Core-shell type catalyst for directional catalytic conversion of biomass synthesis gas, and preparation of core-shell type catalyst

A catalytic conversion and synthesis gas technology, applied in the chemical field, can solve the problems of low hydrogenation conversion rate and achieve huge economic benefits, broad market application prospects, and good shape-selective effects

Pending Publication Date: 2018-11-30
QINGDAO UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

The core-shell structure catalyst adopts CO and CO 2 The solid solution or mixture of small-grain composite metal oxides with synergistic hydrogenation effect is used as the core layer, and the solid acid with microporous, mesoporous or hierarchical pore structure is used as the shell layer, and it is prepared into a core-shell type by freeze-drying method structure; not only solves the problem of CO in the current biomass syngas 2 The problem of low hydrogenation conversion rate, and further increase the conversion rate of CO hydrogenation

Method used

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  • Core-shell type catalyst for directional catalytic conversion of biomass synthesis gas, and preparation of core-shell type catalyst
  • Core-shell type catalyst for directional catalytic conversion of biomass synthesis gas, and preparation of core-shell type catalyst
  • Core-shell type catalyst for directional catalytic conversion of biomass synthesis gas, and preparation of core-shell type catalyst

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Effect test

Embodiment 1

[0029] Embodiment 1: preparation and application of core-shell structure catalyst

[0030] A method for preparing a core-shell structure catalyst for directional catalytic conversion of biomass synthesis gas, comprising the following steps:

[0031] ①Preparation of composite metal oxides with small grains (sol-gel method): 17.65g Zn(NO 3 ) 2 ·6H 2 O, 5.62gZrO(NO 3 ) 2 and 1.76g Ce(NO 3 ) 3 ·6H 2 The aqueous solution of O was stirred evenly, mixed with 15g of citric acid at 80°C, and then the pH value was adjusted to 8-9 with ammonia water to obtain a gel, dried at 100°C for 12 hours, and calcined at 500°C for 4 hours to obtain a small-grain composite metal oxide .

[0032] ②Surface modification of the metal oxide obtained in step ①: supersaturated impregnation with tetraethylammonium hydroxide (TEAOH)—condensation and reflux; use 0.1mol / L TEAOH of small-grain composite metal oxide at 55°C The solution was condensed and refluxed for 38 hours, filtered, and dried at 100...

Embodiment 2

[0042] Embodiment 2: preparation and application of core-shell structure catalyst

[0043] Different from Example 1, the preparation method of the core-shell structure catalyst for the directional catalytic conversion of biomass synthesis gas comprises the following steps:

[0044] ①Preparation of composite metal oxides with small crystal grains (uniform urea precipitation method): 17.65g Zn(NO 3 ) 2 ·6H 2 O, 5.62gZrO(NO 3 ) 2 , 1.76g Ce(NO 3 ) 3 ·6H 2 O and 40g of urea were dissolved in 200mL of water, and put into a stainless steel reactor lined with polytetrafluoroethylene, and reacted at 80°C for 24h to obtain a small-grain composite metal oxide.

[0045]②Surface modification of the metal oxide obtained in step ①: supersaturated impregnation with cetyltrimethylammonium bromide (CTAB)—condensation and reflux; / L CTAB solution was condensed and refluxed for 48 hours, filtered, and dried at 100° C. for 10 hours to obtain a surface-modified small-grain composite metal ...

Embodiment 3

[0054] Embodiment 3: preparation core-shell structure catalyst, contrast CO hydrogenation conversion catalyst and application

[0055] Different from Example 1, the preparation method of the core-shell structure catalyst for the directional catalytic conversion of biomass synthesis gas comprises the following steps:

[0056] ①Preparation of composite metal oxides with small grains (co-precipitation method): 25.30g Zn(NO 3 ) 2 ·6H 2 O, 16.25gCo(NO 3 ) 2 ·6H 2 O and 3.00g In(NO 3 ) 3 The aqueous solution was co-precipitated with 1mol / L ammonia solution, washed until neutral, dried at 120°C for 12h, and calcined at 550°C for 6h to obtain a small-grain composite metal oxide.

[0057] ② Surface modification of the metal oxide obtained in step ①: using cetyltrimethylammonium bromide (CTAB) supersaturated impregnation method—condensation and reflux; / L of CTAB solution was refluxed for 1 h, filtered, and dried at 100° C. for 12 h to obtain a surface-modified small-grain compo...

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Abstract

The invention provides a core-shell structure catalyst for directional catalytic conversion of biomass synthesis gas, and also provides a preparation method and application of the core-shell structurecatalyst. The core-shell structure catalyst comprises a core layer and a shell layer, wherein the core layer is prepared from small-grain composite metal oxide, and the shell layer is prepared from porous solid acid; the small-grain composite metal oxide is a solid solution or mixture of two or more oxides of ZnO, ZrO2, Co3O4, Fe2O3, In2O3, Ga2O3, CuO, Mn2O3, NiO, Cr2O3, La2O3 and CeO2. The core-shell catalyst adopts the solid solution or mixture of the small-grain composite metal oxide having a synergistic effect on hydrogenation of CO and CO2 as the core layer, and uses the solid acid having a microporous, mesoporous or multi-stage pore structure as the shell layer. The catalyst is prepared into a core-shell structure by means of a freeze-drying method, so that not only is the problem of lower hydrogenation conversion rate of CO2 in the biomass synthesis gas at present solved, but the conversion rate of CO hydrogenation is also further improved.

Description

technical field [0001] The invention belongs to the field of chemistry, and in particular relates to a core-shell catalyst for F-T synthesis, in particular to the preparation and application of a core-shell catalyst for directional catalytic conversion of biomass synthesis gas. Background technique [0002] Biomass energy is a carbon resource that is renewable and can replace fossil energy into liquid and gaseous fuels and other chemical raw materials. The thermochemical conversion route of biomass through gasification-synthesis is one of the current research hotspots, and it can better learn from the research and development experience of key technologies such as petroleum, coal, and natural gas chemicals. Biomass is obtained through directional gasification to obtain crude gas, and then reformed and purified to obtain biomass synthesis gas (CO / CO 2 / H 2 ). Then, the biomass synthesis gas can be converted into low-carbon olefins, methanol, dimethyl ether, hydrocarbons an...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/889B01J29/70B01J29/76B01J29/85B01J35/02C10G2/00
CPCB01J23/002B01J23/8898B01J29/7057B01J29/76B01J29/7676B01J29/85B01J35/0073B01J35/023B01J2523/00C10G2/33C10G2/334B01J2523/17B01J2523/32B01J2523/48B01J2523/68B01J2523/72Y02E50/30
Inventor 李琢于建强张妍陈志文李国民
Owner QINGDAO UNIV
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