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Special catalyst for reaction for preparing synthesis gas through dry reforming of methane, and preparation method thereof

A methane dry reforming and catalyst technology, which is applied in hydrogen/syngas production, chemical instruments and methods, chemical elements of heterogeneous catalysts, etc., can solve problems such as multiple side reactions, catalyst carbon deposition, deactivation, etc. Superior, solve the effect of high temperature sintering

Inactive Publication Date: 2019-12-06
FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Literature ACS Catalysis Volume: 9 Issues: 2 Pages: 932-945 (Publication Year: 2019) on Rh-La-based composite metal oxides 2 Zr 2 o 7 and Rh-La 2 Ti 2 o 7 Catalyzed DRM reaction research found: pyrochlore-type Rh-La 2 Zr 2 o 7 The surface Rh only exists in the form of single sites, showing excellent CH 4 Activation performance and anti-sintering ability; but too fast CH 4 The cracking rate caused a large amount of inert C* species to accumulate on the surface of the catalyst, resulting in the deactivation of the catalyst due to carbon deposition after 25 h of reaction
And perovskite-like Rh-La 2 Ti 2 o 7 Rh 0 and Rh δ+ active center, through the synergistic effect of the two can effectively increase the CO 2 The activation rate while CH 4 The cracking of the catalyst is also suppressed to a certain extent, the active O* species consumed on the surface of the catalyst is replenished in time, and the anti-coking ability of the catalyst is greatly improved, but as the reaction proceeds, the product H 2 The / CO ratio presents a gradually decreasing trend, indicating that the Rh-La 2 Ti 2 o 7 There are more side reactions in

Method used

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  • Special catalyst for reaction for preparing synthesis gas through dry reforming of methane, and preparation method thereof
  • Special catalyst for reaction for preparing synthesis gas through dry reforming of methane, and preparation method thereof
  • Special catalyst for reaction for preparing synthesis gas through dry reforming of methane, and preparation method thereof

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0030] A. Dissolve 8.66g of lanthanum nitrate, 6.46g of tetrabutyl titanate and 0.429g of zirconium nitrate in 50ml, 47.5ml and 2.5ml of absolute ethanol respectively. After completely dissolving, mix the three salt solutions in a beaker, and Sonicate at 25k Hz for 10 minutes.

[0031] B. be that 1wt.% is added the rhodium nitrate solution that 0.65g concentration is 1.13M in the solution of step A by rhodium in the final catalyst theoretical load, then add 50g concentration and be the dehydrated alcohol solution of the citric acid of 0.65M Stir evenly, and then sonicate at 25k Hz for 1 h to mix evenly to obtain a mixed solution.

[0032] C. Stir the mixed solution obtained in step B at room temperature under the condition of magnetic stirring for 10 h. Then, rotary evaporation was carried out at 60° C. in a vacuum environment until the solvent was evaporated to dryness to obtain a catalyst precursor.

[0033] D. Dry the catalyst precursor obtained in step C at 100°C for 12h...

Embodiment 2

[0037] A. Dissolve 8.66g of lanthanum nitrate, 3.4g of tetrabutyl titanate and 4.29g of zirconium nitrate in 50ml, 25ml and 25ml of absolute ethanol respectively. Hertzian ultrasound for 10 minutes.

[0038] B. be that 1wt.% is added the rhodium nitrate solution that 0.65g concentration is 1.13M in the solution of step A by the theoretical load of rhodium in the final catalyst, then add 50g concentration and stir the dehydrated ethanol solution that is the citric acid of 0.65M homogeneously, and then ultrasonicated at 25k Hz for 1h to mix uniformly to obtain a mixed solution.

[0039] C. Stir the mixed solution obtained in step B at room temperature under the condition of magnetic stirring for 10 h. Then, rotary evaporation was carried out at 60° C. in a vacuum environment until the solvent was evaporated to dryness to obtain a catalyst precursor.

[0040] D. Dry the catalyst precursor obtained in step C at 100°C for 12h, and then calcinate it in a muffle furnace at 900°C fo...

Embodiment 3

[0044]Step A dissolves 8.66g of lanthanum nitrate in 25ml of absolute ethanol, and others are the same as in Example 1;

[0045] Step B-D is also with embodiment 1, obtains catalyst Rh / 0.95La 2 Ti 2 o 7 -0.05La 2 Zr 2 o 7 . The loaded amount of Rh was measured to be 1.30 wt.% by ICP.

[0046] The performance in different temperature stages in the reaction of methane dry reforming to synthesis gas was measured by the method of implementation 1, and the results are shown in Table 1-3.

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Abstract

The invention provides a special catalyst for a reaction for preparing synthesis gas through dry reforming of methane, and a preparation method thereof, wherein the catalyst has a chemical formula Rh / xLa2Ti2O7-yLa2Zr2O7 (x is 0-1, y is 0-1, and x+y is 1), Rh is an active component and accounts for 1.0-2.0% by mass, and the catalyst has performances of high-temperature sintering resistance, carbondeposition resistance and high selectivity. According to the present invention, with the application of the catalyst in a reaction for preparing synthesis gas through dry reforming of methane, when the reaction temperature is 800 DEG C, the service life of the catalyst is as long as 110 h and has no inactivation trend, the conversion rate of methane is kept at about 90%, the conversion rate of carbon dioxide is kept at more than 85%, and the H2 / CO ratio of the product is stabilized at about 0.93 and has no reduction trend; and the catalyst can effectively solve the problems of high-temperaturesintering and carbon deposition of the catalyst in the reaction for preparing synthesis gas through dry reforming of methane.

Description

Technical field: [0001] The invention belongs to the field of methane dry reforming and corresponding catalyst development, in particular to a catalyst specially used in the reaction process of methane and carbon dioxide dry reforming to produce synthesis gas and a preparation method thereof. Background technique: [0002] As the smallest molecule in organic compounds, methane is widely distributed in nature and is also an important chemical raw material and fuel. It not only has abundant natural reserves, but also can be obtained through various ways such as chemical synthesis, bacterial decomposition, and animal digestion. In addition, methane is a greenhouse gas, and the excessive emission of methane caused by the continuous growth of population is one of the common problems faced by human society. Therefore, reforming methane into more valuable synthesis gas (H 2 and CO) are of great significance. [0003] The technical route of methane reforming mainly includes the f...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/63C01B3/40
CPCB01J23/002B01J23/63B01J2523/00C01B3/40C01B2203/0238B01J2523/3706B01J2523/47B01J2523/48B01J2523/822Y02P20/52
Inventor 姚元根吴娟周张锋乔路阳覃业燕宗珊珊崔国静许东杰
Owner FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
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