan Organ Hybrid Func, Coll Chem & Chem Engn, Hefei 230601, Anhui, Peoples R China.;Anhui Univ, Key Lab Struct & Funct Regulat Hybrid Mat, Minist Educ, Hefei 230601, Peoples R China.;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.
摘要：
Due to their inherent ring strain, three-membered carbocyclic- and heterocyclic ring structures are versatile synthetic building blocks. Traditional ring-opening methods of these molecules require the use of thermolysis, acid catalysts or transition-metals via ionic reaction pathways. Recently, visible light-induced photoredox catalysis has emerged as a powerful platform for initiating new chemical transformations. In this tutorial review, the synthetic and mechanistic aspects of visible light-promoted ring-opening functionalization of three-membered carbo- and heterocycles are highlighted. By using these strategies, a variety of ring-opening functionalization products, including biologically important carbo- and heterocycles, can be efficiently accessed in a high chemo- and regioselective manner. © 2020 The Royal Society of Chemistry.
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Robust and Stable Acidic Overall Water Splitting on Ir Single Atoms
作者：
Luo, Fang;Hu, Hao;Zhao, Xiao;Yang, Zehui* ;Zhang, Quan;...
期刊：
NANO LETTERS ,2020年20(3):2120-2128 ISSN：1530-6984
通讯作者：
Yang, Zehui;Cai, Weiwei;Xu, Jingxiang;Zhu, Chengzhou
作者机构：
[Yang, Zehui; Cai, Weiwei; Hu, Hao; Luo, Fang; Zhang, Quan] China Univ Geosci, Fac Mat Sci & Chem, Sustainable Energy Lab, Wuhan 430074, Peoples R China.;[Xu, Jingxiang] Shanghai Ocean Univ, Coll Engn Sci & Technol, Shanghai 201306, Peoples R China.;[Zhu, Chengzhou] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.;[Yoshida, Yusuke; Zhao, Xiao; Kaneko, Takuma] Univ Electrocommun, Innovat Res Ctr Fuel Cells, Chofu, Tokyo 1828585, Japan.
通讯机构：
[Yang, ZH; Cai, WW; Zhu, Chengzhou] C;[Xu, Jingxiang] S;China Univ Geosci, Fac Mat Sci & Chem, Sustainable Energy Lab, Wuhan 430074, Peoples R China.;Shanghai Ocean Univ, Coll Engn Sci & Technol, Shanghai 201306, Peoples R China.;Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.
关键词：
Acidic water splitting;Iridium single atom;Oxygen evolution reaction;Hydrogen evolution reaction
摘要：
Single-atom electrocatalysts (SAEs) can realize the target of low-cost by maximum atomic efficiency. However, they usually suffer performance decay due to high energy states, especially in a harsh acidic water splitting environment. Here, we conceive and realize a double protecting strategy that ensures robust acidic water splitting on Ir SAEs by dispersing Ir atoms in/onto Fe nanoparticles and embedding IrFe nanoparticles into nitrogen-doped carbon nanotubes ([email protected]@NCNT). When [email protected]@NCNT acts as a bifunctional electrocatalyst at ultralow Ir loading of 1.14 μg cm-2, the required overpotentials to deliver 10 mA cm-2 are 250 and 26 mV for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in 0.5 M H2SO4 electrolyte corresponding to 1370- and 61-fold better mass activities than benchmark IrO2 and Pt/C at an overpotential of 270 mV, respectively, resulting in only 1.51 V to drive overall water splitting. Moreover, remarkable stability is also observed compared to Pt/C-IrO2. © 2020 American Chemical Society.
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Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions
作者：
Li, Jie;Chen, Shang;Quan, Fengjiao;Zhan, Guangming;Jia, Falong;...
期刊：
Chem ,2020年6(4):885-901 ISSN：2451-9294
通讯作者：
Zhang, Lizhi
作者机构：
[Quan, Fengjiao; Zhang, Lizhi; Chen, Shang; Li, Jie; Zhan, Guangming; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构：
[Zhang, Lizhi] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
关键词：
electric field;electrocatalytic ammonia synthesis;interfacial polarization;SDG7: Affordable and clean energy;single atom catalysis
摘要：
Electrocatalytic N2 reduction reaction (NRR) offers a promising low-energy, sustainable ammonia-synthesizing alternative to Haber-Bosch reaction. One roadblock lying in access to high-performance ammonia electrosynthesis emanates from the unsatisfied ability of electrocatalysts to wreck N≡N bond. Here, we report that interfacial polarization is an efficient scenario to enhance N≡N fracture to boost electrocatalytic ammonia synthesis. As a proof-of-concept demonstration, protrusion-shaped Fe single-atom catalysts immobilized onto MoS2 nanosheets engender electric fields to polarize N2. The resultant interfacial polarization fields between Fe-MoS2 and N2 drive the injection of more electrons into N2 antibonding orbitals in a fast manner, leading to a superior ammonia-evolving rate (36.1 ± 3.6 mmol g−1 h−1 or 97.5 ± 6 μg h−1 cm−2) at low applied potential. Similar phenomena are applicable in Co-MoS2, Cu-MoS2, Rh-MoS2, or Ru-MoS2, suggesting the potential universality of our interfacial polarization concept in upgrading wide-scope catalysis. Seeking a green, low-cost, sustainable approach to synthesize ammonia is crucial to society development and human living. A promising candidate is electrocatalytic nitrogen reduction. The insufficient ability of electrocatalysts to split the N≡N bond, however, limits the activity and selectivity. Using interfacial polarization as a conceptually novel strategy to promote N≡N disintegration, high-rate ammonia electrosynthesis up to 36.1 ± 3.6 mmol g−1 h−1 (97.5 ± 6 μg h−1 cm−2) is realized at a low applied potential (−0.2 V versus RHE). This work paves a new way toward replacing Haber-Bosch reaction with ambient ammonia electrosynthesis. Interfacial polarization is reported as a brand new, efficient, and generalizable strategy to accelerate electrocatalytic reduction of N2 to ammonia. The polarization is established by using an electric field to polarize N2. The electric field is triggered by protrusion-like single atoms anchored on MoS2. The interfacial polarization accelerates electron transfer from single atoms to N2 and thus promotes N2 reduction. As a result, ammonia synthesis in an electrochemical flow cell proceeds at a high rate of 36.1 ± 3.6 mmol g−1 h−1. © 2020 Elsevier Inc.
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英文
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CRISPR/Cas Systems towards Next-Generation Biosensing
作者：
Li, Yi;Li, Shiyuan;Wang, Jin* ;Liu, Guozhen*
期刊：
Trends in Biotechnology ,2019年37(7):730-743 ISSN：0167-7799
通讯作者：
Liu, Guozhen;Wang, Jin
作者机构：
[Liu, Guozhen; Li, Yi] Univ New South Wales, Fac Engn, ARC Ctr Excellence Nanoscale Biophoton, Grad Sch Biomed Engn, Sydney, NSW 2052, Australia.;[Liu, Guozhen; Li, Yi] Univ New South Wales, Australian Ctr NanoMed, Sydney, NSW 2052, Australia.;[Li, Shiyuan] Shanghai Tolo Biotechnol Co Ltd, Shanghai 200233, Peoples R China.;[Wang, Jin] Shanghai Normal Univ, Coll Life & Environm Sci, Shanghai 200234, Peoples R China.;[Liu, Guozhen] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Hubei, Peoples R China.
通讯机构：
[Liu, Guozhen] U;[Wang, Jin] S;[Liu, Guozhen] C;Univ New South Wales, Fac Engn, ARC Ctr Excellence Nanoscale Biophoton, Grad Sch Biomed Engn, Sydney, NSW 2052, Australia.;Univ New South Wales, Australian Ctr NanoMed, Sydney, NSW 2052, Australia.
关键词：
CRISPR/Cas;Cas12;Cas13;Cas9;biosensing;diagnostics;nucleic acid detection
摘要：
Beyond its remarkable genome editing ability, the CRISPR/Cas9 effector has also been utilized in biosensing applications. The recent discovery of the collateral RNA cleavage activity of the Cas13a effector has sparked even greater interest in developing novel biosensing technologies for nucleic acid detection and promised significant advances in CRISPR diagnostics. Now, along with the discovery of Cas12 collateral cleavage activities on single-stranded DNA (ssDNA), several CRISPR/Cas systems have been established for detecting various targets, including bacteria, viruses, cancer mutations, and others. Based on key Cas effectors, we provide a detailed classification of CRISPR/Cas biosensing systems and propose their future utility. As the field continues to mature, CRISPR/Cas systems have the potential to become promising candidates for next-generation diagnostic biosensing platforms.
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英文
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Fe-N-C Single-Atom Nanozymes for the Intracellular Hydrogen Peroxide Detection
作者：
Jiao, Lei;Xu, Weiqing;Yan, Hongye;Wu, Yu;Liu, Chunrong;...
期刊：
Analytical Chemistry ,2019年91(18):11994-11999 ISSN：0003-2700
通讯作者：
Zhu, Chengzhou
作者机构：
[Xu, Weiqing; Zhu, Chengzhou; Yan, Hongye; Wu, Yu; Liu, Chunrong; Jiao, Lei] Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, 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;Cent China Normal Univ, Coll Chem, Int Joint Res Ctr Intelligent Biosensing Technol, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.
摘要：
Recently, in situ detection of hydrogen peroxide (H2O2) generated from live cells have caused tremendous attention, because it is of great significance in the control of multiple biological processes. Herein, Fe-N-C single-atom nanozymes (Fe-N-C SAzymes) with intrinsic peroxidase-like activity were successfully prepared via high-temperature calcination using FeCl2, glucose, and dicyandiamide as precursors. The Fe-N-C SAzymes with FeNx as active sites were similar to natural metalloproteases, which can specifically enhance the peroxidase-like activity rather than oxidase-like activity. Accordingly, owing to the excellent catalytic efficiency of the Fe-N-C SAzymes, colorimetric biosensing of H2O2 in vitro was performed via a typical 3,3′,5,5′-tetramethylbenzidine induced an allochroic reaction, demonstrating the satisfactory specificity and sensitivity. With regard to the practical application, in situ detection of H2O2 generated from the Hela cells by the Fe-N-C SAzymes was also performed, which can expand the applications of the newborn SAzymes. Copyright © 2019 American Chemical Society.
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英文
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Single Fe Atom on Hierarchically Porous S, N-Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn-Air Batteries
作者：
Zhang, Jiting;Zhang, Meng;Zeng, Yon;Chen, Jisheng;Qiu, Lingxi;...
期刊：
Small ,2019年15(24):1900307- ISSN：1613-6810
通讯作者：
Zhu, Zhihong;Zhu, Chengzhou
作者机构：
[Qiu, Lingxi; Zhang, Jiting; Zhu, Zhihong; Yu, Ying; Zhang, Meng; Chen, Jisheng] Cent China Normal Univ, Coll Phys Sci & Technol, Inst Nanosci & Nanotechnol, Wuhan 430079, Hubei, Peoples R China.;[Zhu, Chengzhou; Zeng, Yon] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Int Joint Res Ctr Intelligent Biosens, Wuhan 430079, Hubei, Peoples R China.;[Zhou, Hua; Sun, Chengjun] Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA.
通讯机构：
[Zhu, Zhihong; Zhu, Chengzhou] C;Cent China Normal Univ, Coll Phys Sci & Technol, Inst Nanosci & Nanotechnol, Wuhan 430079, Hubei, Peoples R China.;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Int Joint Res Ctr Intelligent Biosens, Wuhan 430079, Hubei, Peoples R China.
关键词：
bifunctional catalysts;biomass;heteroatom doping;rechargeable Zn-air batteries;single-atom electrocatalysts
摘要：
Iron–nitrogen–carbon materials (Fe–N–C) are known for their excellent oxygen reduction reaction (ORR) performance. Unfortunately, they generally show a laggard oxygen evolution reaction (OER) activity, which results in a lethargic charging performance in rechargeable Zn–air batteries. Here porous S-doped Fe–N–C nanosheets are innovatively synthesized utilizing a scalable FeCl3-encapsulated-porphyra precursor pyrolysis strategy. The obtained electrocatalyst exhibits ultrahigh ORR activity (E1/2 = 0.84 V vs reversible hydrogen electrode) and impressive OER performance (Ej= 10 = 1.64 V). The potential gap (ΔE = Ej= 10 − E1/2) is 0.80 V, outperforming that of most highly active bifunctional electrocatalysts reported to date. Furthermore, the key role of S involved in the atomically dispersed Fe–Nx species on the enhanced ORR and OER activities is expounded for the first time by ultrasound-assisted extraction of the exclusive S source (taurine) from porphyra. Moreover, the assembled rechargeable Zn–air battery comprising this bifunctional electrocatalyst exhibits higher power density (225.1 mW cm−2) and lower charging–discharging overpotential (1.00 V, 100 mA cm−2 compared to Pt/C + RuO2 catalyst). The design strategy can expand the utilization of earth-abundant biomaterial-derived catalysts, and the mechanism investigations of S doping on the structure–activity relationship can inspire the progress of other functional electrocatalysts. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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