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Rhodium metal complex-based mesoporous catalyst, as well as preparation method and application thereof

A technology of metal complexes and catalysts, which is applied in the field of heterogeneous mesoporous catalytic materials, can solve problems such as unfavorable industrialization promotion, difficulty in catalyst separation, and troubles for wide application, so as to reduce catalyst cost, high thermal stability, increase yield and selective effect

Inactive Publication Date: 2016-07-20
TAIYUAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] Homogeneous catalysis has mild reaction conditions, high catalytic activity and high selectivity, but the difficulty of catalyst separation and organic solvent pollution have always plagued its wide application in industry.
However, the cost pressure of using three precious metals at the same time makes it unfavorable for industrialization

Method used

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  • Rhodium metal complex-based mesoporous catalyst, as well as preparation method and application thereof
  • Rhodium metal complex-based mesoporous catalyst, as well as preparation method and application thereof
  • Rhodium metal complex-based mesoporous catalyst, as well as preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0029] 1.0gF127 (EO 106 PO 70 EO 106 ) and 0.9g of potassium chloride were added to 40mL of 2.0mol / L hydrochloric acid solution, stirred at 40°C to dissolve the surfactant completely, then 4mL of tetraethyl orthosilicate was added dropwise to the system, stirred for 24h, and the milk The turbid liquid was put into a 100mL stainless steel reaction kettle with a Teflon liner, hydrothermally crystallized at 100°C for 48h, suction filtered, washed, dried, and roasted at 550°C for 6h to remove the organic template to obtain mesoporous SBA-16 Molecular sieve carrier.

[0030] Take 2.0g of SBA-16 molecular sieve and impregnate it in an equal volume of 9.76×10 -4 mol hydrated rhodium trichloride aqueous solution, ultrasonication for 2 hours, standing at room temperature for 24 hours, and drying to obtain a rhodium metal mesoporous catalyst (1g of SBA-16 carrier loaded with 0.48mmol of rhodium metal active components).

[0031] Take 2.2g of rhodium metal mesoporous catalyst, mix wi...

Embodiment 2

[0037] The preparation of the mesoporous catalyst is the same as in Example 1, except that the loading amount of the rhodium metal active component is 0.36 mmol / g, and the ligand material is changed to tributylphosphine.

[0038] The mesoporous catalyst prepared in this example has a highly ordered three-dimensional cubic mesoporous structure, and the mesopore diameter, specific surface area and pore volume are 5.7nm and 698m 2 / g and 0.43cm 3 / g, rhodium metal complex loading 1.8%.

[0039] Carry out methyl acetate carbonylation reaction synthetic ethylene diacetate test according to embodiment 1, the result shows methyl acetate conversion rate 70.1%, ethylene diacetate selectivity 66.3%.

Embodiment 3

[0041] The preparation of the mesoporous catalyst was the same as in Example 1, except that the loading amount of the rhodium metal active component was 0.4 mmol / g, and the solvent of the ligand material was changed to ethanol.

[0042] The mesoporous catalyst prepared in this example has a highly ordered three-dimensional cubic mesoporous structure, and the mesopore diameter, specific surface area and pore volume are 5.8nm and 665m 2 / g and 0.42cm 3 / g, rhodium metal complex loading 2.04%.

[0043] Carry out methyl acetate carbonylation reaction synthetic ethylene diacetate test according to embodiment 1, the result shows methyl acetate conversion rate 73.4%, ethylene diacetate selectivity 66.7%.

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Abstract

The invention discloses a rhodium metal complex-containing mesoporous catalyst for synthesizing ethylidene diacetate by methyl acetate carbonylation reaction. The problems of difficulty in separation, low methyl acetate conversion rate, low ethylidene diacetate yield and low selectivity of an existing homogeneous catalyst are mainly solved. The catalyst consists of an inorganic mesoporous carrier material SBA-16 and a rhodium metal complex dispersed in pore walls of mesopores of the carrier material. The rhodium metal complex is highly uniformly dispersed, higher reactivity and target product selectivity are achieved, and the selectivity of the ethylidene diacetate reaches 70 percent or above.

Description

technical field [0001] The invention relates to a heterogeneous mesoporous catalytic material, in particular to a rhodium metal complex-based mesoporous catalyst with high methyl acetate selective catalytic reaction activity, and a preparation method of the catalyst. Background technique [0002] Ethylene diacetate is an important raw material for the production of vinyl acetate (VAC), and VAC is one of the largest organic chemical raw materials in the world. It is widely used in PVAC, resins, coatings, pastes, adhesives, chemical fiber products, etc. industry. The current research direction of the production process of ethylene diacetate is to produce ethylene diacetate through the carbonylation reaction of methyl acetate and synthesis gas without relying on petrochemical raw materials. [0003] The process for preparing ethylene diacetate by carbonylation of methyl acetate has been disclosed by US4659865 and US4429150. The former uses organic nitrogen, organic phosphorus...

Claims

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Application Information

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IPC IPC(8): B01J31/24B01J31/22C07C67/36C07C69/16
CPCB01J31/185B01J31/24B01J31/2409B01J2231/40B01J2531/0258B01J2531/822C07C67/36C07C69/16
Inventor 李瑞丰韩武刚李成才孙玥荣俊
Owner TAIYUAN UNIV OF TECH
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