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Preparation of porous semi-IPN temperature-sensitive hydrogel-supported nZVI and its application in the reduction of nitrophenol

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Journal of Environmental Sciences 2019年第8期31卷 93-102页

作者： Lixia Li Ruiwei Wang Xiaodong Xing Wenqiang Qu Shutong Chen Yunlong Zhang School of Environment and safety engineering Jiangsu University School of Chemical Engineering Nanjing University of Science and Technology

Nanoscale zero-valent iron(n ZVI) particles supported on a porous, semi-interpenetrating(semi-IPN), temperature-sensitive composite hydrogel(PNIPAm-PHEMA). n ZVI@PNIPAmPHEMA, was successfully synthesized and characterized by FT-IR, SEM, EDS, XRD and the weighing method. The loading of nZVI was 0.1548 ± 0.0015 g/g and the particle size was30–100 nm. NZVI was uniformly dispersed on the pore walls inside the PNIPAm-PHEMA.Because of the well-dispersed n ZVI, the highly porous structure, and the synergistic effect of PNIPAm-PHEMA, nZVI@PNIPAm-PHEMA showed excellent reductive activity and wide p H applicability. 95% of 4-NP in 100 m L of 400 mg/L 4-NP solution with initial p H 3.0–9.0 could be completely reduced into 4-AP by about 0.0548 g of fresh supported n ZVI at 18–25 °C under stirring(110 r/min) within 45 min reaction time. A greater than 99% 4-NP degradation ratio was obtained when the initial p H was 5.0–9.0. The reduction of 4-NP by nZVI@PNIPAm-PHEMA was in agreement with the pseudo-first-order kinetics model with Kobsvalues of 0.0885–0.101 min-1.NZVI@PNIPAm-PHEMA was able to be recycled, and about 85% degradation ratio of 4-NP was obtained after its sixth reuse cycle. According to the temperature sensitivity of PNIPAmPHEMA, n ZVI@PNIPAm-PHEMA exhibited very good storage stability, and about 88.9%degradation ratio of 4-NP was obtained after its storage for 30 days. The hybrid reducer was highly efficient for the reduction of 2-NP, 3-NP, 2-chloro-4-nitrophenol and 2-chloro-4-nitrophenol. Our results suggest that PNIPAm-PHEMA could be a good potential carrier, with n ZVI@PNIPAm-PHEMA having potential value in the application of reductive degradation of nitrophenol pollutants.

关键词： Porous semi-IPN temperature sensitive hydrogel Supported nanoscale zero-valent iron Reductive degradation nitrophenol Storage stability

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Covalent organic hollow nanospheres constructed by using AIEactive units for nitrophenol explosives detection

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Science China Chemistry 2020年第4期63卷 497-503页

作者： Shan Jiang Shengda Liu Lingchen Meng Qingkai Qi Lipeng Wang Bin Xu Junqiu Liu Wenjing Tian State Key Laboratory of Supramolecular Structure and Materials Jilin UniversityChangchun 130000China

The development of conjugated nanomaterials with high sensitivity and super-amplified quenching effect for the detection of nitrophenol explosives is still a great challenge. Herein, we developed conjugated hollow nanospheres constructed by using aggregation-induced emission(AIE) active 1,3,5-tris(4-formyl-phenyl)benzene(TFPB). The high emission hollow nanospheres with uniform size and admirable dispersiveness exhibited obvious fluorescence quenching response with the addition of nitrophenol explosives owing to the photoinduced electron transfer(PET) from the hollow nanospheres to nitrophenol explosives. The Stern-Volmer constants of hollow spheres for 2,4,6-trinitrophenol(TNP), 4-nitrophenol(NP) and 2,4-dinitrophenol(DNP) can reach 9.67×10^5, 3.14×10^5 and 4.8×10^4 M-1, respectively. Furthermore, the handy test paper coated with hollow nanospheres was prepared and showed a good response toward TNP solutions and vapor. The study provides a novel strategy to construct AIE-active conjugated hollow nanospheres for efficient nitrophenol explosives sensing.

关键词： aggregation-induced emission covalent organic nanospheres nitrophenol explosives detection fluorescence quenching

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Assembling of a novel 3D Ag(Ⅰ)-MOFs with mixed ligands tactics：Syntheses, crystal structure and catalytic degradation of nitrophenol

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Chinese Chemical Letters 2018年第6期29卷 845-848页

作者： Dandan Huang Xueqian Wua Junwu Tian Xiaokun Wang Zhihang Zhou Dongsheng Li College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion Materials Hubei Provincial Collaborative Innovation Center for New Energy Microgrid China Three Gorges University Yichang 443002 China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China

A silver-based metal-organic framework（Ag-MOFs）, [Ag2（H3 ddcba）（dpp）2]（1）（H5 ddcba = 3,5-（di（2’,5’-dicarboxylphenyl）benozoic acid, dpp = 1,3-di（4-pyridyl）propane）, was successfully constructed via hydrothermal assembly of a pentacaboxylate ligand, a N-donor ligand and Ag（I） ions, which possesses a pcu topology and exhibits excellent catalytic properties in aqueous solution for the degradation of onitrophenol（2-NP）, m-nitrophenol（3-NP） and p-nitrophenol（4-NP）. Related kinetics of such catalytic reactions, photoluminescent and thermal stability of compound 1 were also investigated.

关键词： Ag（Ⅰ） metal organic framework Mixed ligands tactics Crystal structure nitrophenol Catalytic properties

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Estimation of Time to Maximum Rate Under Adiabatic Conditions(TMR_(ad)) Using Kinetic Parameters Derived From DSC-Investigation of Thermal Behavior of 3-Methyl-4-nitrophenol

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化学推进剂与高分子材料 2011年第1期9卷 84-96页

作者： Bertrand Roduit Patrick Folly Alexandre Sarbach Beat Berger Franz Brogli Francesco Mascarello Mischa Schwaninger Thomas Glarner Eberhard Irle Fritz Tobler Jacques Wiss Markus Luginbühl Craig Williams Pierre Reuse Francis Stoessel AKTS AG TechnoArk 13960 SidersSwitzerland Armasuisse Science and Technology Centre3602 ThunSwitzerland Ciba Schweizerhalle AG P.O.Box4002 BaselSwitzerland DSM Nutritional Products Ltd. Safety laboratory4334 SisselnSwitzerland F.Hoffmann-La Roche Ltd Safety laboratories4070 BaselSwitzerland Lonza AG Safety Laboratory VispRottenstr.63930 Visp Switzerland Novartis Pharma AG Novartis CampusWSJ-145.8.544002 BaselSwitzerland Syngenta Crop Protection Münchwilen AG WMU 3120.1.544333 MünchwilenSwitzerland Swiss Safety Institute Schwarzwaldallee 215WRO-1055.5.024002 BaselSwitzerland

Kinetic parameters of the decomposition of hazardous chemicals can be applied for the estimation of their thermal behavior under any temperature profile.Presented paper describes the application of the advanced kinetic approach for the determination of the thermal behavior also under adiabatic conditions occurring e.***.in batch reactors in case of cooling failure.The kinetics of the decomposition of different samples(different manufacturers and batches) of 3-methyl-4-nitrophenol were investigated by conventional DSC in non-isothermal(few heating rates varying from 0.25 to 8.0K/min) and isothermal(range of 200~260℃) modes.The kinetic parameters obtained with AKTS-Thermokinetics Software were applied for calculating reaction rate and progress under different heating rates and temperatures and verified by comparing simulated and experimental signals.After application of the heat balance to compare the amount of heat generated during reaction and its removal from the system,the knowledge of reaction rate at any temperature profiles allowed the determination of the temperature increase due to the self-heating in adiabatic and pseudo-adiabatic conditions.Applied advanced kinetic approach allowed simulation the course of the Heat-Wait-Search(HWS) mode of operation of adiabatic calorimeters.The thermal safety diagram depicting dependence of Time to Maximum Rate(TMR) on the initial temperature was calculated and compared with the results of HWS experiments carried out in the system with Ф-factor amounting to 3.2.The influence of the Ф-factor and reaction progress reached at the end of the HWS monitoring on the TMR is discussed.Presented calculations clearly indicate that even very minor reaction progress reduces the TMRad of 24h characteristic for a sample with initial reaction progress amounting to zero.Described estimation method can be verified by just one HWS-ARC,or by one correctly chosen ISO-ARC run of reasonable duration by knowing in advance the dependence of the TMR on the initial temperature for any Ф-factor.Prop

关键词： adiabatic condition methyl nitrophenol DSC Ф-factor kinetics thermal runaway,TMR

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Metabolism-independent chemotaxis of Pseudomonas sp. strain WBC-3 toward aromatic compounds

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Journal of Environmental Sciences 2008年第10期20卷 1238-1242页

作者： ZHANG, Junjie XIN, Yufeng LIU, Hong WANG, Shujun ZHOU, Ningyi State Key Laboratory of Virology Wuhan Institute of Virology Chinese Academy of Sciences Wuhan 430071 China Graduate School Chinese Academy of Sciences Beijing 100049 China

Pseudomonas sp. strain WBC-3 utilized methyl parathion or para-nitrophenol (PNP) as the sole source of carbon, nitrogen, and energy, and methyl parathion hydrolase had been previously characterized. Its chemotactic behaviors to aromatics were investigated. The results indicated that strain WBC-3 was attracted to multiple aromatic compounds, including metabolizable or transformable substrates PNP, 4-nitrocatechol, and hydroquinone. Disruption of PNP catabolic genes had no e?ect on its chemotactic behaviors w...

关键词： aromatics chemotaxis metabolism-independent methyl parathion nitrophenol Pseudomonas sp. strain WBC-3

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Nitration Reaction Catalyzed by Horseradish Peroxidase in the Presence of H2O2 and NaNO2

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Chinese Journal of Chemistry 2007年第11期25卷 1690-1694页

作者：戴荣继黄辉陈洁邓玉林肖盛元 School of Life Science and Technology Beijing Institute of Technology Beijing .100081 China

The enzymatic nitration of phenol and m-cresol catalyzed by horseradish peroxidase was studied in the presence of H2O2 and NaNO2. The results showed that the nitration products of phenol were 2-nitro and 4-nitrophenols. There was also a small amount of by-products of hydroquinone and catechol. The influences of various reaction parameters, including pH, organic solvent type, and concentrations of NaNO2 and H2O2, on the nitration products were investigated. The yields of 4-nitrophenol and 2-nitrophenol were 14% and 12%, respectively. The nitration products of m-cresol were 4-nitro-m-cresol and 6-nitro-m-cresol, and the yields of 4-nitro-m-cresol and 6-nitro-m-cresol were 19% and 30%, respectively.

关键词： horseradish peroxidase phenol nitrophenol nitration

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Density Functional Theoretical Studies on Effect of Intramolecular Hydrogen Bonds on Reduction of nitrophenols

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Chemical Research in Chinese Universities 2017年第5期33卷 785-793页

作者： ZHANG Hongmei LIU Yan MA Fangping QIU Wei LEI Bo SHEN Jinyou SUN Xiuyun HAN Weiqing LI Jiansheng WANG Lianjun Jiangsu Key Laboratory for Chemical Pollution Control and Resource Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology Nanjing 210094 P. R. China Chuannan Machinery Factory China Aerospace Science and Technology Corporation Luzhou 646000 P. R. China

Intramolecular hydrogen bonds（IMHBs） can lead to different physicochemical characteristics of nitro- phenols（NPs） that determine their environmental behavior. In the present work, to reveal the relationship between IMHB and nitrophenol reduction, the effects of IMHB on the molecular geometries and properties of a series of ni- trophenols were investigated with density functional theory（DFT） calculations. The results of the geometry optimiza- tion and atoms-in-molecules（AIM） analysis indicate relatively strong IMHBs in ortho-substituted nitrophenols, whose stability could be significantly improved. In comparing the ELUMO and adiabatic electron affinities（AEA） of the nitrophenol isomers, the presence of IMHBs benefited the reductive degradation of NPs, consistent with a previous study. To gain an insight into the effect mechanism of IMHBs on the reductive degradation behavior of these mole- cules, the condensed electrophilicity Fukui index（f-）, natural charges and Wiberg bond orders of these nitrophenol isomers were calculated. The calculations indicate that the electrophilic reactivity activity of the O atom on the nitro group could be significantly improved due to the formation of IMHBs, which results in the enhanced reductive degradation of ortho-substituted NPs.

关键词： nitrophenol Reduction Intramolecular hydrogen bond Effect mechanism Density functional theory

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DFT Studies on Detonation Properties, Pyrolysis Mechanism, and Stability of the Nitro and Hydroxyl Derivatives of Benzene

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Chinese Journal of Chemistry 2011年第3期29卷 455-462页

作者： Du, Hongchen Liu, Hui Liu, Yan Zhang, Jianying Wang, Fang Gong, Xuedong Department of Chemistry Nanjing University of Science and Technology Nanjing Jiangsu 210094 China State Key Laboratory of Explosion Science and Technology Beijing Institute of Technology Beijing 100081 China

Ninety-one nitro and hydroxyl derivatives of benzene were studied at the B3LYP/6-31G＊ level of density functional theory. Detonation properties were calculated using the Kamlet-Jacobs equation. Three candidates （pentanitrophenol, pentanitrobenzene, and hexanitrobenzene） were recommended as potential high energy density compounds for their perfect detonation performances and reasonable stability. The pyrolysis mechanism was studied by analyzing the bond dissociation energy （BDE） and the activation energy （Ea） of hydrogen transfer （H--T） reaction for those with adjacent nitro and hydroxyl groups. The results show that Ea is much lower than BDEs of all bonds, so when there are adjacent nitro and hydroxyl groups in a molecule, the stability of the compound will decrease and the pyrolysis will be initiated by the H--T process. Otherwise, the pyrolysis will start from the breaking of the weakest C--NO2 bond, and only under such condition, the Mulliken population or BDE of the C--NO2 bond can be used to assess the relative stability of the compound.

关键词： high energy density material nitrobenzene nitrophenol density functional theory

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Nitration of Phenol Catalyzed by Horseradish Peroxidase

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Journal of Beijing Institute of Technology 2007年第2期16卷 217-219页

作者：戴荣继黄辉佟斌肖盛元 School of Life Science and Technology Beijing Institute of Technology School of Materials Science and Engineering Beijing Institute of Technology

Horseradish peroxidase, an acidic peroxidase from the horseradish, is one of the most important enzymes as analytical reagent. The enzymatic nitration of phenol by oxidation of nitrite was studied using horseradish peroxidase in the presence of H2O2. The results showed that nitration occur at 2- and 4- positions of phenol. There were also minor products of hydroquinone and catechol. The influence of various reaction parameters, including pH, organic solvent, and concentration of H2O2, on nitration products were discussed. The best nitration pH was 7.0, and H2O2 should be added to the reaction mixture slowly.

关键词： horseradish peroxidase phenol nitrophenol nitrite

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Tunable synthesis solid or hollow Au–Ag nanostructure,assembled with GO and comparative study of their catalytic properties

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Science Bulletin 2016年第19期61卷 1525-1535,1470页

作者：许丽丹洪敏王勇亮李明李海波 Madhavan P.N.Nair 李晨钟 School of Chemistry and Chemical Engineering Liaocheng University Department of Immunology Herbert Wertheim College of Medicine Florida International University Nanobioengineering/Bioelectronics Laboratory Department of Biomedical Engineering Florida International University

介绍了一种简单有效的制备银核金壳核壳纳米粒子(Ag@Au NPs)和银/金中空纳米笼(Ag/Au NCs)的合成方法.该方法分为两步:首先合成银纳米粒子(Ag NPs),然后以该银纳米粒子为种子,通过调整溶液的p H,实现上述两种纳米材料的可控合成.之后基... 详细信息

介绍了一种简单有效的制备银核金壳核壳纳米粒子(Ag@Au NPs)和银/金中空纳米笼(Ag/Au NCs)的合成方法.该方法分为两步:首先合成银纳米粒子(Ag NPs),然后以该银纳米粒子为种子,通过调整溶液的p H,实现上述两种纳米材料的可控合成.之后基于自组装的方法制备得到了银金核壳纳米粒子-氧化石墨烯纳米复合物(Ag@Au NPs-GO)及银/金中空纳米笼-氧化石墨烯纳米复合物(Ag/Au NCs-GO).研究发现,利用静电自组装的方法,Ag/Au NCs比Ag@Au NPs更容易组装到氧化石墨烯上.利用TEM,AFM,ζ-电位,HAADF-STEM,TGA及XRD等方法对所制备的杂化材料进行了表征.另外,研究了Ag@Au NPs,Ag/Au NCs和Ag/Au NCs-GO3种纳米材料在催化4-,3-或2-硝基苯酚还原为4-,3-或2-硝基苯胺方面所表现出的催化性质,对比研究发现其催化活性具有如下趋势:Ag/Au NCs-GO>Ag/Au NCs>Ag@Au NPs.实验结果表明,纳米杂化材料的组分和其提供的有效表面积都对其优异的催化活性起了重要作用.

关键词： Bimetallic nanoparticles GO Electrostatic self-assembly Catalytic properties nitrophenol

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