作者： Qin, Xiaolei;Mukerabigwi, Jean Felix;Ma, Mingzi;Huang, Ruyi;Ma, Mengdi;...

期刊： e-Polymers,2021年21(1):606-615 ISSN：1618-7229

通讯作者： Cao, Yu(caoyu@mail.ccnu.edu.cn);Yu, Yang(yuyangpla301@163.com)

作者机构： [Qin, Xiaolei; Ma, Mengdi; Mukerabigwi, Jean Felix; Huang, Ruyi; Cao, Yu; Huang, Xueying] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Yu, Yang; Ma, Mingzi] Med Sch Chinese PLA, Beijing 100853, Peoples R China.;[Yu, Yang; Ma, Mingzi] Chinese Peoples Liberat Army Gen Hosp, Med Ctr 1, Dept Blood Transfus, Beijing 100853, Peoples R China.;[Mukerabigwi, Jean Felix] Univ Rwanda, Coll Sci & Technol, Dept Chem, POB 3900, Kigali, Rwanda.

通讯机构： [Yu Cao] K;[Yang Yu] M;Medical School of Chinese PLA, Beijing 100853, China<&wdkj&>Department of Blood Transfusion, The First Medical Center, Chinese PLA General Hospital, Beijing 100853, China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology (Ministry of Education), College of Chemistry, Central China Normal University, Wuhan 430079, China

关键词： chitosan;blend hydrogel;antibacterial;rapid hemostatic;wound dressing

摘要： Uncontrollable bleeding is still the main cause of post-traumatic deaths due to the blood loss. Moreover, infectious complication of wound is also still a challenging problem for wound healing. Nevertheless, the currently available hemostasis drugs or materials cannot stanch bleeding well due to single function, slow in effectiveness, adhere to wounds easily, poor gas permeability, etc. Therefore, it is of a great significance to utilize a biomedical hemostatic material that can stop bleeding quickly, preventing from bacterial infections, and with good biocompatibility properties. Herein chitosan (CS) was modified with gallic acid (GA) and thrombin (TB) to prepare an antibacterial hemostatic composite dressing. The CS-based composite hydrogel dressing was obtained by acylation modification, ultraviolet curing crosslinking method and physical mixing. The in vitro results showed that our prepared CS-based composite hydrogel has obvious burst release and good degradation property. Moreover, the in vivo results showed that it has a strong antibacterial property that is much better than single CS, and it can stop bleeding in 1 min which can promote wound healing. Therefore, the findings of this study is expected to contribute to the future designing of biomedical hemostatic materials with improved properties. © 2021 Xiaolei Qin et al., published by De Gruyter 2021.

语种： 英文

作者： Gong, Shengyi;Zheng, Zhoupeng;Guan, Xiaogang;Feng, Shumin;Feng, Guoqiang

期刊： Analytical Chemistry,2021年93(14):5700-5708 ISSN：0003-2700

通讯作者： Feng, Guoqiang(gf256@mail.ccnu.edu.cn)

作者机构： [Zheng, Zhoupeng; Feng, Guoqiang; Gong, Shengyi; Feng, Shumin; Guan, Xiaogang] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Guoqiang Feng] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan 430079, P. R. China

摘要： To elucidate the complex role of biological H2S and study the mitochondrial damage and some related diseases, effective methods for visualization of H2S in mitochondria and in vivo are urgently needed. In this contribution, a novel near-infrared mitochondria-targetable fluorescence probe MI-H2S for H2S detection was developed. MI-H2S shows rapid detection ability for H2S in pure aqueous solution and outputs a highly selective and sensitive fluorescence-on signal at 663 nm with a large Stokes shift of 141 nm. Bioimaging experiments revealed that the probe has good mitochondrial-targeting ability and high-contrast imaging ability for detecting H2S in living systems. The probe also showed great potential in the detection of H2S during inflammation. All of the results demonstrate that MI-H2S can be applied as an effective probe for the visualization and study of H2S in mitochondria and in vivo. ©

语种： 英文

作者： Chen, Zhen;Liu, Qian;Guo, Lei;Zhang, Shoute;Pang, Lei;...

期刊： Applied Catalysis B: Environmental,2021年286:119816 ISSN：0926-3373

通讯作者： Li, Tao

作者机构： [Li, Tao; Chen, Zhen; Liu, Qian; Guo, Lei; Zhang, Shoute] Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Minist Educ, Hubei Key Lab Mat Chem & Serv Failure,Sch Chem &, Wuhan 430074, Peoples R China.;[Pang, Lei] DongFeng Trucks R&D Ctr, Zhushanhu Rd 653, Wuhan 430056, Peoples R China.;[Guo, Yanbing] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.

通讯机构： [Li, Tao] H;Huazhong Univ Sci & Technol, Key Lab Mat Chem Energy Convers & Storage, Minist Educ, Hubei Key Lab Mat Chem & Serv Failure,Sch Chem &, Wuhan 430074, Peoples R China.

关键词： Diesel exhausts purification;Fe-SSZ-13;NH3-SCR;One-pot method;Zr doping

摘要： Fe-SSZ-13 has been proven to be a highly efficient catalyst for the ammonia selective catalytic reduction (NH3-SCR) of NOx, especially at medium and high reaction temperatures. Nevertheless, the hydrothermal stability of Fe-SSZ-13 catalyst is inferior, limiting its application in vehicle exhaust purification. Impressively, it is found that the hydrothermal stability of Fe-SSZ-13 can be remarkably enhanced (as high as 30 % improvement at 300 °C) by in situ introduction of Zr and Fe into initial gels via one-pot synthesis in this work. A small amount of Zr addition (0.31 wt.%) is beneficial for improving the relative crystallinity of Fe-SSZ-13. The characterization results (obtained by 27Al NMR, NH3-TPD, UV–vis, XPS and in situ DRIFTS) revealed that Zr doping by a one-pot method would not only enhance the dispersion of active isolated Fe ions but also inhibit the migration and agglomeration of isolated Fe ions during hydrothermal aging, improving the stability of the catalyst. Additionally, the introduction of Zr generates new hydroxy groups and Lewis acid sites, facilitating the formation of reaction intermediates, such as -NH2, -HNO2, -NO2, etc., and promoting the SCR reaction especially over the aged catalyst. © 2020

语种： 英文

作者： Li, Jinli;Wu, Yu;Qin, Ying;Liu, Mingwang;Chen, Guojuan;...

期刊： Chemical Communications,2021年57(100):13788-13791 ISSN：1359-7345

通讯作者： Gu, Wenling;Zhu, Chengzhou;Hu, Liuyong

作者机构： [Chen, Guojuan; Qin, Ying; Zhu, Chengzhou; Liu, Mingwang; Gu, Wenling; Zhu, CZ; Wu, Yu; Li, Jinli] 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.;[Li, Jinli] Jingchu Univ Technol, Sch Elect & Informat Engn, Jingmen 448000, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Sch Mat Sci & Engn, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chemist 1y & Adv Mat, Wuhan 430205, Peoples R China.

通讯机构： [Gu, WL; Zhu, CZ] C;[Hu, Liuyong] W;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.;Wuhan Inst Technol, Sch Mat Sci & Engn, Hubei Engn Technol Res Ctr Optoelect & New Energy, Hubei Key Lab Plasma Chemist 1y & Adv Mat, Wuhan 430205, Peoples R China.

摘要： Photoelectrochemical (PEC) enzymatic biosensors integrate the excellent selectivity of enzymes and high sensitivity of PEC bioanalysis, but the drawbacks such as high cost, poor stability, and tedious immobilization of natural enzymes on photoelectrodes severely suppress their applications. AgCu@CuO aerogel-based photoelectrode materials with both remarkable enzyme-like activities and outstanding photoelectric properties were innovatively designed and synthesized to evaluate the activity of xanthine oxidase with a wide linear detection range and a low limit of detection.

语种： 英文

作者： Xu, Weiwei;Cheng, Ming;Zhang, Siyun;Wu, Qifa;Liu, Zhuo;...

期刊： Chemical Communications,2021年57(61):7480-7492 ISSN：1359-7345

通讯作者： Liang, Feng(feng_liang@whu.edu.cn)

作者机构： [Cheng, Ming; Xu, Weiwei; Li, Haibing; Dhinakaran, Manivannan Kalavathi; Zhang, Siyun] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol CCNU, Wuhan 430079, Peoples R China.;[Liang, Feng; Wu, Qifa; Liu, Zhuo] Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Coal Convers & New Carbon Mat Hubei Key Lab, State Key Lab Refractories & Met, Wuhan 430081, Peoples R China.;[Kovaleva, Elena G.] Ural Fed Univ, Dept Technol Organ Synth, Mira St 28, Ekaterinburg 620002, Russia.

通讯机构： [Feng Liang] T;[Elena G. Kovaleva] D;[Haibing Li] K;The State Key Laboratory of Refractories and Metallurgy, Coal Conversion and New Carbon Materials Hubei Key Laboratory, School of Chemistry & Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China<&wdkj&>Department of Technology for Organic Synthesis, Ural Federal University, Mira Street, 28, 620002 Yekaterinburg, Russia<&wdkj&>Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, P. R. China

摘要： Chiral discrimination has gained much focus in supramolecular chemistry, since it is one of the fundamental processes in biological systems, enantiomeric separation and biochemical sensors. Though most of the biochemical processes can routinely recognize biological enantiomers, enantioselective identification of chiral molecules in artificial systems is currently one of the challenging topics in the field of chiral discrimination. Inaccuracy, low separation efficiency and expensive instrumentation were considered typical problems in artificial systems. Recently, chiral recognition on the interfaces has been widely used in the fields of electrochemical detection and biochemical sensing. For the moment, a series of macrocyclic host functionalized interfaces have been developed for use as chiral catalysts or for enantiomeric separation. Here, we have briefly exposited the most recent advances in the fabrication of supramolecular functionalized interfaces and their application for chiral recognition.

语种： 英文

作者： Wu, Nannan;Jiao, Lei;Song, Shaojia;Wei, Xiaoqian;Cai, Xiaoli;...

期刊： Analytical Chemistry,2021年93(48):15982-15989 ISSN：0003-2700

通讯作者： Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn)

作者机构： [Wu, Nannan; Jiao, Lei; Wei, Xiaoqian; Cai, Xiaoli; Huang, Jiajia; Sha, Meng; Gu, Wenling; Zhu, Chengzhou] Key Laboratory of Pesticides 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, China;[Song, Shaojia; Song, Weiyu] State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing;102249, China;[Wu, Nannan; Jiao, Lei; Wei, Xiaoqian; Cai, Xiaoli; Huang, Jiajia; Sha, Meng; Gu, Wenling; Zhu, Chengzhou] 430079, China

通讯机构： [Chengzhou Zhu] K;Key Laboratory of Pesticides 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

摘要： Rational design and construction of advanced sensing platforms for sensitive detection of H2O2released from living cells is one of the challenges in the field of physiology and pathology. Noble metal clusters are a kind of nanomaterials with well-defined chemical composition and special atomic structures, which have been widely explored in catalysis, biosensing, and therapy. Compared with noble metal nanoparticles, noble metal clusters exhibit great potential in electrochemical biosensing due to their high atom utilization efficiency and abundant reactive active sites. Herein, Pt nanoclusters anchored on hollow carbon spheres (PtNCS/HCS) were successfully prepared for sensitive detection of H2O2. By tuning the ratio of Pt(0)/Pt(II) at different annealing temperatures, the optimized PtNCS/HCS-550 showed higher H2O2reduction and oxidation catalytic activities than other control samples. Density functional theory calculations revealed that H2O2*can be better activated and dissociated in the Pt0IImodel featured with the co-existence of Pt(0)/Pt(II) and the key intermediates OOH*/OH* have a stronger interaction with the Pt0IImodel. As a concept application, the electrochemical biosensing platform was successfully applied to sensitive detection of H2O2released from the cells. © 2021 American Chemical Society

语种： 英文

作者： Tang, Yuchen;Chen, Xuqi;Zhang, Shaohua;Smith, Zachary J.;Gao, Tingjuan

期刊： Analytical Chemistry,2021年93(47):15659-15666 ISSN：0003-2700

通讯作者： Tang, Yuchen(ytang@mail.ccnu.edu.cn);Gao, Tingjuan(tingao@mail.ccnu.edu.cn)

作者机构： [Tang, Yuchen; Chen, Xuqi; Zhang, Shaohua; Gao, Tingjuan] Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan;430079, China;[Smith, Zachary J.] Department of Precision Machinery and Precision Instrumentation, University of Science and Technology of China, Anhui, Hefei;230027, China;[Tang, Yuchen; Chen, Xuqi; Zhang, Shaohua; Gao, Tingjuan] 430079, China

通讯机构： [Yuchen Tang; Tingjuan Gao] K;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China

摘要： Due to the fundamental mechanism of vibrational state transitions for chemical bonds, the spectra of Raman scattering are narrow-banded and photostable signals capable of probing specific reactions. In the case of protonation/deprotonation reactions, certain chemical bonds are broken and new bonds are formed. Based on the changes of the vibrational modes for the corresponding bonds, fingerprint analysis of multiple Raman bands may allow for the in situ visualization of proton distribution in live cells. However, Raman scattering faces the well-known challenge of low sensitivity. To perform the vibrational fingerprint analysis of Raman scattering by overcoming this challenge, we developed an azo-based resonance Raman pH probe. It was an azobenzene-featured small molecule responsive to protons with the inherent Raman signal ∼104-fold more intense than that of the conventional alkyne-type Raman reporter 5-ethynyl-2′-deoxyuridine. Through the substitution of the electron-donating and -withdrawing entities to the azobenzene group, the effect of resonance Raman scattering and fluorescence quenching was obtained. This effect resulted in a significant Raman enhancement factor of ∼103 compared to the counterpart molecules without the molecular design. Based on the enhanced Raman sensitivity of the azo-based resonance Raman pH probe, the identification of vibrational fingerprint changes at the azo group was achieved during the protonation/deprotonation reactions, and the vibrational fingerprint analysis resolved a pH difference of less than 0.2 unit. The method enabled sensitive hyperspectral cell imaging that clearly visualized the change of proton distribution in autophagic cells. © 2021 American Chemical Society.

语种： 英文

作者： Wang, Yingqian;Zhang, Siyun;Yan, Hewei;Quan, Jiaxin;Yang, Lei;...

期刊： Analytical Chemistry,2021年93(15):6145-6150 ISSN：0003-2700

通讯作者： Li, Haibing(lhbing@mail.ccnu.edu.cn)

作者机构： [Wang, Yingqian; Yang, Lei; Li, Haibing; Zhang, Siyun; Quan, Jiaxin; Yan, Hewei; Chen, Xue] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Trautmann, Christina; Toimil-Molares, Maria Eugenia] GSI Helmholtzzentrum Schwerionenforsch, D-64291 Darmstadt, Germany.;[Trautmann, Christina] Tech Univ Darmstadt, D-64287 Darmstadt, Germany.

通讯机构： [Haibing Li] K;Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China

摘要： Enantiomers of various drug molecules have a specific effect on living organisms. Accordingly, developing a sample method for the efficient and rapid recognition of chiral drug enantiomers is of great industrial value and physiological significance. Here, inspired by the structure of ion channels in living organisms, we developed a chiral nanosensor based on an artificial tip-modified nanochannel system that allows efficient selective recognition of chiral drugs. In this system, l-alanine-pillar[5]arenes as selective receptors were introduced on the tip side of conical nanochannels to form an enantioselective 'gate'. The selective coefficient of our system toward R-propranolol is 4.96, which is higher than the traditional fully modified nanochannels in this work. © 2021 American Chemical Society.

语种： 英文

作者： Zhang, Yi*;Zhang, Xiangqian*;Yang, Huocheng;Yu, Le*;Xu, Yunjie;...

期刊： CHEMICAL SOCIETY REVIEWS,2021年50(20):11227-11248 ISSN：0306-0012

通讯作者： Zhang, Yi;Zhang, Xiangqian;Yu, Le

作者机构： [Zhang, Yi; Sun, Yao; Yang, Huocheng] Cent China Normal Univ, Key Lab Pesticides & Chem Biol, Minist Educ, Coll Chem, Wuhan 430079, Peoples R China.;[Zhang, Xiangqian; Li, Xiangyang] Guizhou Univ, State Key Lab Breeding Base Green Pesticide & Agr, Minist Educ, Guiyang 550025, Peoples R China.;[Zhang, Xiangqian] Huazhong Agr Univ, State Key Lab Agr Microbiol, Coll Anim Sci & Vet Med, Wuhan 430070, Peoples R China.;[Xu, Yunjie; Kim, Jong Seung; Yu, Le] Korea Univ, Dept Chem, Seoul 02841, South Korea.;[Sharma, Amit] CSIR Cent Sci Instruments Org, Sect 30C, Chandigarh, India.

通讯机构： [Yu, Le] D;[Zhang, Xiangqian] S;[Zhang, Yi] K;Department of Chemistry, Korea University, Seoul 02841, Korea<&wdkj&>Key Laboratory of Pesticides and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Guizhou University, Guiyang 550025, China

摘要： Despite significant advances, the therapeutic impact of photodynamic therapy is still substantially hampered by the restricted penetration depth of light and the reactive oxygen species (ROS)-mediated toxicity, which is impeded by the shorter effective half-life and radius of ROS produced during treatment. Sonodynamic therapy (SDT), on the other hand, provides unrivalled benefits in deep-seated tumour ablation due to its deep penetration depth and not totally ROS-dependent toxicity, exhibiting enormous preclinical and clinical potential. In this tutorial review, we highlight imaging-guided precise SDT, which allows choosing the best treatment option and monitoring the therapy response in real-Time, as well as recent clinical trials based on SDT. Aside from that, the subtle design strategies of sonosensitizers based on tumour environment shaping and rational structure modification, as well as SDT combination treatment (chemotherapy, chemodynamic therapy, photodynamic therapy, photothermal therapy, gas therapy and immunotherapy), aimed at a more effective treatment outcome, are summarized. Finally, we discussed the future of SDT for personalized cancer and other disease treatments. This journal is © The Royal Society of Chemistry.

语种： 英文

作者： Wang, Xiaobing;Chen, Na;Liu, Xiufan;Shi, Yanbiao;Ling, Cancan;...

期刊： Applied Catalysis B: Environmental,2021年282:119558 ISSN：0926-3373

通讯作者： Zhang, Lizhi

作者机构： [Ling, Cancan; Zhang, Lizhi; Liu, Xiufan; Shi, Yanbiao; Wang, Xiaobing; Chen, Na] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Zhang, Lizhi] C;Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.

关键词： Ascorbate;Goethite;H2O2 conversion;Heterogeneous fenton reaction;Quantitative determination

摘要： In this study, we demonstrate that the addition of ascorbate can lower the conversion percentage of H2O2 to O2 from 71% to 11%, and thus increase the conversion percentage of H2O2 to [rad]OH from 11% to 82% on goethite within 3 h. This greatly enhanced production of [rad]OH could be attributed to the efficient Fe(III)/Fe(II) redox cycle accelerated by ascorbate, which produced abundant Fe(II) confined on the goethite surface, favoring the conversion of H2O2 to [rad]OH. Meanwhile, the decreased surface Fe(III) of goethite strongly inhibited the conversion of H2O2 to O2. These findings can clarify the quantitative influence of ascorbate on the H2O2 decomposition process over the iron mineral surface, and thus deepen the understanding of heterogeneous Fenton reaction mechanism during organic containment treatment. © 2020 Elsevier B.V.

语种： 英文

作者： Ling, Cancan;Liu, Xiufan;Li, Meiqi;Wang, Xiaobing;Shi, Yanbiao;...

期刊： Applied Catalysis B: Environmental,2021年290:120051 ISSN：0926-3373

通讯作者： Zhang, Lizhi(zhanglz@mail.ccnu.edu.cn)

作者机构： [Ling, Cancan; Zhang, Lizhi; Liu, Xiufan; Shi, Yanbiao; Zhao, Jincai; Wang, Xiaobing; Qi, Jing; Li, Meiqi] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Zhang, L.] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, China

关键词： Anaerobic;Hydroxyl radical;Localized electron;Pyrite-water interface;Sulfur vacancies

摘要： We demonstrate that FeS2 possessing sulfur vacancies (SVs), under anaerobic water environment, can stabilize the H2O adsorption with a strong exothermic effect to compensate the apparent energy barrier of H2O oxidation on pyrite surface. Adsorbed H2O dissociates at SV site via π-back donation of localized electron, and thus breaks through thermodynamic restriction of H2O oxidation to generate bound hydroxyl radical through a one-electron transfer process of localized holes (Vs+). Meanwhile, the synergistic effect of surface Fe3+ and circumjacent H2O molecule can also promote the oxidation of H2O adsorbed at Fe3+ site to produce free hydroxyl radical via oxidation reaction. The generated hydroxyl radical on pyrite surface can induce the oxidation of different pollutants, and also contribute to the pyrite self-oxidation process. These findings clarify the in-depth mechanism of anaerobic hydroxyl radical generation at pyrite-water interface, and shed light on anaerobic environmental effect of pyrite and other natural iron sulfide minerals. © 2021 Elsevier B.V.

语种： 英文

作者： Xu, Tianyuan;Fang, Yumin;Tong, Tianyi;Xia, Yabei;Liu, Xiao*;...

期刊： Applied Catalysis B: Environmental,2021年283:119645 ISSN：0926-3373

通讯作者： Liu, Xiao

作者机构： [Zhang, Lizhi; Tong, Tianyi; Fang, Yumin; Xia, Yabei; Liu, Xiao; Xu, Tianyuan] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Liu, Xiao] C;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.

关键词： Hematite;Interfacial reaction;Oxalate;Photodissociation;Reactive oxygen species

摘要： Oxalates, together with iron (hydr)oxides, play important roles in environmental decontamination by photochemical generation of reactive oxygen species (ROS). However, comprehending reaction mechanism about photolytic behaviors across solid-liquid interface is scarce. Here, the photochemical properties of hematite-oxalate system were investigated from complexation, photolysis, and ROS generation tests. Results implied adsorbed oxalate on hematite surface was detached via non-reductive dissolution by irradiating light. Then, the photolysis of Fe(III)-oxalate complexes on hematite surface or dissolved in solution was followed by photodissociation mechanism, in which per Fe(III)-oxalate complex led to two CO2[rad]− formation. Moreover, O2[rad]−/[rad]OOH and [rad]OH amounts induced by photodissociation mechanism were much higher than that by classic intramolecular ligand-to-metal charge transfer mechanism in Fe3+-Ox homogeneous system. The photo-degradation and mineralization of sulfadimidine (5 mg/L) reached 95 % and 59 % within 2 h using hematite-Ox system. These findings can help in implementing environmental remediation by utilizing iron (hydr)oxides and oxalate in natural environment. © 2020 Elsevier B.V.

语种： 英文

作者： Li, Hao;Jiang, Fuze;Drdova, Sarka;Shang, Huan;Zhang, Lizhi;...

期刊： Catalysis Science & Technology,2021年11(1):319-331 ISSN：2044-4753

通讯作者： Wang, Jing

作者机构： [Drdova, Sarka; Li, Hao; Wang, Jing; Jiang, Fuze] Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;[Drdova, Sarka; Li, Hao; Wang, Jing; Jiang, Fuze] Swiss Fed Labs Mat Sci & Technol, Empa, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.;[Zhang, Lizhi; Shang, Huan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Wang, Jing] S;Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;Swiss Fed Labs Mat Sci & Technol, Empa, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.

摘要： Solar-driven molecular oxygen activation by semiconductor photocatalysts is a prototypical reaction manifesting complex interactions among photons, charge carriers, and reactants. In this study, we demonstrate that energetic O2 activation towards volatile organic compound control can be realized via constructing a sophisticated surface hydrogen bond (HB) network having a dual-function. The extensive HBs established between the hydroxyl-rich BiOCl surface and phosphoric acid are first shown to significantly weaken surface Bi-O bonds, enabling facile oxygen vacancy (OV) generation. OVs, which act as reliable electron capture and static O2 activation centers, reinforce the interaction between photons and excitons for rapid charge carrier separation. Moreover, dynamic O2 activation with sluggish kinetics can be surmounted by another type of HB localized between hydroxyl groups of phosphoric acid and OV-adsorbed O2. These unique localized HBs facilitate interfacial electron transfer from BiOCl to O2, displaying a unique energy coupling route between charge carriers and reactants. For simulated indoor toluene oxidation, the substantially boosted O2 activation is shown to accelerate the kinetic processes associated with the primary oxidation of toluene into benzaldehyde and benzoic acid, as well as aromatic ring opening towards deep oxidation. Undesirable intermediate accumulation and catalyst deactivation are thus avoided. The present work highlights the pivotal roles of HBs in robust photocatalytic O2 activation. It will provide novel insights into the design of high-performance catalysts for efficient and safe control of indoor volatile organic compounds. This journal is © The Royal Society of Chemistry.

语种： 英文

作者： Li, Hao;Shang, Huan;Jiang, Fuze;Zhu, Xingzhong;Ruan, Qifeng;...

期刊： CHEMICAL SCIENCE,2021年12(46):15308-15317 ISSN：2041-6520

通讯作者： Wang, Jing

作者机构： [Li, Hao; Wang, Jing; Jiang, Fuze] Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;[Li, Hao; Wang, Jing; Jiang, Fuze] Empa, Swiss Fed Labs Mat Sci & Technol, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.;[Zhang, Lizhi; Shang, Huan] Cent China Normal Univ, Coll Chem, Inst Appl & Environm Chem, Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Zhu, Xingzhong] Nanjing Univ Aeronaut & Astronaut, Coll Sci, Nanjing 210016, Peoples R China.;[Ruan, Qifeng] Singapore Univ Technol & Design, Engn Prod Dev, Singapore 487372, Singapore.

通讯机构： [Wang, Jing] S;[Wang, Jing] E;Swiss Fed Inst Technol, Inst Environm Engn, CH-8093 Zurich, Switzerland.;Empa, Swiss Fed Labs Mat Sci & Technol, Lab Adv Analyt Technol, CH-8600 Dubendorf, Switzerland.

摘要： Manipulating O2 activation via nanosynthetic chemistry is critical in many oxidation reactions central to environmental remediation and chemical synthesis. Based on a carefully designed plasmonic Ru/TiO2-x catalyst, we first report a room-temperature O2 dissociation and spillover mechanism that expedites the 'dream reaction'of selective primary C-H bond activation. Under visible light, surface plasmons excited in the negatively charged Ru nanoparticles decay into hot electrons, triggering spontaneous O2 dissociation to reactive atomic O. Acceptor-like oxygen vacancies confined at the Ru-TiO2 interface free Ru from oxygen-poisoning by kinetically boosting the spillover of O from Ru to TiO2. Evidenced by an exclusive isotopic O-transfer from 18O2 to oxygenated products, O displays a synergistic action with native O2- on TiO2 that oxidizes toluene and related alkyl aromatics to aromatic acids with extremely high selectivity. We believe the intelligent catalyst design for desirable O2 activation will contribute viable routes for synthesizing industrially important organic compounds. This journal is © The Royal Society of Chemistry.

语种： 英文

作者： Luo, Xin;Yan, Min;Song, Weiyu;Fang, Qie;Wei, Xiaoqian;...

期刊： Advanced Functional Materials,2021年31(24):2101193- ISSN：1616-301X

通讯作者： Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn)

作者机构： [Zhu, Chengzhou; Wu, Nannan; Jiao, Lei; Gu, Wenling; Xu, Weiqing; Fang, Qie; Wei, Xiaoqian; Luo, Xin; Wang, Hengjia] Cent China Normal Univ, Coll Chem, Key Lab Pesticides & Chem Biol,Minist Educ, Int Joint Res Ctr Intelligent Biosensing Technol, Wuhan 430079, Peoples R China.;[Kang, Yikun; Song, Weiyu; Yan, Min] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.;[Zheng, Lirong] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China.;[Hu, Liuyong] Wuhan Inst Technol, Sch Mat Sci & Engn, Hubei Key Lab Plasma Chem & Adv Mat, Hubei Engn Technol Res Ctr Optoelect & New Energy, Wuhan 430205, Peoples R China.

通讯机构： [Chengzhou Zhu] K;Key Laboratory of Pesticides 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

关键词： biosensors;neutral zinc‐air batteries;oxygen reduction reaction;self‐powered sensing systems;single‐atom catalysts

摘要： Self-powered sensing systems (SPSSs) are critical components in smart portable electronic devices. Zinc-air batteries (ZABs) as promising energy devices provide a great opportunity to develop novel SPSS for sensing applications owing to the merit of high open-circuit potential. Herein, hierarchically porous single-atom iridium embedded nitrogen-doped carbon (SA-Ir/NC) is reported as an efficient catalyst for the oxygen reduction reaction (ORR) in the neutral ZABs, enabling the SPSSs towards glucose detection with a high sensitivity and stable output signal. The resultant SA-Ir/NC shows superior ORR activity and stability to commercial Pt/C in neutral electrolytes. According to the theoretical calculations, IrN5 active sites in SA-Ir/NC exhibit moderate adsorption free energy to reaction intermediates, giving SA-Ir/NC excellent four-electron ORR activity and well-enhanced H2O2 tolerance. When SA-Ir/NC is applied as an air cathode, the as-prepared ZABs display a large open-circuit voltage of 1.42V, a remarkable power density of 90.4mW cm−2, and excellent long-term stability. After being integrated with glucose oxidase, the SPSSs are successfully established for sensitive detection of glucose based on a competitive model, holding great promise in biosensing applications. © 2021 Wiley-VCH GmbH

语种： 英文

作者： Guo, Taolian;Mo, Kaili;Zhang, Nannan;Xiao, Lipengcheng;Liu, Wenlong;...

期刊： DALTON TRANSACTIONS,2021年50(5):1774-1779 ISSN：1477-9226

通讯作者： Wen, Lili

作者机构： [Mo, Kaili; Zhang, Nannan; Xiao, Lipengcheng; Guo, Taolian; Wen, Lili] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Liu, Wenlong] Yangzhou Univ, Coll Chem & Chem Engn, Yangzhou 225002, Jiangsu, Peoples R China.

通讯机构： [Wen, Lili] C;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.

摘要： Metal nanoparticle-incorporated metal-organic framework (MOF) nanosheets can integrate their respective merits to have important applications in heterogeneous catalysis. Herein, we report the loading of ultra-fine Pd nanoparticles within ultra-thin nanosheetsNMOF-Nithrough anin situreduction strategy under mild conditions. Owing to the synergetic effects of ultra-small Pd NPs and the intrinsic characteristics of two-dimensional supports, the obtainedPd@NMOF-Nishowed high catalytic activity and size-selectivity in olefin hydrogenation with easy recovery. Meanwhile,Pd@NMOF-Niis also highly active in the catalytic reduction of aqueous 4-nitrophenol to 4-aminophenol. © The Royal Society of Chemistry 2021.

语种： 英文

作者： Chen, Yifeng;Jiao, Lei;Yan, Hongye;Xu, Weiqing;Wu, Yu;...

期刊： Analytical Chemistry,2021年93(36):12353-12359 ISSN：0003-2700

通讯作者： Zhu, Chengzhou(czzhu@mail.ccnu.edu.cn)

作者机构： [Chen, Yifeng; 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.;[Zheng, Lirong] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China.

通讯机构： [Chengzhou Zhu] K;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

摘要： Although single-atom catalysts with high enzyme-like activities have been found, the rational design of highly active peroxidase (POD)-like nanozymes is still a formidable challenge. Herein, highly active POD-like nanozymes were synthesized through loading Pt clusters on the Fe single-atom (FeSA-PtC) nanozymes. The POD-like activity of FeSA-PtCnanozymes is enhanced 4.5-fold and 7-fold, in comparison to that of FeSAand PtCnanozymes, respectively, which is attributed to the unexpected synergistic effect between Fe single atoms and Pt clusters. Based on the outstanding POD-like activity of FeSA-PtCnanozymes, a cascade signal amplification strategy was constructed by combining glucose oxidase for the colorimetric biosensing of prostate-specific antigens, exhibiting satisfactory sensitivity, high selectivity, a low detection limit of 1.8 pg/mL, and practical feasibility in serum sample detection. This work may serve as a tough foundation to guide the design of superior POD-like nanozymes and expand the application in biosensing. © 2021 American Chemical Society

语种： 英文

作者： Dong, Wenbo;Yang, Yi;Xiang, Yonggang;Wang, Shengyao;Wang, Pei;...

期刊： Green Chemistry,2021年23(16):5797-5805 ISSN：1463-9262

通讯作者： Xiang, Yonggang(ygxiang@mail.hzau.edu.cn);Chen, Hao(hchenhao@mail.hzau.edu.cn);Rao, Li(raoli@mail.ccnu.edu.cn)

作者机构： [Xiang, Yonggang; Hu, Jianxiang; Wang, Shengyao; Dong, Wenbo; Wang, Pei; Chen, Hao; Yang, Yi] Huazhong Agr Univ, Coll Sci, Wuhan 430070, Peoples R China.;[Rao, Li] Cent China Normal Univ, Dept Chem, Key Lab Pesticide Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.

通讯机构： [Yonggang Xiang; Hao Chen] C;[Li Rao] K;College of Science, Huazhong Agricultural University, Wuhan 430070, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology (CCNU), Ministry of Education, Department of Chemistry, Central China Normal University, Wuhan 430079, PR China

摘要： The efficient conversion of aryl bromides to the corresponding aryl alkyl ethers by dual nickel/photocatalysis has seen great progress, but difficulties of recycling the photosensitizer or nickel complexes cause problems of sustainability. Here, we report the design of a novel, highly stable vinyl bridge 2D covalent organic framework (COF) containing Ni, which combines the role of photosensitizer and reactive site. The as-prepared sp2c-COFdpy-Ni acts as an efficient heterogeneous photocatalyst for C-O cross coupling. The sp2c-COFdpy-Ni can be completely recovered and used repeatedly without loss of activity, overcoming the limitations of the prior methods. Preliminary studies reveal that strong interlayer electron transfer may facilitate the generation of the proposed intermediate sp2c-COFdpy-NiI in a bimolecular and self-sustained manner. This all-in-one heterogeneous photocatalyst exhibits good compatibility of substrates and tolerance of functional groups. The successful attempt to expand the 2D COFs with this new catalyst into photocatalytic organic transformation opens an avenue for photoredox/transition metal mediated coupling reactions. © 2021 The Royal Society of Chemistry.

语种： 英文

作者： Zhang, Jin;Lucas, Rachel A.;Gu, Yulin;Yang, Yuxia;Sun, Kunpeng;...

期刊： Analytical Chemistry,2021年93(13):5430-5436 ISSN：0003-2700

通讯作者： Sun, Kunpeng(sunkp@licp.cas.cn);Li, Haibing(lhbing@mail.ccnu.edu.cn)

作者机构： [Sun, Kunpeng; Zhang, Jin] Chinese Acad Sci, Natl Engn Res Ctr Fine Petrochem Intermediates, Lanzhou Inst Chem Phys, Lanzhou 730000, Peoples R China.;[Zhang, Jin; Li, Haibing; Gu, Yulin; Yang, Yuxia] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Lucas, Rachel A.] Univ Calif Irvine, Dept Phys & Astron, Irvine, CA 92697 USA.

通讯机构： [Kunpeng Sun] N;[Haibing Li] K;National Engineering Research Center for Fine Petrochemical Intermediates, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou730000, P. R. China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China

摘要： Nanopore-based detection techniques, with a wide range of transport properties, exhibit impressive selectivity and sensitivity for analytes. To expand the application of nanoporous sensors, real-time and fast detection of targets, all within a portable device, is highly desired for nanopore-based sensors. In addition, to improve the accuracy of the output signal, more appropriate readout methods also need to be explored. In this manuscript, we describe a nanopore-based electrode, regarded as NAC-P6-PC@AuE, prepared by coupling a pillararene-based nanoporous membrane with an electrochemical impedance measurement method. The fabricated device is demonstrated by exposing pillararene-based receptors to trace amounts of pesticide molecules. NAC-P6-PC@AuE devices exhibit distinguished selectivity to quinotrione, as well as the ability to quantify quinotrione with a limit of quantitation (LOQ) of 10 nM. The mechanism that allows sensing was verified using finite-element simulations and may be explained as host-guest-induced surface charge shielding, which influences the electrochemical response of probe molecules. The applications of this nanopore-based electrode may be extended toward other target molecules by decorating the nanopore surfaces with specifically chosen receptors. ©

语种： 英文

作者： Cao, Zhusong;Li, Jianye;Sun, Youwen;Zhang, Hanwen;Mo, Xueling;...

期刊： CHEMICAL SCIENCE,2021年12(13):4836-4840 ISSN：2041-6520

通讯作者： Cao, Xin(caox@fudan.edu.cn)

作者机构： [Cao, Zhusong; Zhang, Guozhu; Zhang, Hanwen; Sun, Youwen; Mo, Xueling] Chinese Acad Sci, Univ Chinese Acad Sci, Ctr Excellence Mol Synth, Shanghai Inst Organ Chem,Key Lab Organometall Che, 345 Lingling Rd, Shanghai 200032, Peoples R China.;[Zhang, Guozhu; Li, Jianye] Cent China Normal Univ CCNU, Coll Chem, 152 Luoyu Rd, Wuhan 430079, Hubei, Peoples R China.;[Cao, Xin] Fudan Univ, Zhongshan Hosp, 180 Fenglin Rd, Shanghai 200032, Peoples R China.

通讯机构： [Xin Cao] Z;[Guozhu Zhang] K;Zhongshan Hospital, Fudan University, 180 Fenglin Road, Shanghai 200032, P. R. China<&wdkj&>Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Center for Excellence in Molecular Synthesis, University of Chinese Academy of Sciences, Chinese Academy of Sciences, 345 Lingling Road, Shanghai 200032, P. R. China<&wdkj&>College of Chemistry, Central China Normal University (CCNU), 152 Luoyu Road, Wuhan, Hubei 430079, P. R. China

摘要： A method for remote radical C-H alkynylation and amination of diverse aliphatic alcohols has been developed. The reaction features a copper nucleophile complex formedin situas a photocatalyst, which reduces the silicon-tethered aliphatic iodide to an alkyl radical to initiate 1,n-hydrogen atom transfer. Unactivated secondary and tertiary C-H bonds at β, γ, and δ positions can be functionalized in a predictable manner. © The Royal Society of Chemistry 2021.

语种： 英文