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Preparation method of ZnO-ZrO2-coated ZSM-5 core-shell structure catalyst

A core-shell structure and catalyst technology, applied in catalyst activation/preparation, preparation of organic compounds, molecular sieve catalysts, etc., can solve the problems of poor catalytic effect of composite catalysts, poor anti-sintering stability, etc., to inhibit the generation of by-products, alleviate the The effect of carbon deposition and high reactivity

Inactive Publication Date: 2018-09-28
GUIZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the active components of existing composite catalysts are randomly distributed, and the structure only provides an open reaction environment. More importantly, the distribution structure with traditional nano-copper particles as the active component has extremely poor anti-sintering stability and cannot effectively solve the problem of CO 2 CO in the two-step process of hydrogenation and methanol to light olefins 2 The hydrogenation synthesis of methanol process and methanol catalytic conversion to light olefins process require different reaction formation and dissociation conversion environmental conditions, resulting in the poor catalytic effect of existing composite catalysts

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0011] A method for preparing a ZnO-ZrO2@ZSM-5 core-shell structure catalyst, comprising the following steps:

[0012] (1) ZnO-ZrO 2 Preparation: According to the molar ratio of raw materials NH 4 CO 3 :Zr(NO 3 ) 4 ·5H 2 O: Zn(NO 3 ) 2 ·6H 2 O=2.2:1.0:0.2, under stirring, flow 1.0 mol L at a flow rate of 3ml / min -1 Add the ammonium carbonate solution to the zinc-zirconium mixed solution to form a precipitate, keep stirring and aging at 70°C for 2h, cool to room temperature, filter, wash, dry at 110°C for 4h, and roast at 500°C for 3h to obtain ZnO-ZrO 2 powder.

[0013] (2) Preparation of ZnO-ZrO2@ZSM-5 core-shell structure catalyst: according to the molar ratio of raw materials n(TEOS):n(NaAlO 2 ):n(TPAOH):n(H 2 O)= 40:1:19:4015 under stirring, sequentially add NaAlO 2 , TPAOH and TEOS were added to deionized water, continuously stirred evenly, stirred and aged at room temperature for 3 hours to form a sol system, according to the core-shell mass ratio ZnO-ZrO 2 ...

Embodiment 2

[0016] A method for preparing a ZnO-ZrO2@ZSM-5 core-shell structure catalyst, comprising the following steps:

[0017] (1) ZnO-ZrO 2 Preparation: According to the molar ratio of raw materials NH 4 CO 3 :Zr(NO 3 ) 4 ·5H 2 O: Zn(NO 3 ) 2 ·6H 2 O=2.2:1.0:0.2, under stirring, flow 1.0 mol L at a flow rate of 3ml / min -1 Add the ammonium carbonate solution to the zinc-zirconium mixed solution to form a precipitate, keep stirring and aging at 70°C for 2h, cool to room temperature, filter, wash, dry at 110°C for 4h, and roast at 500°C for 3h to obtain ZnO-ZrO 2 powder.

[0018] (2) Preparation of ZnO-ZrO2@ZSM-5 core-shell structure catalyst: according to the molar ratio of raw materials n(TEOS):n(NaAlO 2 ):n(TPAOH):n(H 2 O)=80:1:19:4015 under stirring, sequentially add NaAlO 2 , TPAOH and TEOS were added to deionized water, continuously stirred evenly, stirred and aged at room temperature for 3 hours to form a sol system, according to the core-shell mass ratio ZnO-ZrO 2 :...

Embodiment 3

[0021] A method for preparing a ZnO-ZrO2@ZSM-5 core-shell structure catalyst, comprising the following steps:

[0022] (1) ZnO-ZrO 2 Preparation: According to the molar ratio of raw materials NH 4 CO 3 :Zr(NO 3 ) 4 ·5H 2 O: Zn(NO 3 ) 2 ·6H 2 O=2.2:1.0:0.2, under stirring, flow 1.0mol L at a flow rate of 3ml / min-1 The ammonium carbonate solution was added to the mixed solution of zinc and zirconium to form a precipitate, which was continuously stirred and aged at 70 °C for 2 hours, cooled to room temperature, filtered, washed, dried at 110 °C for 4 hours, and calcined at 500 °C for 3 hours to obtain ZnO-ZrO 2 powder.

[0023] (2) Preparation of ZnO-ZrO2@ZSM-5 core-shell catalyst: according to the molar ratio of raw materials n(TEOS):n(NaAlO 2 ): n(TPAOH): n(H 2 O) = 200: 1: 19: 4015 Under stirring, the NaAlO 2 , TPAOH and TEOS were added to deionized water, stirred continuously, and aged at room temperature for 3h to form a sol system. According to the mass ratio of ...

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PUM

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Abstract

The invention discloses a preparation method of a ZnO-ZrO2-coated ZSM-5 core-shell structure catalyst. The preparation method comprises the following steps: preparing ZnO-ZrO2 powder: stirring the materials according to a raw material mole ratio of n(TEOS): n(NaAlO2): n(TPAOH): n(H2O) being 40-360: 1: 19: 4015, adding NaAlO2, TPAOH and TEOS in deionized water in order, continuously and uniformly stirring the materials, stirring and aging the materials for 3 h under room temperature to form a sol system, placing the ZnO-ZrO2 powder according to a core-shell mass ratio being 1:8-8:1 in a systemfor continuous and uniform stirring, performing a hydrothermal reaction for 36-48 h at the temperature of 170-190 DEG C in a homogeneous reactor, cooling the materials to room temperature, performingcentrifugation, washing the materials with deionized water and absolute ethyl alcohol, drying the material for 12 h at the temperature of 120 DEG C, and performing roasting for 3 h at the temperatureof 500-600 DEG C. The ZnO-ZrO2-coated ZSM-5 core-shell structure catalyst can increase carbon dioxide conversion rate and low carbon olefin selectivity during a low carbon olefin two-step preparationtechnology by CO2 hydrogenation through methanol.

Description

technical field [0001] The invention belongs to the technical field of chemical industry, in particular to a ZnO-ZrO 2 The preparation method of @ZSM-5 core-shell structure catalyst. Background technique [0002] Zinc Zirconium (ZnO-ZrO 2 ) The two-component catalyst is CO 2 Catalytic hydrogenation synthesis methanol process is a kind of metal oxide catalyst with strong anti-sintering stability and anti-sulfur ability and good effect. ZSM-5 molecular sieve is made of SiO 4 and AlO 4 Microporous silica-alumina molecular sieves with tetrahedral units interlaced to form a three-dimensional intersecting channel structure are widely used in methanol catalytic cracking because of their rich and adjustable B-acid properties, high specific surface area and unique shape-selective function of microporous products. Low Carbon Olefin Process (MTO). Accordingly, a bifunctional core-shell catalyst was prepared by coupling metal oxides and acidic molecular sieves, and applied to CO...

Claims

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Application Information

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IPC IPC(8): B01J29/40B01J37/08B01J37/10C07C1/20C07C11/02C07C29/153C07C31/04C01B39/40
CPCC01B39/40C07C1/20C07C29/153B01J23/002B01J29/405B01J35/397C07C11/02C07C31/04Y02P20/52
Inventor 刘飞曹建新王冠超王晓丹
Owner GUIZHOU UNIV
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