通讯机构:
[Shi-Yu Liu; Quan Gong] C;Clinical Molecular Immunology Center, School of Medicine, Yangtze University, Jingzhou, China, Jingzhou, Hubei 434023, PR China<&wdkj&>Department of Laboratory Medicine, School of Medicine, Yangtze University, Jingzhou, Hubei 434023, PR China
摘要:
Peroxynitrite (ONOO-) plays important roles in the progression of important disease such as inflammation, cancer, and diabetes, which made it an attractable target for biosensor development. However, to detect ONOO- solely is highly dependent on the sensitivity of the detection method and may be disturbed by unwillingly false-positive signal. Cellular viscosity is an important microenvironmental parameter and its abnormal changes are closely related to diseases such as diabetes and cancer. In this case, to construct a "dual-locked " molecular tool for both ONOO- and viscosity sensing and to evaluate the performance such strategy in disease diagnosis is of great importance. We herein firstly reported the construction of novel "dual-locked " probe DCI-OV which showed capability for simultaneous measuring ONOO- concentration and system viscosity with high sensitivity (LOD = 4.7 nM) and high specificity. Moreover, both exogenous and low level of endogenous ONOO- in living cells could be detected using DCI-OV due to viscosity amplified signal. Furthermore, cancer cells and insulin-resistant cells could be easily distinguished using DCI-OV. By taking advantage of the "dual-locked " sensing strategy, a total of 85 samples of human serum were screened using DCI-OV based rapid disease screening method and it was capable of differentiated and subdivided patients into specific type of disease, indicating the great potential of application of DCI-OV into clinical related disease diagnosis. (C) 2022 Elsevier B.V. All rights reserved.
通讯机构:
[An-Xin Wu] K;[Zhi-Xin Liao] D;Department of Pharmaceutical Engineering, School of Chemistry and Chemical Engineering and Jiangsu Province Hi-Tech Key Laboratory for Biomedical Research, Southeast University, Nanjing 211189, China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
摘要:
Precise control of the chemoselectivity of the halogenation of a substrate equipped with multiple nucleophilic sites is highly demanding and challenging. Most reported chlorinations of methyl ketones show poor compatibility or even exclusive selectivity toward electron-rich arene, olefin, and alkyne residues. This is attributed to the direct or in situ employment of electrophilic Cl2/Cl+ species. Here, we reported that, even bearing those competitive residues, methyl ketones can still undergo dichlorination to afford α,α-dichloroketones in a chemo-specific manner. Enabled by the I2-dimethyl sulfoxide catalytic system, in which hydrochloric acid only acts as a nucleophilic Cl– donor, this straightforward dichlorination reaction is safe and operator-friendly and has high atomic economy, giving access to structurally diverse α,α-dichloroketones in good yields and with good functional-group tolerance.
摘要:
As a colorless, highly toxic and widely used chemical reagent, phosgene poses a potentially serious threat to public health and environmental safety. Therefore, there is an urgent need to develop a simple and sen-sitive method for detecting phosgene. In this work, a ratiometric fluorescent probe (NED) for phosgene was developed by utilizing 4-substituted 1,8-naphthimide unit as the fluorophore and ethylenediamine as the recognition moiety. The probe NED undergoes intramolecular cyclization reaction with phosgene, resulting in a remarkable ratiometric fluorescence response. The probe NED displays high sensitivity (LOD = 4.9 nM), excellent ratiometric fluorescence signal, and high selectivity toward phosgene over other relevant analytes. In addition, paper test strip capable of visually detecting gaseous phosgene has also been fabricated. (c) 2021 Elsevier B.V. All rights reserved.
期刊:
Journal of Chromatography A,2022年1678:463322 ISSN:0021-9673
通讯作者:
Jing Cheng
作者机构:
[Li, Aimin] Hubei Ecol Environm Monitoring Ctr, Wuhan, Peoples R China.;[Huang, Xiaolan; Yan, Ling; Li, Aimin; Cheng, Jing] Cent China Normal Univ, Inst Environm Chem, Coll Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Jing Cheng] K;Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, Institute of Environmental Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, China
摘要:
2,4,6-trihalorophenol disinfection by-products (DBPs) have strong toxicity to be needed for monitoring. In this study, two kind of molecularly imprinted polymeric fibers were prepared using 2,4,6-trichlorophenol as template and tricuronic phloroglucinol (MOP) as pseudo-template, respectively. The two fibers were assembled as solid phase microextraction (SPME) fiber to extract 2,4,6-trihalophenol DBPs from water and detect them by gas chromatography coupled to electron capture detector (GC-ECD). The results of F-test and t-test stated that there are significant difference in the analytical results of 2,4,6-trichlorophenol between using the fiber based on 2, 4, 6-trichlorophenol as template and MOP as pseudo-template. It was found that the carry-over of template (2,4,6-trichlorophenol) leaked from the fiber in GC thermal desorption, resulting in the wrong quantitative analytical result for 2,4,6-trichlorophenol in water. Hence, molecularly imprinted polymeric fibers based on MOP as pseudo-template was applied for the determination of 2,4,6-trihalophenol DBPs in water combined with GC-ECD. The selectivity of the fiber for 2,4,6-trihalophenol DBPs was investigated and demonstrated. Under the optimized condition, the method has much lower limit of detection (0.5-1.1 pg mL(-1)) than most reported methods. The method was applied for the determination of 2,4,6-trihalophenol DBPs in environmental water and the relative recoveries were found to be in the range from 77.1% to 105.6% and the relative standard deviation was 0.5-9.4%. 2,4,6-tribromophenol was found at concentration of 0.054 ng mL(-1) in a swimming pool. (C) 2022 Elsevier B.V. All rights reserved.
期刊:
Drug Discovery Today,2022年27(8):2216-2225 ISSN:1359-6446
通讯作者:
Hao, G.-F.
作者机构:
[Chen, Yi; Song, Bao-An; Hao, Ge-Fei] Guizhou Univ, Ctr Res & Dev Fine Chem, State Key Lab Breeding Base Green Pesticide & Agr, Key Lab Green Pesticide & Agr Bioengn,Minist Educ, Guiyang 550025, Peoples R China.;[Wang, Zhi-Zheng] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan, Peoples R China.
通讯机构:
[Hao, G.-F.] S;State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Center for Research and Development of Fine Chemicals, Guizhou University, Guiyang, China
通讯机构:
[An-Xin Wu] K;Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
摘要:
Pd-catalyzed cascade hydroarylation and C-H germylation of nonterminal alkenes and aryl iodides enabled by hydroxyl assistance have been developed. The key step in this C-H germylation cascade is the formation of a highly reactive oxo-palladacycle intermediate, which markedly restrained the beta-H elimination process. Mechanistically, control experiments indicated that the hydroxyl group played an important role in this process. This transformation shows excellent reactivity and selectivity for most substrates investigated.
作者机构:
[Liu, Bing; Li, Xun; Yang, Hanmin; Nie, Jiabao; Yuan, Ziliang] South Cent Minzu Univ, Key Lab Catalysis & Energy Mat Chem, Minist Educ, Wuhan 430074, Peoples R China.;[Wang, Guanghui; Yuan, Ziliang] Wuhan Univ Sci & Technol, Coll Chem Engn & Technol, Hubei Coal Convers & New Carbon Mat Key Lab, Wuhan 430081, Peoples R China.;[Liu, Yi] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Prof. Hanmin Yang; Prof. Bing Liu; Prof. Hanmin Yang Prof. Hanmin Yang Prof. Hanmin Yang; Prof. Bing Liu Prof. Bing Liu Prof. Bing Liu] K;Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education, South-Central Minzu University, Wuhan, 430074 P. R. China
期刊:
Biosensors and Bioelectronics,2022年213:114484 ISSN:0956-5663
通讯作者:
Li, C.;Liu, Z.
作者机构:
[Zhai, Shuyang; Liu, Zhihong] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Peoples R China.;[Chai, Li; Li, Chunya; Hu, Wei; An, Qian] South Cent Univ Nationalities, Coll Chem & Mat Sci, Key Lab Analyt Chem State Ethn Affairs Commiss, Wuhan 430074, Peoples R China.;[Wang, Weibo] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Coll Chem, Minist Educ, Wuhan 430079, Peoples R China.
通讯机构:
[Chunya Li] K;[Zhihong Liu] C;College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, China<&wdkj&>Key Laboratory of Analytical Chemistry of the State Ethnic Affairs Commission, College of Chemistry and Material Science, South-central University for Nationalities, Wuhan, 430074, China
关键词:
Ratiometric autophagy probes;Lysosomal viscosity;Two-photon confocal imaging;Through bond energy transfer;Inflammation and stroke
摘要:
Autophagy is a self-degradation process in cells, which is of vital significance to the health and operation of organisms. Due to the increase of lysosomal viscosity during autophagy, viscosity probes that specifically accumulate in lysosome are powerful tools for monitoring autophagy and investigating related diseases. However, there is still a lack of viscosity-sensitive ratiometric autophagy probes, which restricts the tracking of autophagy with high accuracy in complex physiological environment. Herein, a viscosity-responsive, lysosome targeted two-photon fluorescent probe Lyso-Vis was designed based on through bond energy transfer (TBET) mechanism. The TBET-based probe achieved the separation of two emission baselines, which greatly improved the resolution and reliability of sensing and imaging. Under 810 nm two-photon excitation, the emission intensity ratio of the red and green channel increased with a viscosity dependent manner. Lyso-Vis not only for the first time realized ratiometric sensing of lysosomal viscosity during autophagy process, but also visualized the association of autophagy with inflammation and stroke, and it was applied to explore the activation and inhibition of autophagy during stroke in mice.
期刊:
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY,2022年70(22):6617-6623 ISSN:0021-8561
通讯作者:
Ge-Fei Hao<&wdkj&>Guang-Fu Yang
作者机构:
[Yang, Guang-Fu; Chen, Hui-Min; Mei, Long-Can; Huang, Guang-Yi; Hao, Ge-Fei] Cent China Normal Univ, Key Lab Pesticide & Chem Biol, Minist Educ, Coll Chem, Wuhan 430079, Hubei, Peoples R China.;[Zhang, Xiao; Liu, Ying-Wei; Wang, Wei; Dong, An-Yu; Hao, Ge-Fei] Guizhou Univ, Key Lab Green Pesticide & Agr Bioengn, State Key Lab Breeding Base Green Pesticide & Agr, Minist Educ,Res & Dev Ctr Fine Chem, Guiyang 550000, Guizhou, 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, Hubei 430079, People’s Republic of China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, Hubei 430079, People’s Republic of China<&wdkj&>State Key Laboratory Breeding Base of Green Pesticide and Agricultural Bioengineering, Key Laboratory of Green Pesticide and Agricultural Bioengineering, Ministry of Education, Research and Development Center for Fine Chemicals, Guizhou University, Guiyang, Guizhou 550000, People’s Republic of China
摘要:
Pesticides are widely used agrochemicals for crop protection. The need for novel pesticides becomes urgent as a result of the emergence of resistance and environmental toxicity. Pesticide informatics has been applied in different phase processes of pesticide target identification, active ingredient design, and impact evaluation. However, these valuable resources are scattered over the literature and web, limiting their availability. Here, we summarize and connect research on pesticide informatics resources. A pesticide informatics platform (PIP) was constructed to share these tools. We finally discuss the future direction of pesticide informatics, including pesticide contamination. We expect to share the pesticide informatics approaches and stimulate further research.
作者机构:
[Chao, Hui; Ouyang, Cheng; Lin, Xinlin; Ji, Liangnian; Xiong, Kai; Chen, Yu; Chen, Xiang] Sun Yat Sen Univ, Affiliated Hosp 7, MOE Key Lab Bioinorgan & Synthet Chem, Sch Chem,Guangdong Prov Key Lab Digest Canc Res, Guangzhou 510006, Peoples R China.;[Liu, Jiaqi; Wan, Jian] Cent China Normal Univ, Coll Chem, Wuhan 430079, Peoples R China.;[Karges, Johannes] Univ Calif San Diego, Dept Chem & Biochem, 9500 Gilman Dr, La Jolla, CA 92093 USA.;[Chao, Hui] Hunan Univ Sci & Technol, Sch Chem & Chem Engn, MOE Key Lab Theoret Organ Chem & Funct Mol, Xiangtan 400201, Peoples R China.
通讯机构:
[Dr. Yu Chen; Prof. Dr. Hui Chao] M;[Prof. Dr. Jian Wan] C;College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China<&wdkj&>MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Guangdong Provincial Key Laboratory of Digestive Cancer Research, The Seventh Affiliated Hospital, Sun Yat-Sen University, Guangzhou, 510006 P. R. China<&wdkj&>MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Guangdong Provincial Key Laboratory of Digestive Cancer Research, The Seventh Affiliated Hospital, Sun Yat-Sen University, Guangzhou, 510006 P. R. China<&wdkj&>MOE Key Laboratory of Theoretical Organic Chemistry and Functional Molecule, School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan, 400201 P. R. China
关键词:
Bioinorganic Chemistry;G-Quadruplexes;Metals in Medicine;Platinum;Ruthenium
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, P. R. China<&wdkj&>School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China<&wdkj&>Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China
关键词:
Cu recovery;decomplexation;electro-Fenton;heavy metal−organic complexes;sodium tetrapolyphosphate electrolyte
作者机构:
[Zhang, Siyun; Li, Haibing] Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan;430079, China;College of Chemical Engineering, North China University of Science and Technology, Tangshan;063210, China;[Zhou, Juan] State Key Laboratory of Virology, Wuhan Institute of Virology, Center for Biosafety Mega-Science, Chinese Academy of Sciences, Wuhan
通讯机构:
[Prof. Juan Zhou] S;[Prof. Haibing Li] K;Key Laboratory of Pesticide and Chemical Biology, Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China<&wdkj&>State Key Laboratory of Virology, Wuhan Institute of Virology, Center for Biosafety Mega-Science, Chinese Academy of Sciences, Wuhan, 430071 P. R. China
作者机构:
[Qu, Yanjuan; Hu, Hao] Wuhan Univ, Zhongnan Hosp, Dept Radiol, 169 East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Hu, Heng] Huazhong Univ Sci & Technol, Tongji Med Coll, Liyuan Hosp, Dept Resp & Crit Care Med, East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Lu, Zhiyan; Liu, Zhuo; Lu, Minxiang] Wuhan Univ, Zhongnan Hosp, Dept Forens Med, 169 East Lake Rd, Wuhan 430071, Hubei, Peoples R China.;[Liang, Feng] Wuhan Univ Sci & Technol, Sch Chem & Chem Engn, Wuhan 430065, Hubei, Peoples R China.;[Li, Guang; Li, Haibing] Cent China Normal Univ, Minist Educ, Coll Chem, Key Lab Pesticide & Chem Biol CCNU, Wuhan 430079, Hubei, Peoples R China.
通讯机构:
[Yanjuan Qu; Minxiang Lu] D;[Feng Liang] S;[Haibing Li] K;Department of Radiology, Zhongnan Hospital of Wuhan University, Wuhan, People’s Republic of China<&wdkj&>Department of Forensic Medicine, Zhongnan Hospital of Wuhan University, Wuhan, People’s Republic of China<&wdkj&>School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, People’s Republic of China<&wdkj&>Key Laboratory of Pesticide and Chemical Biology (CCNU), Ministry of Education, College of Chemistry, Central China Normal University, Wuhan, People’s Republic of China
作者机构:
[Chen, Weijie; Chen, Huijuan; Huang, Yurou; Yin, Jun] 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, China;[Tan, Ying; Tan, Chunyan] State Key Laboratory of Chemical Oncogenomics, Key Laboratory of Chemical Biology, Shenzhen International Graduate School, Tsinghua University, Guangdong, Shenzhen;518055, China;[Xie, Yuan] Guangdong Provincial Key Laboratory of Radioactive and Rare Resource Utilization, Shaoguan
通讯机构:
[Ying Tan; Chunyan Tan] S;[Jun Yin] K;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, P. R. China<&wdkj&>State Key Laboratory of Chemical Oncogenomics, Key Laboratory of Chemical Biology, Shenzhen International Graduate School, Tsinghua University, Shenzhen, Guangdong 518055, P. R. China
作者机构:
[Liu, Lijuan; Zhang, Lizhi; Gong, Jingming; Yao, Qingfeng; Sun, Hongwei; Hu, Yachen; Li, Xin] 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.
通讯机构:
[Jingming Gong] K;Key Laboratory of Pesticide and Chemical Biology of the Ministry of Education, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, People’s Republic of China
摘要:
A smart temperature stimuli-driven multiplex photoelectrochemical (PEC) assay was constructed for antibiotic resistance genes (ARGs) detection, where the stimuli-responsive gatekeeping by regulating the alternative release of "cargo" allowed for the simultaneous detection of multiple tetracycline resistance gene, using tetA (T(DNA1)) and tetC (T(DNA2)) as the model. Dual temperature-responsive nanoassemblies were embedded in the PEC bioassay as signal DNA tages: one thermoresponsive polymer (poly(N-isopropylacrylamide), PNIPAM)-capped mesoporous silica nanoparticles (MSN) with loading the "cargo" of HgO nanoparticles as signal DNA1 tags (S(DNA1)-PNIPAM@MSN@HgONPs) and the other antimony tartrate (SbT)-anchored silica nanospheres as signal DNA2 tags (S(DNA2)-SbT@SiO(2)NSs). At 20 °C, below the lower critical solution temperature (LCST) of PNIPAM, the "gatekeeper" PNIPAM in S(DNA1)-PNIPAM@MSN@HgONPs was in an ON state, igniting Hg(2+) release through the pore of SiO(2). While at above LCST (40 °C), it was in an OFF state. Likewise, the thermo-dependent dissociation of SbT endowed the grafted S(DNA2) tags switching from the OFF (at 20 °C) to ON state (at 40 °C), igniting SbO(+) release. The released Hg(2+) and SbO(+) triggered the amplified photocurrents due to the structure evolution of the photoactive layer into HgS/ZnS or Sb(2)S(3)/ZnS heterostructure, thus achieving sensitive detection of multiple ARGs: tetA, tetC, tetG, tetM, tetO, tetZ, tetX, and tetW. Combined with heat map analysis, rapid screening of the ARGs profiles in 12 samples could be realized. This bioassay is simple and accessible for multiple genes analysis with the detection limit down to 0.50 nM. And it was successfully applied for measuring tetracycline ARGs in real sludge samples.
通讯机构:
[Jingming Gong] 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:
Hydrated electron;Integrated oxidation and reduction;Nitrate;Perfluorooctanoic acid;Reactive nitrogen species
摘要:
The environmental persistence, high toxicity and wide spread presence of perfluorooctanoic acid (PFOA) in aquatic environment urgently necessitate the development of advanced technologies to eliminate PFOA. Here, the simultaneous application of a heterogeneous In(2)O(3) photocatalyst and homogeneous persulfate oxidation (In(2)O(3)/PS) was demonstrated for PFOA degradation under solar light irradiation. The synergistic effect of direct hole oxidation and in-situ generated radicals, especially surface radicals, was found to contribute significantly to PFOA defluorination. Fourier infrared transform (FTIR) spectroscopy, Raman, electrochemical scanning microscope (SECM) tests and density functional theory (DFT) calculation showed that the pre-adsorption of PFOA and PS onto In(2)O(3) surface were dramatically critical steps, which could efficiently facilitate the direct hole oxidation of PFOA, and boost PS activation to yield high surface-confined radicals, thus prompting PFOA degradation. Response surface methodology (RSM) was applied to regulate the operation parameters for PFOA defluorination. Outstanding PFOA decomposition (98.6%) and near-stoichiometric equivalents of fluorides release were achieved within illumination 10h. An underlying mechanism for PFOA destruction was proposed via a stepwise losing CF(2) unit. The In(2)O(3)/PS remediation system under solar light provides an economical, sustainable and environmentally friendly approach for complete mineralization of PFOA, displaying a promising potential for treatment of PFOA-containing water.
通讯作者:
Hong Yuan<&wdkj&>Bien Tan<&wdkj&>Jingyu Wang
作者机构:
[Wang, Jingyu; Li, Tao; Cai, Zhongjie; Hu, Xiantao; Li, Zhong'an; He, Huijie; Tan, Bien] Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Hubei Key Lab Mat Chem & Serv Failure, Key Lab Mat Chem Energy Convers & Storage,Minist E, Wuhan 430074, Peoples R China.;[Yuan, Hong] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Zhang, Yanrong] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China.
通讯机构:
[Hong Yuan; Bien Tan; Jingyu Wang] K;Key Laboratory of Pesticide & Chemical Biology (Ministry of Education), College of Chemistry, Central China Normal University, Wuhan 430079, China<&wdkj&>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, China
摘要:
Solar-driven photocatalysis offers an environmentally friendly and sustainable approach for the degradation of organic pollutants in water without chemical additives, but the low specific surface area and adsorption capacity of common photocatalysts restricts the surface reactions with the contaminants. Herein, we hypercrosslinked polymer layers on TiO2-graphene surface to enlarge the specific surface area from 136 to 988 m2/g, leading to a high adsorption capacity of sulfadiazine as 54.3 mg/g, which is 15.5 times that of TiO2-graphene (3.5 mg/g). The adsorption kinetics reveals the combination of physical and chemical adsorption by porous benzene-based polymer for sulfadiazine enrichment. Besides, the polymer layers with broad light absorption enable the composite to function efficiently as visible-light-driven photocatalysts. Thus, the as-designed composite exhibits excellent performance for sulfadiazine removal by integrating the adsorptive and photocatalytic processes, especially for the diluted sulfadiazine solution. More importantly, the porous polymer layer can function as a filter for weakening the interference of TiO2 surface with the natural matters from complex water matrices. Based on the identification of dominant reactive species, the possible attacking pathway and the sulfadiazine subsequent degradation are presented. Further, the enhanced adsorption and photodegradation efficiency can also be achieved for the removal of other typical pollutants such as 4-chlorophenol and methylene blue. This study highlights an adsorption-enhanced-degradation mechanism for water pollutants that can direct the design of high-performance photocatalysts under visible light.