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Iron-phosphorus-base catalyst for preparing bromomethane by methane oxybromination, and preparation method and application thereof

A methane bromide oxidation and catalyst technology, applied in chemical instruments and methods, physical/chemical process catalysts, carbon monoxide, etc., can solve the problem of precious metal Rh loss, etc., and achieve excellent anti-carbon performance, excellent structural stability, and good stability Effect

Inactive Publication Date: 2012-08-15
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Synthesis of Rh / SiO by sol-gel method by Liu et al. 2 Catalyst and investigated its catalytic methane bromination oxidation reaction performance, even if the catalyst can get nearly 40% methane conversion rate and 90% CH at the reaction temperature of 660 ° C 3 Br selectivity, but there is a significant loss of noble metal Rh after nearly 700 hours of reaction (Z.Liu, W.S.Li, X.P.Zhou, J.Nat.Gas.Chem., 2010, 19, 522-529)

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0030] 16.0g triblock polymer P123 (EO) 20 (PO) 70 (EO) 20 , 28.06g phosphoric acid aqueous solution (phosphoric acid mass specific gravity is 85%) mixed with 562g deionized water, and mechanically stirred for 2 hours at 35° C. in a water bath to obtain solution A. 2.89g ferric nitrate nonahydrate [Fe(NO 3 ) 3 .9H 2 [0], 32.8mL tetraethyl orthosilicate and 40mL deionized water were magnetically stirred at room temperature for 0.5 hour to obtain solution B. Under vigorous mechanical stirring at 35°C, solution B was added to solution A, and stirring was continued for 20 hours to obtain emulsion C. Emulsion C was transferred to a hydrothermal synthesis kettle for crystallization at 90° C. for 24 hours. After filtering the slurry containing the precipitate obtained in the hydrothermal kettle and washing with deionized water, the filter cake was dried at 60°C, and finally roasted at 600°C for 4 hours in a muffle furnace to obtain a solid sample (inductively coupled plasma In...

Embodiment 2

[0037] Mix 16.0 g of triblock polymer P123, 28.06 g of phosphoric acid aqueous solution (85% by mass of phosphoric acid) and 556 g of deionized water, and mechanically stir in a water bath at 35° C. for 2 hours to obtain solution A. 6.51g ferric chloride [FeCl 3 .6H 2 O], 32.8mL tetraethyl orthosilicate and 40mL deionized water were magnetically stirred at room temperature for 0.5 hours to obtain solution B. Under vigorous mechanical stirring at 35°C, solution B was added to solution A, and stirring was continued for 20 hours to obtain emulsion C. The emulsion C was transferred to a hydrothermal synthesis kettle for crystallization at 100° C. for 24 hours. After filtering the slurry containing the precipitate prepared in the hydrothermal kettle and washing with deionized water, the filter cake was dried at 80°C, and finally roasted at 600°C for 4 hours in a muffle furnace to obtain a solid sample (inductively coupled plasma In the composition of the solid (ICP) test sample,...

Embodiment 3

[0039] Mix 16.0 g of triblock polymer P123, 41.16 g of phosphoric acid aqueous solution (85% by mass of phosphoric acid) and 562 g of deionized water, and mechanically stir in a water bath at 35° C. for 2 hours to obtain solution A. 3.82g ferrous sulfate [FeSO 4 .7H 2 O], 32.8mL tetraethyl orthosilicate and 40mL deionized water were magnetically stirred at room temperature for 0.5 hours to obtain solution B. Under vigorous mechanical stirring at 35°C, solution B was added to solution A, and stirring was continued for 20 hours to obtain emulsion C. The emulsion C was transferred to a hydrothermal synthesis kettle for crystallization at 110° C. for 24 hours. After filtering the slurry containing the precipitate obtained in the hydrothermal kettle and washing with deionized water, the filter cake was dried at 60°C, and finally roasted at 600°C for 4 hours in a muffle furnace to obtain a solid sample (inductively coupled plasma In the composition of the solid (ICP) test sample,...

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PUM

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Abstract

The invention relates to an Fe-P-O / SBA-15 catalyst for preparing bromomethane and CO by methane oxybromination, which is composed of an active component and a support, wherein the active component comprises one or more of FePO4, Fe2P2O7 and alpha-Fe3(P2O7)2; the active component accounts for 1.0-60.0% of the catalyst by weight; the Fe / Si mol ratio in the catalyst is 0.001-1.0; the P / Si mol ratio in the catalyst is 1.0-5.0; the support is an SBA-15 full-silicon molecular sieve; and the specific area of the catalyst is 100-1500m<2> / g, and the pore volume is 0.65-1.20m<3> / g. The preparation method of the catalyst comprises the following steps: by using ferric salt, phosphoric acid [H3PO4] and ethyl orthosilicate [(C2H5O)4Si] as precursors and a triblock polymer [(EO)20(PO)70(EO)20] (P123 for short) as a template, introducing the active component into the support by a hydrothermal method, washing, filtering, drying, roasting and forming to obtain the Fe-P-O / SBA-15 catalyst.

Description

technical field [0001] The invention relates to a Fe-P-O / all-silicon molecular sieve SBA-15 catalyst used for methane bromination oxidation to prepare methyl bromide and CO, its preparation method and its use for preparing methyl bromide and CO from methane, oxygen and HBr aqueous solution. Background technique [0002] Natural gas is considered to be the cleanest fossil energy. With the increasing energy consumption for human survival, how to convert natural gas into other chemical raw materials is a key issue to reduce human dependence on petroleum resources. At present, the main way of industrial utilization of natural gas is to firstly synthesize gas through steam recombination, and then realize the indirect conversion of natural gas into chemicals through the subsequent Fischer-Tropsch synthesis reaction. Due to the high energy consumption and complicated process of this process, only the application in large natural gas fields can produce economic benefits. Natural ga...

Claims

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Application Information

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IPC IPC(8): B01J29/03C07C19/075C07C17/154C01B31/18C01B32/40
Inventor 林荣和丁云杰王润琴
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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