Use Of A Porous Crystalline Hybrid Solid As A Nitrogen Oxide Reduction Catalyst And Devices

A porous crystalline, nitrogen oxide technology, applied in metal/metal oxide/metal hydroxide catalysts, organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, etc., can solve the problem of insufficient activity, Structural collapse, instability, etc.

Active Publication Date: 2012-05-30
CENT NAT DE LA RECHERCHE SCI +3
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0097] However, their activity remains insufficient in the presence of large amounts of oxygen, and in addition they are particularly unstable under real conditions, especially in the presence of steam and at high temperatures, which may sometimes even lead to the collapse of the structure

Method used

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  • Use Of A Porous Crystalline Hybrid Solid As A Nitrogen Oxide Reduction Catalyst And Devices
  • Use Of A Porous Crystalline Hybrid Solid As A Nitrogen Oxide Reduction Catalyst And Devices
  • Use Of A Porous Crystalline Hybrid Solid As A Nitrogen Oxide Reduction Catalyst And Devices

Examples

Experimental program
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Effect test

Embodiment 1

[0375] Example 1: Synthesis and data of examples of iron carboxylates useful as catalysts according to the invention

[0376] This example describes the synthesis of various metal carboxylates useful in the application of the invention. The solid obtained was characterized according to the method described below.

[0377] The crystallographic structure of iron carboxylate solid was analyzed by X-ray diffraction, using Siemens D5000 diffractometer (Cu Kα radiation, Mode θ-2θ), in air at room temperature. The figure is in terms of angular distance (2θ, degree °) or interplanar spacing (d, (Angstrom) shown).

[0378] The porosity (Langmuir specific surface area and pore volume) properties of the solid were measured by nitrogen adsorption at 77K, using a Micromeretics ASAP-2010 instrument. The solid was previously dehydrated overnight at 150° C. under one vacuum. The nitrogen adsorption isotherm of this solid is given by the curve representing the volume of adsorbed nitrog...

Embodiment 2

[0616] Example 2: Synthesis of iron(III) acetate for the manufacture of MOFs that can be used in the present invention

[0617] The iron(III) acetate used in the examples given below for the synthesis of the MOF material according to the present invention was synthesized according to the following scheme. This step of synthesis can refer to the work of Dziobkowski et al., Inorg. Chem., 1982, 21, 671 [87].

[0618] 6.72g metallic iron powder (Riedel-de , 99%), 64mL deionized water and 33.6mL water containing 70% perchloric acid (Riedel-de ) with magnetic stirring and heating at 50°C for 3 hours. After turning off the heat, the solution was stirred for 12 hours. The remaining metallic iron was removed by decantation, followed by replacement of the vessel. With stirring, 20.6 mL of aqueous hydrogen peroxide solution (35% sold by Alfa Aesar) was added dropwise, and the whole was kept under an ice bath at 0°C. 19.7 g of sodium acetate (Aldrich, 99%) was added to the blue sol...

Embodiment 3

[0619] Embodiment 3: synthesis can be used for the MOF ligand of the present invention

[0620] a) Synthesis A: Synthesis of chloroterephthalic acid

[0621] 6 g (0.043 mol) of chloroxylene (sold by Aldrich Corporation, >99%), 16 mL of nitric acid (sold by VWR Corporation, 70%), and 60 mL of distilled water were placed in a 120-mL polytetrafluoroethylene container. The container was placed in a PAAR metal cylinder and heated at 170°C for 12h. The product was recovered by filtration and washed with a large amount of distilled water. A yield of 75% was obtained.

[0622] 1 H NMR (300MHz, d 6 -DMSO): δ (ppm): 7.86 (d, J = 7.8 Hz), 7.93 (dd, J = 7.8; 1.2 Hz), 7.96 (d, J = 1.2 Hz).

[0623] b) Synthesis B: Synthesis of 3,5,3',5'-tetramethylbiphenyl-4,4'-dicarboxylic acid

[0624] The reaction scheme for this synthesis is Figure 48 shown in .

[0625] first step:

[0626] 10.2 g of tetramethylbenzidine (98%, Alfa Aesar) were suspended in 39 mL of concentrated hydroch...

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Abstract

The present invention relates to the use of solids consisting of a metal-organic framework (MOF) and having the units of the following formula (I): MmOkXILp as a nitrogen-oxide catalyst. The present invention also relates to devices for enabling the implementation of said use. The nitrogen oxides in question are nitrogen monoxide and nitrogen dioxide, collectively referred to as NOx. The MOF solids of the present invention are advantageously capable of removing nitrogen oxides from a liquid or gaseous effluent, for example from water, from the exhaust gases of a vehicle, factory, workshop, laboratory, stored products, urban air vents, etc., without any reducing agent and at a low temperature. The DeNOx catalysis is a major issue for our societies. The invention can be used for reducing or even avoiding the consequences for public health of the toxic NOx gases resulting from human activity.

Description

technical field [0001] The present invention relates to the use of solids composed of metal organic frameworks (MOF, metal organic framework) as nitrogen oxide reduction catalysts. [0002] The solids in question are crystalline hybrid solids consisting of inorganic units such as transition metals, lanthanum, alkali metals, etc., and organic ligands with several ligands such as carboxylate, phosphonate ), phosphate (phosphate), imidazolate and other ionic covalent assemblies. These solids useful in the present invention are defined herein. [0003] The nitrogen oxides in question are nitric oxide (NO) and nitrogen dioxide (NO 2 ), collectively referred to as NO X , and nitrous oxide (N 2 O), dinitrogen trioxide (N 2 o 3 ), and dinitrogen tetroxide (N 2 o 4 ). [0004] The MOF solids of the present invention can advantageously remove nitrogen oxides from liquid or gaseous effluents such as water, remove nitrogen oxides from exhaust gases from vehicles, factories, works...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22B01D53/94B01D53/86B01D53/56B01J23/745
CPCB01J2531/72B01D53/8628B01J2531/16B01J2531/56B01J2531/38B01J2531/31B01J2531/22B01J2531/46B01J2531/26B01J2531/62B01J31/2239B01J31/069Y02C20/10B01J2531/23B01D2255/20738B01J2531/842B01D53/9413B01J2531/32B01J31/1691B01J2531/48B01D53/56B01J2531/10
Inventor 亚历山大·维蒙特帕特里西亚·霍卡雅达科尔特斯黄瑛圭杰勒德·费里马尔科·达图里张钟山克里斯蒂安·塞尔尹志雄
Owner CENT NAT DE LA RECHERCHE SCI
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