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Composite material for improving reaction activity of Fe(III)-TAML and preparation method and application method thereof

A technology based on hexamethylphenyl and composite materials, which can be used in chemical instruments and methods, other chemical processes, organic compounds/hydrides/coordination complex catalysts, etc., and can solve the problems of high synthesis cost and low yield. , to achieve the effect of improving the reactivity, improving the reactivity and promoting the ionization of water molecules

Active Publication Date: 2017-12-22
NANJING UNIV
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  • Claims
  • Application Information

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Problems solved by technology

[0006] The activity of Fe(III)-TAML in the prior art has a strong pH dependence and will be significantly reduced under neutral conditions. The existing preparations contain -F, -Cl and -NO 2 The yield of Fe(III)-TAML of the substituent is very low, which requires high synthesis cost. Therefore, it is necessary to develop an economical and simple method to improve Fe(III)-TAML at neutral or near-neutral reactivity under conditions

Method used

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  • Composite material for improving reaction activity of Fe(III)-TAML and preparation method and application method thereof
  • Composite material for improving reaction activity of Fe(III)-TAML and preparation method and application method thereof
  • Composite material for improving reaction activity of Fe(III)-TAML and preparation method and application method thereof

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preparation example Construction

[0045] The preparation method of the composite material for improving the reaction activity of tetraamidohexamethylphenyl ring iron of the present invention comprises the following steps:

[0046] (1) DODMA is dissolved in methylene chloride;

[0047] (2) Dissolving Fe(III)-TAML in ultrapure water;

[0048] (3) Dissolve PFOA in ultrapure water, adjust the pH of the solution to 6-8;

[0049] (4) adding the PFOA in step (3) to the Fe(III)-TAML solution in step (2) to obtain a mixed solution of Fe(III)-TAML and PFOA;

[0050] (5) DODMA, Fe(III)-TAML and PFOA are mixed in a molar ratio of 1:(3-12):(0.01-1);

[0051] (6) after adding the DODMA solution dropwise to the mixed solution of Fe(III)-TAML and PFOA, use a magnetic stirrer to stir for 24 hours to ensure that dichloromethane is completely volatilized;

[0052] (7) After the stirring is completed, let it stand for at least 24 hours, so that the composite material Fe(III)-TAML / DODMA / PFOA can be fully aged.

[0053] In the ...

Embodiment 1

[0061] A composite material preparation method for improving the reactivity of tetraamidohexamethylphenyl ring iron, comprising the steps of: using a surfactant-assisted self-assembly method to dissolve dioctadecyldimethyl chloride in dichloromethane Ammonium DODMA (30 mM) was added dropwise to 20 mL of a mixed aqueous solution of Fe(III)-TAML (100 μM) and PFOA (1, 5, 10, 50, and 100 μM) to synthesize Fe(III)-TAML-based composites Fe(III)-TAML / DODMA / PFOA; wherein the molar ratio of Fe(III)-TAML, DODMA and PFOA is 1:3:0.01, 1:3:0.1, 1:3:1, 1:6:0.01, 1:6:0.1, 1:6:1, 1:12:0.01, 1:12:0.1, 1:12:1. During the preparation process, for all treatment groups, a yellow opaque emulsion was formed when DODMA was added, and Fe(III)-TAML in the solution settled to the bottom of the solution after standing for separation; After stirring for more than 24 hours, a stable yellow suspension was obtained, which was then used for characterization, degradation and stability experiments after standi...

Embodiment 2

[0064] A composite material preparation method for improving the reactivity of tetraamidohexamethylphenyl ring iron, comprising the steps of: using a surfactant-assisted self-assembly method to dissolve dioctadecyldimethyl chloride in dichloromethane Ammonium DODMA (30 mM) was added dropwise to 20 mL of a mixed aqueous solution of Fe(III)-TAML (100 μM) and PFOA (1, 5, 10, 50, and 100 μM) to synthesize Fe(III)-TAML-based composites Fe(III)-TAML / DODMA / PFOA. The molar ratios of Fe(III)-TAML, DODMA and PFOA were 1:3:0.01, 1:3:0.1, 1:3:1, 1:6:0.01, 1:6:0.1, 1:6:1, 1:12:0.01, 1:12:0.1, 1:12:1. During the preparation process, for all treatment groups, a yellow opaque emulsion was formed when DODMA was added, and Fe(III)-TAML in the solution settled to the bottom of the solution after standing for separation. When vigorously stirred for more than 24 hours, a stable yellow suspension was obtained, which was then used for characterization, degradation and stability experiments after s...

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Abstract

The invention discloses a composite material for improving the reaction activity of Fe(III)-tetra-amido macrocyclic ligand (Fe(III)-TAML) and a preparation method and application method thereof, belongs to the field of synthesis of environment functional materials, and solves the issue of significantly reduced reaction activity of the Fe(III)-TAML under neutral or near neutral conditions. A micro Composite material Fe(III)-TAML / DODMA / PFOA, with the Fe(III)-TAML as a base, is synthesized by a self-assembly method assisted by a surface active agent dioctadecyl dimethyl ammonium chloride (DODMA), wherein a dichloromethane / water mixed solvent is used as a medium and perfluorooctanoic acid (PFOA) is used as a dopant. Compared with the free Fe(III)-TAML of the prior art, the reaction activity of the composite material Fe(III)-TAML / DODMA / PFOA synthesized by the self-assembly method assisted by the surface active agent is significantly improved.

Description

technical field [0001] The invention belongs to the field of environmental functional material synthesis, and more particularly relates to a composite material for improving the reaction activity of tetraamidohexamethylphenyl ring iron and a preparation method and an application method thereof. Background technique [0002] The hydrogen peroxide activator tetraamidohexamethylphenyl iron (referred to as tetraamidocyclic iron, Fe(III)-TAML) can efficiently remove a variety of organic pollutants, such as chlorophenols (S.S.Gupta, M.Stadler, et al. al., Rapid TotalDestruction of Chlorophenols by Activated Hydrogen Peroxide, Science 296(2002) 326-328; K. Mierzwicki, S. Berski, et al., AIM and ELF analysis of the H-, Me-, and F-substituted FeIII- TAML complexes, Chemical Physics Letters 507(2011) 29-36), Organophosphorus Pesticide Fe-TAML Peroxide Activators (A. Chanda, S.K. Khetan, et al., Total Degradation of Fenitrothion and Other Organophosphorus Pesticides by Catalytic Oxidat...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J20/20B01J20/30C02F1/72C02F101/36
CPCB01J20/223C02F1/722C02F1/725B01J31/0232B01J31/0239B01J31/183C02F2101/36B01J2531/0238B01J2531/842B01J35/19
Inventor 谷成王超
Owner NANJING UNIV
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