作者： Shang, Huan;Chen, Ziyue;Wang, Xiao;Li, Meiqi;Li, Hao;...

期刊： Applied Catalysis B: Environmental,2022年308:121217 ISSN：0926-3373

通讯作者： Ai, Zhihui(jennifer.ai@mail.ccnu.edu.cn)

作者机构： [Yu, Linghao; Zhang, Lizhi; Shang, Huan; Mao, Chengliang; Li, Hao; Chen, Ziyue; Ai, Zhihui; Li, Meiqi] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Sun, Jing; Wang, Xiao] Chinese Acad Sci, Shanghai Inst Ceram, Shanghai 200050, Peoples R China.

通讯机构： [Zhihui Ai; Lizhi Zhang] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, PR China

关键词： Heterogeneous SO2 oxidation;HONO;Nitrate photolysis;Photochemistry;TiO2 mineral

摘要： In this study, we investigated the nitrate photolysis on photoactive TiO2 particles in the presence of SO2 through theoretic DFT calculation and in situ DRIFTS analysis, and found that in a clean atmosphere nitrate was oxidized to •NO3 radicals by the holes generated on the surface of TiO2 under solar irradiation, followed reactive nitrogen species generation via •NO3 radicals reduction by photoinduced electrons. After shifting to the SO2-polluted environment, •NO3 radicals preferentially reacted with abundant sulfites to significantly increase nitrogen species formation, the online measured concentrations of NOx and HONO increased by approximately 2-fold and 6-fold respectively in comparison with clean atmosphere. These results demonstrate that photogenerated holes play a key role in nitrate photolysis on photoactive mineral dusts with or without the coexistence of SO2, providing new insights into the source of NOx and HONO in complex air polluted areas during the daytime. © 2022 Elsevier B.V.

语种： 英文

作者： Zhang, Shoute;Meng, Ying;Pang, Lei;Ding, Qianzhao;Chen, Zhen;...

期刊： Catalysis Science & Technology,2022年12(2):579-595 ISSN：2044-4753

通讯作者： Li, Tao;Guo, Yanbing

作者机构： [Meng, Ying; Li, Tao; Chen, Zhen; Zhang, Shoute; Ding, Qianzhao] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Mat Chem & Serv Failure, Key Lab Mat Chem Energy Convers & Storage,Minist, 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, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Cai, Weiquan] Guangzhou Univ, Guangzhou Higher Educ Mega Ctr, Sch Chem & Chem Engn, 230 Wai Huan Xi Rd, Guangzhou 510006, Peoples R China.

通讯机构： [Li, Tao] H;[Guo, Yanbing] C;Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Mat Chem & Serv Failure, Key Lab Mat Chem Energy Convers & Storage,Minist, Wuhan 430074, Peoples R China.;Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.

摘要： Cu-SAPO-34 catalysts used for the selective catalytic reduction with ammonia (NH3-SCR) reaction deteriorate when exposed to moisture at low temperature (<100 °C), which seriously hinders their commercial application prospects. In this work, Cu-SAPO-34 catalysts templated using various structure-directing agents (SDAs), i.e., DEA, TEA, PA, and TEAOH, were elegantly fabricated via a “one-pot” protocol. The direct relationship between the various SDAs and low-temperature moisture degradation were determined in this work. Via thorough characterizations, it was evidenced that the Cu-SAPO-34 catalysts with more Si–O(H)–Al bonds, more Cu(OH)+ moieties and fewer CuOx clusters exhibited higher SCR catalytic activities and N2 selectivity. After low-temperature hydration treatment, the relative crystallinity, porosity, Si–O(H)–Al density, and active Cu(OH)+ in the catalysts declined, but in varying degrees, where the Cu-SAPO-34 catalysts possessing more Si–O(H)–Al density and Cu(OH)+ moieties being the more susceptible to hydrolysis and structural degradation, and vice versa. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis confirmed that both the fresh and degraded Cu-SAPO-34 catalysts primarily follow the Langmuir–Hinshelwood pathway due to its faster reaction rate and lower reaction barrier than the Eley–Rideal pathway.

语种： 英文

作者： Yang, Lei;Zhang, Fan;Quan, Jiaxin;Li, Jia;Li, Haibing

期刊： ChemNanoMat,2022年8(10):e202200342- ISSN：2199-692X

通讯作者： Li, Haibing(lhbing@mail.ccnu.edu.cn);Li, Jia(2014079@mail.scuec.edu.cn)

作者机构： [Yang, Lei; Li, Haibing] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol CCNU, Wuhan 430079, Peoples R China.;[Zhang, Fan] Hubei Univ, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Minist Educ, Key Lab Synth & Applicat Organ Funct Mol,Coll Che, Wuhan 430062, Peoples R China.;[Quan, Jiaxin] Hanjiang Normal Univ, Coll Chem & Environm Engn, Shi Yan 432200, Peoples R China.;[Li, Jia] South Cent Minzu Univ, Coll Resources & Environm Sci, Wuhan 430074, Peoples R China.

通讯机构： [Prof. Jia Li; Prof. Jia Li Prof. Jia Li Prof. Jia Li] C;[Prof. Dr. Haibing Li; Prof. Dr. Haibing Li Prof. Dr. Haibing Li Prof. Dr. 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<&wdkj&>College of Resources and Environmental Science, South-Central Minzu University, Wuhan, 430074 P. R. China

关键词： DANN;multi-chiral;nanochannel;pillar[5]arene;translocation

摘要： Chirality is an intrinsic feature of nature and plays a crucial role in molecular translocation. However, how chirality affects or even more strongly affects DNA translocation remains largely unknown. Here, a facile and feasible strategy was contributed for the construction of chiral pillar[5]arene-modified nanochannels (D/L-Phe-P5 nanochannels) that can enhance recognition and accelerate DNA translocation. The results showed the L-Phe-P5 nanochannel elevated the DNA translocation efficiency by about 6.59-fold compared to the Mono-L-Phe-P5 channel. Furthermore, the translocation efficiency of the L-Phe-P5 nanochannel with multi-chiral centers was 3.06-fold higher than that of the D-Phe-P5 nanochannel, and this value was 2.25-fold higher than the ratio of the translocation efficiency between the Mono-L-Phe-P5 channel and Mono-D-Phe-P5 channel. Finally, the theoretical simulation and analysis of the translocation mechanism were performed by COMSOL Multiphysics software. This research not only enriches the basic theory research related to the influence of chirality on DNA translocation, but also has great reference value for the further development of DNA application. More importantly, the chiral amplification strategy could also extend to the selectivity of other chiral biomolecules, which may have potentially far-reaching implications. © 2022 Wiley-VCH GmbH.

语种： 英文

作者： Qu, Haonan;Dai, Shaoming;Qu, Yanquan;Zhang, Siyun;Lu, Mingxiang;...

期刊： ACS Applied Nano Materials,2022年5(10):14970-14977 ISSN：2574-0970

通讯作者： Li, Haibing(lhbing@mail.ccnu.edu.cn);Lu, Zhiyan(1657168843@qq.com);Zhou, Juan(zhoujuan@wh.iov.cn)

作者机构： [Li, Haibing; Qu, Haonan; Zhang, Siyun] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Qu, Yanquan; Lu, Mingxiang] Tradit Chinese Med Hosp Wuxue, Dept Radiol, Huanggang 438200, Hubei, Peoples R China.;[Qu, Yanquan; Lu, Zhiyan] Wuhan Univ, Zhongnan Hosp, Dept Radiol, Wuhan 430071, Hubei, Peoples R China.;[Zhou, Juan; Li, Haibing] Chinese Acad Sci, Wuhan Inst Virol, Ctr Biosafety Mega Sci, State Key Lab Virol, Wuhan 430071, Peoples R China.;[Li, Haibing; Lu, Mingxiang] Wuhan Univ, Zhongnan Hosp, Dept Forens Med, Wuhan 430071, Peoples R China.

通讯机构： [Zhiyan Lu] D;[Juan Zhou] S;[Haibing Li] K;State Key Laboratory of Virology, Wuhan Institute of Virology, Center for Biosafety Mega-Science, Chinese Academy of Sciences, Wuhan 430071, 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<&wdkj&>Department of Forensic Medicine, Zhongnan Hospital of Wuhan University, No.169 East Lake Road, Wuchang District, Wuhan 430071, P. R. China<&wdkj&>Department of Forensic Medicine, Zhongnan Hospital of Wuhan University, No.169 East Lake Road, Wuchang District, Wuhan 430071, P. R. China

关键词： pillar[5]arenes;sub-nanoporous;proton;selective;unidirectional transport

摘要： Proton transport is involved in many biological processes, such as viral replication and enzymatic catalysis. However, one-way transmission is the premise of the realization of the above functions. Actually, the unidirectional transport of protons is significant not only for biology but also for practical applications. Herein, inspired by the influenza A M2 channel, a sub-nanoporous proton transport membrane was constructed by layer-by-layer assembly of two oppositely charged pillar[n]arenes with sub-nanometer cavities. A good selectivity of the proton transport membranes to protons was achieved by exploiting the size effect of sub-nanometer pores. And the proton transport membrane has a transport capacity of 459 μM·m-2·h-1 for protons. For nanofluidic diodes, the construction of the sub-nanopore proton transport membrane was very meaningful. For energy conversion applications such as catalytic transformations, although the flux cannot meet the application in these fields, the development of this membrane provides an idea for it. What is more, it can help deepen the understanding of the relationship between sub-nanostructure and function. © 2022 American Chemical Society.

语种： 英文

作者： Chen, Tiantian;Hu, Jiajia;Chen, Yanyan;Liu, Ying;Li, Yan;...

期刊： Analytica Chimica Acta,2022年1190:339263 ISSN：0003-2670

通讯作者： Xu, Hui

作者机构： [Liu, Ying; Hu, Jiajia; Li, Yan; Chen, Tiantian; Xu, Hui; Chen, Yanyan] Cent China Normal Univ, Coll Chem, Key Lab Insecticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.

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

关键词： Fipronil;Gas chromatography-mass spectrometry;Invivo solid phase microextraction;Long-term monitoring;Metabolites

摘要： In this study, a sampling rate-corrected in vivo solid-phase microextraction-gas chromatography-mass spectrometry method (SR-in vivo SPME-GC-MS) was constructed to simultaneously detect fipronil and three of its metabolites in garlic, and their environmental behavior was long-term monitored in in vivo mode. All of three fipronil metabolites were more difficult to degrade than the parent pesticide. The final degradation rates of the metabolites in garlic were in the range of 4.4%-25.1%, much lower than that of the parent (78.6%-85.8%). While their total residues amount was about 3 times as high as fipronil, exceeding the maximum residue limits regulated by China and the European Union. The steady-state concentrations of fipronil and its metabolites in garlic were positively correlated with the pesticide stress dose. In short, the established in vivo tracking method is efficient and convenient. The features of simple operation, fast analysis, acceptable sensitivity, non-harmful or non-lethal to plants, available repeated and long-term monitoring of the same organism make it attractive for in vivo tracking assay, it is of great significance for the guidance of rational use of fipronil and protection of food safety. © 2021 Elsevier B.V.

语种： 英文

作者： Jia, Shuwen;Fan, Lingyue;Zheng, Chunyang;Jin, Sai;Li, Dongfeng

期刊： DALTON TRANSACTIONS,2022年51(34):12968-12974 ISSN：1477-9226

通讯作者： Zheng, Chunyang(zcy800204@163.com);Li, Dongfeng(dfli@mail.ccnu.edu.cn)

作者机构： [Jia, Shuwen; Li, Dongfeng; Fan, Lingyue; Jin, Sai] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Zheng, Chunyang] Hubei Normal Univ, Hubei Collaborat Innovat Ctr Rare Met Chem, Inst Adv Mat, Hubei Key Lab Pollutant Anal & Reuse Technol, Huangshi 435002, Hubei, Peoples R China.

通讯机构： [Jia, Shuwen] K;[Zheng, Chunyang] H;Hubei Collaborative Innovation Center for Rare Metal Chemistry, Hubei Key Laboratory of Pollutant Analysis and Reuse Technology, Institute for Advanced Materials, Hubei Normal University, 435002 Huangshi, P. R. China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, Central China Normal University, 430079 Wuhan, P. R. China

摘要： Cyano-bridged mixed-valence {Fe6} hexanuclear complexes {[Tp4-MeFeII(CN)3]2[FeIII(Tpa)]2[FeIII(OR)(Tpa)]2}·6ClO4·S (Tp4-Me = tri(4-methyl-pyrazol-1-yl)borate, Tpa = tris(2-pyridylmethyl)amine; R = -CH3, S = 8MeOH 1, R = -C2H5, S = 6EtOH 2) have been obtained by building the units of [Tp4-MeFe(CN)3]− and [Fe(Tpa)]2+ in methanol and ethanol, respectively. Complex 1 exhibited single-crystal-to-single-crystal (SCSC) transformation to give {[Tp4-MeFeII(CN)3]2[FeIII(Tpa)]2[FeIII(OH)(Tpa)]2}·6ClO4·8H2O (3) in water. Detailed analysis of the coordination environment of the FeIII centers on the square lattice and magnetic susceptibility measurements of all the complexes confirmed their Fe3+ spin-crossover (SCO) properties (T1/2 = 178 K, 1; 185 K, 2; 208 K, 3). © 2022 The Royal Society of Chemistry.

语种： 英文

作者： Liu, Yanping;Jia, Shanshan;Zheng, Shi;Tan, Ying;Yang, Xiaojie;...

期刊： Analytical and Bioanalytical Chemistry,2022年414(17):4809-4819 ISSN：1618-2642

通讯作者： Zhong, Hongying(hyzhong@gxu.edu.cn)

作者机构： [Shen, Baojie; Yang, Xiaojie; Zheng, Shi; Zhong, Hongying; Tan, Ying; Liu, Yanping; Jia, Shanshan] Cent China Normal Univ, Minist Educ, Key Lab Pesticides & Chem Biol, Lab Mass Spectrometry,Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Zhong, Hongying] Guangxi Univ, Coll Life Sci & Technol, State Key Lab Conservat & Utilizat Subtrop Agro B, Ctr Instrumental Anal, Nanning 530004, Guangxi, Peoples R China.

通讯机构： [Hongying Zhong] L;Laboratory of Mass Spectrometry, College of Chemistry, Key Laboratory of Pesticides and Chemical Biology, Ministry of Education, Central China Normal University, Wuhan, People’s Republic of China<&wdkj&>Center for Instrumental Analysis, State Key Laboratory for Conservation and Utilization of Subtropical Agro Bioresources, College of Life Science and Technology, Guangxi University, Nanning, People’s Republic of China

关键词： Fractionation of essential oils;Active alumina beads;Porous TiO2 thin film;Cu benzene-1,3,5-tricarboxylate (Cu-BTC);Metal organic framework (MOF)

摘要： Fractionation of essential oils is technically challenging due to enormous scaffold diversities and structural complexities as well as difficulties in the implementation of the fractionation in the gas phase. Packing beads with multi-dimensional hierarchical nanostructures have been developed herein to pack fractional columns for atmospheric distillations. Activated alumina beads were coated with a porous TiO2 thin film. Growth of Cu-BTC (benzene-1,3,5-tricarboxylate) crystals in resultant porous surfaces leads to the generation of new nanopores and increased metal centers for differential coordination with diverse components of essential oils. The TiO2 thin film is not only an integral part of the composites but also induces the oriented growth of Cu-BTC metal organic framework (MOF) crystals through coordinative interactions. These Al2O3@TiO2@Cu-BTC MOF beads show very strong absorptive capability for major components of essential oils, except for a single cyclic ether eucalyptol with steric hindrances. The eucalyptol was fractionated by using the column packed with those modified alumina beads from raw materials of Artemisia argyi, and Rosmarinus officinalis with high purities up to 96% and 93%, respectively. Graphical abstract: [Figure not available: see fulltext.]. © 2022, Springer-Verlag GmbH Germany, part of Springer Nature.

语种： 英文

作者： Li, Guang;Gong, Wen;Yang, Lei;Cheng, Ming;Yan, Hewei;...

期刊： Bioconjugate Chemistry,2022年33(12):2237-2244 ISSN：1043-1802

通讯作者： Li, Haibing;Lu, Zhiyan;Zhang, Fan;Quan, Jiaxin

作者机构： [Cheng, Ming; Li, Guang; Yang, Lei; Li, Haibing; Yan, Hewei] Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Gong, Wen] Hosp Hubei Prov, Peoples Hosp Hubei Prov 3, Dept Cardiol, Wuhan 430030, Peoples R China.;[Lu, Zhiyan] Wuhan Univ, Zhongnan Hosp, Dept Forens Med, Wuhan 430071, Peoples R China.;[Zhang, Fan] Hubei Univ, Coll Chem & Chem Engn, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Minist Educ,Key Lab Synth & Applicat Organ Funct, Wuhan 430062, Peoples R China.;[Quan, Jiaxin] Hanjiang Normal Univ, Dept Chem & Environm Engn, Shiyan 442000, Peoples R China.

通讯机构： [Li, Haibing] C;[Lu, Zhiyan] W;[Zhang, Fan; Quan, Jiaxin] H;Cent China Normal Univ, Coll Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;Wuhan Univ, Zhongnan Hosp, Dept Forens Med, Wuhan 430071, Peoples R China.

摘要： In living systems, the adsorption of a protein on biointerfaces is a universal phenomenon, such as the specific binding of an antibody and antigen, which plays an important role in body growth and life maintenance. The exploration of a protein-selective adsorption on the biointerface is of great significance for understanding the life process and treatment in vitro. Herein, on the basis of biomimetic strategies, we fabricated a planar-chiral NH2-pillar[5]arene modified silicon surface (pR-/pS-NP5 surfaces) for a highly enantioselective adsorption of protein by taking advantage of the guest-induced planar chirality of pillar[5]arenes. Results from practical experiments and theoretical calculations show that the pR-NP5 surface possesses a high adsorption capacity and chiral selectivity for bovine serum albumin (BSA). Moreover, it was identified that the guest-induced chiral effect the generation and amplification of planar chirality, which was much beneficial for enhancing the interaction between planar-chiral pillar[5]arene host and BSA. The binding capacity of pR-NP5 and BSA is stronger than that of pS-NP5, thus promoting the chiral selective adsorption of BSA. This work affords a deeper understanding of the chiral influence of protein adsorption on biointerfaces and meanwhile provides a new perspective for chiral-sensing applications. © 2022 American Chemical Society. All rights reserved.

语种： 英文

作者： Wang, Zhe;Mao, Boyang;Zhao, Ming;Calatayud, David G.;Qian, Wei;...

期刊： ACS Nano,2022年16(3):3934-3942 ISSN：1936-0851

通讯作者： He, DP;Kou, ZK

作者机构： [Wang, Zhe; Zhao, Xin; Qian, Wei; Yan, Shilin; He, DP; He, Daping; Li, Peng] Wuhan Univ Technol, Sch Sci, Wuhan 430070, Peoples R China.;[Hu, Zhigang; Mao, Boyang] Univ Cambridge, Dept Engn, Cambridge CB3 0FA, England.;[Zhao, Ming] Cent China Normal Univ, Minist Educ, Coll Chem, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Calatayud, David G.] Inst Ceram & Vidrio CSIC, Dept Electroceram, Madrid 28049, Spain.;[Kou, ZK; Kou, Zongkui; Fu, Huaqiang] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.

通讯机构： [Kou, ZK ; He, DP ] W;Wuhan Univ Technol, Sch Sci, Wuhan 430070, Peoples R China.;Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China.;Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China.

关键词： graphene oxide;membranes;ultrafast macroscopic assembly;strength;superhydrophilic aisle

摘要： A macroscopic-assembled graphene oxide (GO) membrane with sustainable high strength presents a bright future for its applications in ionic and molecular filtration for water purification or fast force response for sensors. Traditionally, the bottom-up macroscopic assembly of GO sheets is optimized by widening the interlaminar space for expediting water passage, frequently leading to a compromise in strength, assembly time, and ensemble thickness. Herein, we rationalize this strategy by implanting a superhydrophilic bridge of cobalt-based metal-organic framework nanosheets (NMOF-Co) as an additional water "aisle" into the interlaminar space of GO sheets (GO/NMOF-Co), resulting in a high-strength macroscopic membrane ensemble with tunable thickness from the nanometer scale to the centimeter scale. The GO/NMOF-Co membrane assembly time is only 18 s, 30800 times faster than that of pure GO (154 h). More importantly, the obtained membrane attains a strength of 124.4 MPa, which is more than 3 times higher than that of the GO membrane prepared through filtration. The effect of hydrophilicity on membrane assembly is also investigated by introducing different intercalants, suggesting that, except for the interlamellar spacing, the interlayered hydrophilicity plays a more decisive role in the macroscopic assembly of GO membranes. Our results give a fundamental implication for fast macroscopic assembly of high-strength 2D materials. © 2022 American Chemical Society. All rights reserved.

语种： 英文

作者： Guo, Jing*;Si, Mingming;Zhao, Xuetong;Wang, Li;Wang, Ke;...

期刊： Carbon,2022年190:255-261 ISSN：0008-6223

通讯作者： Guo, Jing;Wang, H;Randall, CA

作者机构： [Wang, Hong; Si, Mingming; Hao, Jianyu; Guo, Jing; Guo, J] Xi An Jiao Tong Univ, Sch Mat Sci & Engn, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China.;[Zhao, Xuetong] Chongqing Univ, State Key Lab Power Transmiss Equipment & Syst Se, Chongqing 400044, Peoples R China.;[Wang, Li] Cent China Normal Univ, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.;[Wang, Li] Cent China Normal Univ, Sch Chem, Wuhan 430079, Peoples R China.;[Randall, CA; Wang, Ke; Randall, Clive A.] Penn State Univ, Mat Res Inst, University Pk, PA 16802 USA.

通讯机构： [Randall, CA ] P;[Wang, H ; Guo, J] X;Xi An Jiao Tong Univ, Sch Mat Sci & Engn, State Key Lab Mech Behav Mat, Xian 710049, Peoples R China.;Penn State Univ, Mat Res Inst, University Pk, PA 16802 USA.;Penn State Univ, Dept Mat Sci & Engn, University Pk, PA 16802 USA.

关键词： C60;Cold sintering process;Composites;Interfacial effects;Low temperature sintering;ZnO

摘要： A lot of nanocomposites containing C60 have been developed to enable various application opportunities. However, it seems impossible to incorporate C60 into ceramics without destroying the C60 molecules, because ceramics are typically sintered at high temperatures that could result in the chemical reaction of C60. Herein, we report the successful integration of C60 with ZnO using cold sintering process. (1-x)ZnO-xC60 composites with x ranging from 0 to 5 wt% are densified into monolithic structures with relative densities over 95%. Clear C60 molecules are observed in the cold sintered composites, and thin C60 layers with less than 10 nm are located at the ZnO grain boundaries. With C60 altering the interfacial structures of ZnO ceramics, the electrical properties are improved significantly, especially, the breakdown electric field at 1 mA cm−2 is enhanced from ∼80 V mm−1 to ∼2100 V mm−1. The FEM analysis indicates that the current density at the interfaces of ZnO and C60 is higher than other regions. This work thus indicates that cold sintering process provides a promising pathway to design new types of functional materials through the integration of C60 and ceramics. © 2022 Elsevier Ltd

语种： 英文

作者： Yang, Jing-Fang;Chen, Wei-Jie;Zhou, Li-Ming;Hewage, Kamalani Achala H.;Fu, Yi-Xuan;...

期刊： ACS Applied Materials & Interfaces,2022年14(25):28489-28500 ISSN：1944-8244

通讯作者： Hao, Ge-Fei(gefei_hao@foxmail.com);Yang, Guang-Fu(gfyang@mail.ccnu.edu.cn)

作者机构： [Song, Ke; Chen, Wei-Jie; Yang, Jing-Fang; Yang, Guang-Fu; Yin, Jun; Fu, Yi-Xuan; Pei, Rong-Jie; Zhou, Li-Ming; Hewage, Kamalani Achala H.; He, Bo; Hao, Ge-Fei] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Song, Ke; Chen, Wei-Jie; Yang, Jing-Fang; Yang, Guang-Fu; Yin, Jun; Fu, Yi-Xuan; Pei, Rong-Jie; Zhou, Li-Ming; Hewage, Kamalani Achala H.; He, Bo; Hao, Ge-Fei] Cent China Normal Univ, Int Joint Res Ctr Intelligent Biosensor Technol &, Wuhan 430079, Peoples R China.;[Chen, Mo-Xian] Nanjing Forestry Univ, Coll Biol & Environm, Coinnovat Ctr Sustainable Forestry Southern China, Nanjing 210037, Peoples R China.;[Chen, Mo-Xian] Nanjing Forestry Univ, Coll Biol & Environm, Key Lab Natl Forestry & Grassland Adm Subtrop For, Nanjing 210037, Peoples R China.;[Zhang, Jian-Hua] Hong Kong Baptist Univ, Dept Biol, Hong Kong 300072, Peoples R China.

通讯机构： [Ge-Fei Hao; Guang-Fu Yang] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>International Joint Research Center for Intelligent Biosensor Technology and Health, Central China Normal University, Wuhan 430079, China

关键词： KEYWORDS;indicator dye;dansylamide;PYR1;noninvasive;salt stress

摘要： Environmental stress greatly decreases crop yield. The application of noninvasive techniques is one of the most practical and feasible ways of monitoring the health condition of plants under stress. However, it remains largely unsolved. A chemical fluorescent probe can be applied as a typical nondestructive method, but it has not been applied in living plants for stress detection to date. The abscisic acid (ABA) receptor plays a central role in conferring tolerance to environmental stresses and is an excellent target for developing fluorescent probes. Herein, we developed a fluorescence molecular imaging technology to monitor live plant stress by visualizing the protein expression level of the ABA receptor PYR1. A computer-aided designed indicator dye, flubactin, exhibited an 8-fold enhancement in fluorescence intensity upon interaction with PYR1. In vitro and in vivo experiments showed that flubactin is suitable to be used to detect salt stress in plants in real time. Moreover, the low toxicity of flubactin promotes its application in the future. Our work opens a new era for the nondestructive visualization of plant stress in vivo. © 2022 American Chemical Society. All rights reserved.

语种： 英文

作者： Li, Wenlu;Wei, Zhen;Zhu, Kaijian;Wei, Weiqin;Yang, Jun;...

期刊： Applied Catalysis B: Environmental,2022年306:121142 ISSN：0926-3373

通讯作者： Wei, Zhen(xfwz522@126.com)

作者机构： [Jing, Jianfang; Yang, Jun; Zhu, Yongfa; Li, Wenlu] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China.;[Phillips, David Lee; Wei, Zhen] Univ Hong Kong, Dept Chem, Pokfulam Rd, Hong Kong, Peoples R China.;[Zhu, Kaijian] Univ Twente, MESA, PhotoCatalyt Synth Grp, Inst Nanotechnol, POB 217, NL-7500AE Enschede, Netherlands.;[Wei, Weiqin] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.

通讯机构： [Zhen Wei; David Lee Phillips; Yongfa Zhu] D;Department of Chemistry, University of Hong Kong, Pokfulam Road, Hong Kong, China<&wdkj&>Department of Chemistry, Tsinghua University, Beijing 100084, PR China

关键词： Femtosecond transient absorption spectroscopy;Graphite carbon nitride;Nitrogen defects;Photocatalysis;Trap states

摘要： Defect structures of semiconductors intrinsically regulate the trap states, excitons and active charge carriers for artificial photosynthesis systems. A g-C3N4 system with abundant nitrogen defects was prepared through a thermal polycondensation strategy to reveal the role of trap states and exhibited a 20-fold enhanced H2 evolution efficiency relative to bulk g-C3N4 under visible light irradiation. Subsequent femtosecond transient absorption spectroscopy study found that the N-defect induced shallow trap states can capture photogenerated electrons to inhibit deep trapping and direct recombination of photogenerated charges. The active electrons in shallow trap states can enhance the photocatalytic H2 evolution when compared with the inactive electrons in deep trap states. Mid-infrared transient absorption spectroscopy also confirmed the increased quantity of shallow-trapped electrons without interference of other signals. This work provides new insights for steering depth of trap states and photocatalytic processes through N defects to achieve high photocatalytic performance using femtosecond transient absorption spectroscopy. © 2022 Elsevier B.V.

语种： 英文

作者： Yan, Hewei;Quan, Jiaxin;Qu, Haonan;Zhu, Fei;Wang, Yingqian;...

期刊： ACS Applied Nano Materials,2022年5(12):18637-18644 ISSN：2574-0970

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

作者机构： [Wang, Yingqian; Li, Haibing; Qu, Haonan; Zhu, Fei; Dhinakaran, Manivannan Kalavathi; Quan, Jiaxin; Yan, Hewei] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Han, Ting; Yan, Hewei] Shenzhen Univ, Coll Mat Sci & Engn, Ctr AIE Res, Guangdong Res Ctr Interfacial Engn Funct Mat, Shenzhen 518060, Peoples R China.;[Quan, Jiaxin] Hanjiang Normal Univ, Dept Chem & Environm Engn, Shiyan 442000, Peoples R China.

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, Wuhan430079, China

关键词： aligned;nanochannel;directional assembly;pillar[6]arenes;isomers

摘要： Membrane separation technology has been widely applied in material separation fields. However, it still has the disadvantage of poor selectivity at nanometer and sub-nanometer scales. Here, two kinds of pillar[6]arene with opposite charges were prepared by modification, and the aligned nanochannel composite membrane was successfully constructed by directional assembly on a negatively charged silicon interface. The precise sieving properties of aligned channels were studied using the xylene isomer as a model molecule. It has been proved that the aligned channel can better maintain the pore size close to the macrocyclic molecules, which is beneficial to realize the customized construction of the through-ordered nanochannel. The experimental results show that the aligned nanochannel can selectively transport xylene isomers, and the flux (J) values of o, m, and p-xylene were 9.2, 11.6, and 171.3 nM m-2h-1, respectively. Finally, the separation and purification of mixed samples have been achieved. This method provides a strategy for constructing ordered nanochannels. © 2022 American Chemical Society. All rights reserved.

语种： 英文

作者： Tang, Yinjun;Wu, Yu;Xu, Weiqing;Jiao, Lei;Chen, Yifeng;...

期刊： Analytical Chemistry,2022年94(2):1022-1028 ISSN：0003-2700

通讯作者： Zhu, CZ

作者机构： [Xu, Weiqing; Chen, Yifeng; Tang, Yinjun; Zhu, Chengzhou; Sha, Meng; Wu, Yu; Jiao, Lei; Zhu, CZ; 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.;[Ye, Hua-Rong] Wuhan Univ Sci & Technol, China Resources & Wisco Gen Hosp, Dept Med Ultrasound, Wuhan 430080, Peoples R China.

通讯机构： [Zhu, CZ ] C;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.

摘要： Noble-metal-based nanozymes have attracted great interest as enzyme mimics because of their unique properties. To modulate the performance and meet the requirements of practical biosensing applications, phase engineering is promising for the design of novel noble-metal-based nanomaterials. Herein, a simple salt-assist strategy was employed for the synthesis of Ru nanosheets (NSs) with the controlled crystalline degree. The crystalline degree plays a significant role in tuning peroxidase-like activity by optimizing the affinity toward the catalytic substrate. Furthermore, the inhibition effect of mercapto molecules on the peroxidase-like activity of Ru NSs was investigated. As a proof-of-concept, the Ru NSs-based colorimetric sensing arrays were developed to distinguish mercapto molecules, and five model molecules were well classified according to the different inhibition effects. Given the complexity of practical conditions, the sensing array was further applied to discriminate proteins possessing rich mercapto groups. This work not only provides an effective strategy for the design of highly active nanozymes but also achieves promising sensing arrays for practical needs. © 2021 American Chemical Society

语种： 英文

作者： Zhang, Mao-Mao;Qu, Bao-Le;Shi, Bin;Xiao, Wen-Jing;Lu, Liang-Qiu

期刊： CHEMICAL SOCIETY REVIEWS,2022年51(10):4146-4174 ISSN：0306-0012

通讯作者： Lu, LQ

作者机构： [Lu, Liang-Qiu; Lu, LQ; Qu, Bao-Le; Xiao, Wen-Jing; Zhang, Mao-Mao; Shi, Bin] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Peoples R China.;[Xiao, Wen-Jing] Shanghai Inst Organ Chem, State Key Lab Organometall Chem, 345 Lingling Rd, Shanghai 200032, Peoples R China.;[Lu, Liang-Qiu; Lu, LQ] Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China.;[Lu, Liang-Qiu; Lu, LQ] Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China.

通讯机构： [Lu, LQ ] C;Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticide & Chem Biol,Minist Educ, 152 Luoyu Rd, Wuhan 430079, Peoples R China.;Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China.;Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China.

摘要： Medium-sized heterocycles are widespread among a spectrum of structurally intriguing and biologically significant natural products and synthetic pharmaceuticals. Metal-catalyzed high-order dipolar annulations resembling reactions of metal-containing reactive dipoles with dipolarophiles constitute a highly efficient and flexible strategy for constructing medium-sized heterocycles. Mechanistically, these annulation reactions usually proceeding through stepwise pathways are different from the classic high-order pericyclic reactions that follow the Woodward-Hoffman rules. More significantly, asymmetric high-order dipolar annulations using chiral organometallic catalysts have been proven successful for constructing chiral medium-sized heterocycles with high enantio- and diastereoselectivity. This review highlights the impressive advances in this area and is focused on the reactivity, scope, mechanisms and applications of high-order dipolar annulation reactions. © 2022 The Royal Society of Chemistry

语种： 英文

作者： Yang, Lei;Zhang, Fan;Chen, Chunxiu;Liu, Zhisheng;Liu, Lu;...

期刊： CHEMISTRY-AN ASIAN JOURNAL,2022年17(14):e202200455- ISSN：1861-4728

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

作者机构： [Chen, Chunxiu; Yang, Lei; Liu, Zhisheng; Li, Haibing; Liu, Lu] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Minist Educ, Wuhan 430079, Peoples R China.;[Zhang, Fan] Hubei Univ, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Coll Chem & Chem Engn, Minist Educ,Key Lab Synth & Applicat Organ Funct, Wuhan 430062, Peoples R China.

通讯机构： [Prof. 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

关键词： BSA;host-guest.;light-responsive;pillararene;protein transport

摘要： Protein transport is an interesting and intrinsic life feature that is highly relevant to physiology and disease in living beings. Herein, inspired by nature, based on the supramolecular host-guest interaction, we have introduced the classical azobenzene light switches and L-phenylalanine derived pillar[6]arene (L-Phe-P6) into the artificial nanochannel to construct light-responsive nanochannels that could regulate protein transport effectively under the control of ultraviolet (UV) and visible (Vis) light. The light-controlled distribution of L-Phe-P6 in the channel led to the difference in surface charges in the nanochannel, which eventually brought the difference in protein transport. This research may not only provide a convenient theoretical model for biological research, but also a flexible light-responsive protein transport model, which will play a crucial role in light-controlled release of protein drugs and so on. © 2022 Wiley-VCH GmbH.

语种： 英文

作者： Li, Dan;Meng, Ying;Hao, Dapeng;Ding, Qianzhao;Pang, Lei;...

期刊： Chemical Engineering Journal,2022年446:136779 ISSN：1385-8947

通讯作者： Yu, Jihong(jihong@jlu.edu.cn)

作者机构： [Li, Dan; Meng, Ying; Li, Tao; Ding, Qianzhao] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Minist Educ, Key Lab Mat Chem Energy Convers & Storage,Hubei Ke, Wuhan 430074, Peoples R China.;[Yang, Guoju; Yu, Jihong; Hao, Dapeng] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China.;[Pang, Lei] Dongfeng Trucks R&D Ctr, Wuhan 430056, Peoples R China.;[Guo, Yanbing] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Yu, Jihong; Hao, Dapeng] Jilin Univ, Int Ctr Future Sci, Changchun 130012, Peoples R China.

通讯机构： [Jihong Yu] S;[Tao Li] K;Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, PR China<&wdkj&>State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China<&wdkj&>International Center of Future Science, Jilin University, Changchun 130012, PR China

关键词： Cold-start application;Hydrothermal aging;Passive NOx adsorber (PNA);Pd/SSZ-13;Phosphorus poisoning

摘要： Phosphorus is one of the typical derivatives that cause irreversible deactivation of passive NOx adsorber (PNA). In this work, the deactivation effects of phosphorus on Pd/SSZ-13 were investigated in combination with hydrothermal aging treatment to gain deeper insights into phosphorus-induced deactivation. It was found that phosphorus decreased the porosity and acidity of Pd/SSZ-13 and the deactivation behavior mainly resulted from the decrease of active sites. Specifically, the isolated Pd sites (Pd2+ and [Pd(OH)]+) were poisoned by phosphorus species, leading to the transformation of isolated Pd sites to bulk PdO. After hydrothermal aging treatment, the phosphorus induced the extensive formation of AlPO4 that significantly accelerated the dealumination of zeolite framework, thus resulting in the decrease in activity and stability. Our work sheds light on the deactivation mechanism of Pd/SSZ-13 from the perspectives of phosphorus poisoning and hydrothermal aging, expecting to provide guidance on the design of Pd-based zeolites with high tolerance and high stability for cold-start application. © 2022 Elsevier B.V.

语种： 英文

作者： Wang, Peng-Zi;Liang, Yu-Jie;Wu, Xue;Guan, Wei;Xiao, Wen-Jing;...

期刊： ACS CATALYSIS,2022年12(17):10925-10937 ISSN：2155-5435

通讯作者： Xiao, Wen-Jing(wxiao@mail.ccnu.edu.cn);Chen, Jia-Rong(chenjiarong@mail.ccnu.edu.cn);Guan, Wei(guanw580@nenu.edu.cn)

作者机构： [Wu, Xue; Xiao, Wen-Jing; Chen, Jia-Rong; Wang, Peng-Zi] Cent China Normal Univ, Coll Chem, CCNU uOttawa Joint Res Ctr, Key Lab Pesticides & Chem Biol,Minist Educ, Wuhan 430079, Hubei, Peoples R China.;[Liang, Yu-Jie; Guan, Wei] Northeast Normal Univ, Inst Funct Mat Chem, Fac Chem, Changchun 130024, Peoples R China.;[Xiao, Wen-Jing] Lanzhou Univ, State Key Lab Appl Organ Chem, Lanzhou 730000, Peoples R China.;[Chen, Jia-Rong] Henan Normal Univ, Sch Chem & Chem Engn, Xinxiang 453007, Henan, Peoples R China.

通讯机构： [Wei Guan] I;[Wen-Jing Xiao; Jia-Rong Chen] C;CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticides & Chemical Biology Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, China<&wdkj&>State Key Laboratory of Applied Organic Chemistry, Lanzhou University, Lanzhou 730000, P. R. China<&wdkj&>CCNU-uOttawa Joint Research Centre, Key Laboratory of Pesticides & Chemical Biology Ministry of Education, College of Chemistry, Central China Normal University, 152 Luoyu Road, Wuhan, Hubei 430079, China<&wdkj&>School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, Henan 453007, China<&wdkj&>Institute of Functional Material Chemistry, Faculty of Chemistry, Northeast Normal University, Changchun 130024, P. R. China

关键词： photocatalysis;copper catalysis;C-O coupling;alkene carbo-esterfication;photo-ATRA-type reaction

摘要： Atom transfer radical addition (ATRA) reaction of alkenes has had a significant impact on the field of radical difunctionalization of alkenes. Particularly, in the three-component photo-ATRA-type processes, a rich chemical space and structural diversity could be achieved by smart combination of redox-active radical precursors and the third coupling components (e.g., halides, C-, N-, and O-nucleophiles) under mild conditions. However, the inherent complicated mechanisms involving radical chain or outer-sphere SET of the incipient radical intermediates have led to a dearth of general catalytic methods for highly enantioselective variants, especially those regarding asymmetric intermolecular C-O bond formation. Here, we report a visible-light-induced copper-catalyzed asymmetric three-component photo-ATRA-type reaction of alkenes with oxime esters and carboxylic acids. In this process, a highly enantioselective intermolecular C-O cross-coupling between incipient sp3-hybridized carbon radicals and carboxylic acids was enabled by the formation of an aryl π-bond-engaged [σ + π]-copper complex. This working hypothesis renders naphthyl or extended conjugation of alkenes to be suitable substrates and allows good stereocontrol. This three-component photo-ATRA-type reaction exhibits broad substrate scope and high functional group tolerance with respect to each component, giving the desired cross-coupling products with generally good yields and enantioselectivity (>70 examples; up to 97% ee). Preliminary experimental and computational studies are also performed to gain insight into the mechanism and stereoregulatory elements. This finding provides a promising platform for the development of other enantioselective benzylic-type radical-based cross-coupling reactions. © 2022 American Chemical Society.

语种： 英文

作者： Zhang, Hanjie;Li, Linghan;Chen, Na;Ben, Haijie;Zhan, Guangming;...

期刊： Applied Catalysis B: Environmental,2022年312:121410 ISSN：0926-3373

通讯作者： Sun, Hongwei(sunhw@ccnu.edu.cn)

作者机构： [Li, Qin; Zhang, Hanjie; Li, Linghan] South Cent Univ Nationalities, Sch Chem & Mat Sci, Wuhan 430074, Peoples R China.;[Zhang, Lizhi; Ben, Haijie; Sun, Hongwei; Chen, Na; Zhan, Guangming] Cent China Normal Univ, Inst Environm & Appl Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.;[Sun, Jie] South Cent Univ Nationalities, Coll Resources & Environm Sci, Wuhan 430074, Peoples R China.

通讯机构： [Hongwei Sun; Lizhi Zhang] K;Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, PR China

关键词： Antibiotic removal;Ferric phosphate;Heterogeneous-homogeneous coupled Fenton;Hydroxylamine;Iron cycle

摘要： Heterogeneous-homogeneous coupled Fenton (HHCF) processes compromise the merits of rapid degradation and catalyst reusability, thus are very attractive for environmental remediation and water treatment. However, the development of HHCF processes suffers from the lack of desirable catalysts and Fe(III)/Fe(II) redox cycle (iron cycle) mediators. Herein we demonstrate the combination of hydrogen peroxide, ferric phosphate and hydroxylamine offers a promising HHCF process, where ferric phosphate and hydroxylamine serve as the catalyst and iron cycle mediator, respectively. Hydroxylamine can realize suitable iron release from ferric phosphate, effective iron cycle, and •OH consumption, resulting in efficient conversion of H2O2 to •OH for sulfamethazine removal. More importantly, the phosphorus release from ferric phosphate and nitrogen residual during this HHCF process are limited to reduce the risk of secondary pollution. This study clarifies the importance of iron dissolution and iron cycle on highly efficient Fenton processes, and also provides a promising antibiotic pollutant removal strategy. © 2022 Elsevier B.V.

语种： 英文

作者： Li, Ziyong;Chen, Si;Huang, Yurou;Zhou, Hui;Yang, Shuren;...

期刊： Chemical Engineering Journal,2022年450:138087 ISSN：1385-8947

通讯作者： Guo, Hui(guohui0319@nankai.edu.cn)

作者机构： [Li, Ziyong; Guo, Hui; Chen, Si; Wang, Mingxing; Zhou, Hui; Zhang, Haining; Yang, Shuren] Luoyang Normal Univ, Coll Food & Drug, Coll Chem & Chem Engn, Luoyang Key Lab Organ Funct Mol, Luoyang 471934, Peoples R China.;[Huang, Yurou; Yin, Jun] Cent China Normal Univ, Minist Educ,Coll Chem,Hubei Int Sci & Technol Coop, Int Joint Res Ctr Intelligent Biosensing Technol &, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China.

通讯机构： [Hui Guo] L;[Jun Yin] K;Luoyang Key Laboratory of Organic Functional Molecules, College of Food and Drug, College of Chemistry and Chemical Engineering, Luoyang Normal University, Luoyang 471934, PR China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, Hubei International Scientific and Technological Cooperation Base of Pesticide and Green Synthesis, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, PR China

关键词： Aggregation-induced emission (AIE);Dithienylethene;Photochromism;Photodynamic therapy (PDT);Photosensitizer;Singlet oxygen

摘要： The photosensitizer system that allows for reversible noninvasive control over singlet oxygen generation (1O2) is in great demand for precise photodynamic therapy (PDT) aimed at reducing non-specific damage to the normal cells or tissues. However, they often suffer from fluorescence quenching and insufficient 1O2 generation due to aggregation-caused quenching (ACQ) phenomenon in a hydrophilic and physiological environment, severely limiting their applications in both imaging and PDT therapy. Herein, a novel positively charged photoswitchable photosensitizer with aggregation-induced emission (AIE) has been rationally designed and successfully developed, in which pyridinium-tetraphenylethylene (Py-TPE) photosensitizing fragment and dithienylethene (DTE) switch unit were covalently linked through a flexible C4 chain enabling efficient intramolecular energy transfer between both functional entities, thus allowing for reversible control of 1O2 generation. Preliminary evaluation of the photophysical properties revealed excellent AIE properties and photoswitching behavior in various solvents. Furthermore, the nanoparticles (NPs) fabricated by the amphiphilic Pluronic F127 exhibited excellent photochromic performance in the aqueous medium. Significantly, 1O2 generation in the closed NPs was suppressed by the competitive energy transfer, while the generation of 1O2 in the open NPs was activated upon light irradiation, demonstrating its reversible control over 1O2 generation under irradiation with 420 nm light. As expected, it has been proved to perform well in specific bacterial discrimination and photocontrolled antimicrobial PDT against Staphylococcus aureus (S. aureus) in vitro. © 2022 Elsevier B.V.

语种： 英文