CN110026198A - Using magnalium hydrotalcite as the preparation method and applications of the nickel-base catalyst of presoma - Google Patents

Using magnalium hydrotalcite as the preparation method and applications of the nickel-base catalyst of presoma Download PDF

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Publication number
CN110026198A
CN110026198A CN201910315241.8A CN201910315241A CN110026198A CN 110026198 A CN110026198 A CN 110026198A CN 201910315241 A CN201910315241 A CN 201910315241A CN 110026198 A CN110026198 A CN 110026198A
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nickel
base catalyst
presoma
preparation
reaction
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CN201910315241.8A
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Chinese (zh)
Inventor
陈海涛
王沈峰
陶红
郭依洁
杨文�
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Guilin University of Technology
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Guilin University of Technology
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/78Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with alkali- or alkaline earth metals
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/12Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon dioxide with hydrogen
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2523/00Constitutive chemical elements of heterogeneous catalysts
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C2523/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00
    • C07C2523/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of the iron group metals or copper
    • C07C2523/76Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups C07C2523/02 - C07C2523/36
    • C07C2523/78Catalysts comprising metals or metal oxides or hydroxides, not provided for in group C07C2521/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups C07C2523/02 - C07C2523/36 with alkali- or alkaline earth metals or beryllium

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Materials Engineering (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Catalysts (AREA)

Abstract

The invention discloses a kind of using magnalium hydrotalcite as the preparation method and applications of the nickel-base catalyst of presoma.First, the magnesium aluminum oxide using magnalium hydrotalcite as presoma is prepared by hydrothermal synthesis method and high-temperature roasting method, then, the nickel-base catalyst that magnesium aluminum oxide supports is prepared by infusion process and high-temperature roasting method, which can be used in carbon dioxide methanation catalysis reaction.Preparation method of the invention is simple, easy to operate, and nickel-base catalyst made from this method can be used in carbon dioxide methanation catalysis reaction, and catalytic performance with higher, and when reaction temperature is 400 DEG C, methane production reaches 80.1%.

Description

Using magnalium hydrotalcite as the preparation method and applications of the nickel-base catalyst of presoma
Technical field
The present invention relates to a kind of preparation methods of carbon dioxide methanation nickel-base catalyst, and especially one kind is with magnalium water Talcum is the preparation method and applications of the nickel-base catalyst of presoma.
Background technique
The main reason for the discharged GHG carbon dioxide of fossil fuel burning is caused global warming.To reduce The discharge of carbon dioxide, people to carbon dioxide using having carried out a large amount of research, as carbon dioxide capture and storage, two The chemical conversion etc. of carbonoxide.The catalyzed conversion that hydrogenation of carbon dioxide prepares methane is the important side for reducing CO2 emission Method.For this purpose, developing high-performance carbon dioxide methanation catalyst is the most important thing.
Currently, commercial carbon dioxide methanation catalyst is mainly the nickel-base catalyst of alumina load, raw material at This is low, and the selectivity of methane is good in catalytic conversion process.But conversion ratio is low for noble metal catalyst.Therefore, Research and the excellent nickel-base catalyst of processability have important practical significance to catalysis transform of carbon dioxide.Magnalium hydrotalcite With properties such as excellent alkalinity, adsorptivity, thermal stability, nontoxicitys, so in catalyst carrier, environment-friendly materials, adsorption material There is good application prospect in the fields such as material, pharmaceutical carrier, functional material.
Summary of the invention
The object of the present invention is to provide a kind of using magnalium hydrotalcite as the preparation method of the nickel-base catalyst of presoma and its Using the nickel-base catalyst can be improved the conversion ratio and yield that catalysis transform of carbon dioxide prepares methane.
Thinking of the present invention: firstly, being prepared by hydrothermal synthesis method and high-temperature roasting method using magnalium hydrotalcite as presoma Carrier-magnesium aluminum oxide be then prepared what magnesium aluminum oxide supported by nickel impregnation method and high-temperature roasting method Nickel-base catalyst.
Preparation is using magnalium hydrotalcite as the specific steps of the nickel-base catalyst of presoma are as follows:
(1) 1.03 g magnesium nitrates, 0.75 g aluminum nitrate, 80 mL distilled water and 1.5 g urea are successively added into beaker, and will Beaker is placed on magnetic stirring apparatus stirring until solid is completely dissolved, and mixed solution is made.
(2) mixed solution made from step (1) is transferred in the reaction kettle of 100 mL polytetrafluoroethyllining linings, will be reacted Kettle, which is placed at 110 DEG C, to react 10 hours, and cooled to room temperature, then depressurizes and filter, with distilled water and ethyl alcohol after reaction 10 hours dry at 90 DEG C after washing 3 ~ 5 times respectively, products therefrom is transferred in the middle part of tube furnace, and lower 600 DEG C of air atmosphere Roasting 3 hours, cooled to room temperature, is made magnesium aluminum oxide catalyst carrier after reaction.
(3) 0.22 g nickel nitrate is dissolved in 1 mL distilled water, the oxidation of magnalium made from 0.4 g step (2) is then added Object catalyst carrier, after being uniformly mixed and standing 3 hours, 5 hours dry in 90 DEG C, products therefrom is transferred to tube furnace Middle part, prior to 350 DEG C constant temperature 1 hour under air atmosphere, then roasts 3 hours in 450 DEG C, naturally cools to after reaction Room temperature obtains the nickel-base catalyst using magnalium hydrotalcite as presoma.
Of the invention reacts using magnalium hydrotalcite as the nickel-base catalyst of presoma applied to carbon dioxide methanation.
Preparation method of the invention is low in cost, easy to operate.It is of the invention using magnalium hydrotalcite as the Ni-based of presoma Catalyst has excellent catalytic properties when carbon dioxide methanation reacts, and can be improved catalysis transform of carbon dioxide preparation first The conversion ratio and yield of alkane.
Detailed description of the invention
Fig. 1 is that prepare in the embodiment of the present invention is the nickel-base catalyst of presoma in carbon dioxide first using magnalium hydrotalcite The variation relation figure of methane production and reaction temperature when alkylation reaction.
Specific embodiment
Embodiment:
(1) 1.03 g magnesium nitrates, 0.75 g aluminum nitrate, 80 mL distilled water and 1.5 g urea are successively added into beaker, and will Beaker is placed on magnetic stirring apparatus stirring until solid is completely dissolved, and mixed solution is made.
(2) mixed solution made from step (1) is transferred in the reaction kettle of 100 mL polytetrafluoroethyllining linings, will be reacted Kettle, which is placed at 110 DEG C, to react 10 hours, and cooled to room temperature, then depressurizes and filter, with distilled water and ethyl alcohol after reaction 10 hours dry at 90 DEG C after washing 4 times respectively, products therefrom is transferred in the middle part of tube furnace, the lower 600 DEG C of roastings of air atmosphere It burns 3 hours, cooled to room temperature, is made magnesium aluminum oxide catalyst carrier after reaction.
(3) 0.22 g nickel nitrate is dissolved in 1 mL distilled water, the oxidation of magnalium made from 0.4 g step (2) is then added Object catalyst carrier, after being uniformly mixed and standing 3 hours, 5 hours dry in 90 DEG C, products therefrom is transferred to tube furnace Middle part, prior to 350 DEG C constant temperature 1 hour under air atmosphere, then roasts 3 hours in 450 DEG C, naturally cools to after reaction Room temperature obtains the nickel-base catalyst using magnalium hydrotalcite as presoma.
It weighs 0.1 g of nickel-base catalyst made from the present embodiment to be packed into reaction tube, be restored 1 hour at 750 DEG C, hydrogen Throughput is 20 mL/min.After end cooled to room temperature to be restored, the temperature was then adjusted to temperature needed for carbon dioxide methanation Degree, and gas is switched to carbon dioxide and hydrogen volume than the mixed gas for 1:4, mixed gas flow is 50 mL/min, Using the gas-chromatography on-line analysis gaseous product of thermal conductivity detector (TCD).
It finds after tested, the nickel-base catalyst of the method for the invention preparation is with higher in carbon dioxide methanation Methane production, at 400 DEG C of reaction temperature, methane production reaches 80.1%.Using magnalium hydrotalcite as the nickel-base catalyst of presoma Methane production at a temperature of differential responses is as shown in Figure 1.

Claims (2)

1. a kind of using magnalium hydrotalcite as the preparation method of the nickel-base catalyst of presoma, it is characterised in that specific steps are as follows:
(1) 1.03 g magnesium nitrates, 0.75 g aluminum nitrate, 80 mL distilled water and 1.5 g urea are successively added into beaker, and will Beaker is placed on magnetic stirring apparatus stirring until solid is completely dissolved, and mixed solution is made;
(2) mixed solution made from step (1) is transferred in the reaction kettle of 100 mL polytetrafluoroethyllining linings, reaction kettle is set It is reacted at 110 DEG C 10 hours, cooled to room temperature, then depressurizes and filter after reaction, is distinguished with distilled water and ethyl alcohol 10 hours dry at 90 DEG C after washing 3 ~ 5 times, products therefrom is transferred in the middle part of tube furnace, the lower 600 DEG C of roastings 3 of air atmosphere Hour, cooled to room temperature, is made magnesium aluminum oxide catalyst carrier after reaction;
(3) 0.22 g nickel nitrate is dissolved in 1 mL distilled water, magnesium aluminum oxide made from 0.4 g step (2) is then added and urges Agent carrier, 5 hours dry in 90 DEG C after being uniformly mixed and standing 3 hours, products therefrom is transferred in the middle part of tube furnace, Then prior to 350 DEG C constant temperature 1 hour under air atmosphere roasts 3 hours, cooled to room temperature after reaction in 450 DEG C, Obtain the nickel-base catalyst using magnalium hydrotalcite as presoma.
2. a kind of answering using magnalium hydrotalcite as the nickel-base catalyst of presoma of preparation method preparation as described in claim 1 With, it is characterised in that the nickel-base catalyst is reacted applied to carbon dioxide methanation.
CN201910315241.8A 2019-04-18 2019-04-18 Using magnalium hydrotalcite as the preparation method and applications of the nickel-base catalyst of presoma Pending CN110026198A (en)

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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109621939A (en) * 2019-01-04 2019-04-16 北京化工大学 Ternary composite metal oxide solid base catalyst and its preparation method and application

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109621939A (en) * 2019-01-04 2019-04-16 北京化工大学 Ternary composite metal oxide solid base catalyst and its preparation method and application

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
ZHIGANGFAN等: "Improved activity of Ni/MgAl2O4 for CO2 methanation by the plasma decomposition", 《JOURNAL OF ENERGY CHEMISTRY》 *

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