Sulfur-tolerant shift methanation integrated catalyst and preparation method thereof

A sulfur-resistant shift, catalyst technology, applied in catalyst activation/preparation, physical/chemical process catalyst, metal/metal oxide/metal hydroxide catalyst, etc., can solve problems such as retention, unindustrial application, etc. Low cost, low preparation cost, and the effect of increasing calorific value

Active Publication Date: 2019-04-16
CHINA PETROLEUM & CHEM CORP
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] China began to develop sulfur-resistant methanation catalysts in the 1980s. Research institutes such as Dalian Institute of Chemical Physics, University of Science and Technology of China, and Shanghai Gas Research Institute developed a batch of catalysts in the 1990s, but most of them only stayed at the scale of "upgrading" experimental devices , have not been applied industrially

Method used

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  • Sulfur-tolerant shift methanation integrated catalyst and preparation method thereof
  • Sulfur-tolerant shift methanation integrated catalyst and preparation method thereof
  • Sulfur-tolerant shift methanation integrated catalyst and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0031] (1) Dissolve 15.8 g of ammonium heptamolybdate with 40 mL of deionized water to obtain a clear solution A.

[0032] (2) Add 7.8g of cobalt nitrate, 4.6g of cerium nitrate, 3g of oxalic acid and 1mL of dilute nitric acid into 15mL of deionized water respectively to obtain solution B;

[0033] (3) Dry mix 98g of metatitanic acid, 14g of 80# calcium aluminate, and 3g of Tianqing powder, add solutions A and B respectively, knead evenly, form, dry naturally, and roast at 550°C to prepare a semi-finished catalyst.

[0034] (4) place the catalyst semi-finished product in the airtight reactor, with 500h -1 Air mixture containing 0.2% hydrogen sulfide was introduced at space velocity and maintained at 200°C for 10 hours, and then the temperature was lowered to room temperature to obtain finished catalyst C1. Its strength, pore structure and catalytic activity data are shown in Tables 1 and 2.

Embodiment 2

[0036] (1) Dissolve 18.5 g of ammonium tetramolybdate with 50 mL of deionized water to obtain clear solution A.

[0037] (2) Add 2.2g of cobalt nitrate, 2.5g of lanthanum nitrate, and 4g of citric acid into 15mL of deionized water to obtain solution B;

[0038] (3) Dry mix 75.6g of metatitanic acid, 30g of 85# calcium aluminate, and 2g of starch, add solutions A and B respectively, knead evenly, shape, dry naturally, and roast at 700°C to obtain a semi-finished catalyst.

[0039] (4) place the catalyst semi-finished product in the airtight reactor, with 1000h -1 Air mixture containing 0.1% hydrogen sulfide was introduced at space velocity and maintained at 150° C. for 15 hours, and then the temperature was lowered to room temperature to obtain finished catalyst C2. Its strength, pore structure and catalytic activity data are shown in Tables 1 and 2.

Embodiment 3

[0041] (1) Dissolve 9.8 g of ammonium heptamolybdate with 35 mL of deionized water to obtain a clear solution A.

[0042] (2) Add 16.0 g of cobalt nitrate, 3.6 g of yttrium nitrate, 3 g of oxalic acid and 2 mL of acetic acid into 20 mL of deionized water respectively to obtain solution B.

[0043] (3) Dry mix 74g of anatase, 13g of 75# calcium aluminate, and 6g of Tianqing powder, add solutions A and B respectively, knead evenly, form, dry naturally, and roast at 650°C to obtain a semi-finished catalyst.

[0044] (4) place the catalyst semi-finished product in the airtight reactor, with 200h -1 Air mixture containing 0.3% hydrogen sulfide was introduced at space velocity, maintained at 150°C for 20 hours, and then the temperature was lowered to room temperature to obtain finished catalyst C3. Its strength, pore structure and catalytic activity data are shown in Tables 1 and 2.

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Abstract

The invention relates to a catalyst of a sulfur-tolerant shift methanation reaction for preparing syngas by using residual oil, heavy oil, petroleum coke, coal and other heavy raw materials, particularly to a sulfur-tolerant shift methanation integrated catalyst and a preparation method thereof, wherein the sulfur-tolerant shift methanation integrated catalyst comprises active components, carriersand an auxiliary agent, and is prepared by using cobalt sulfide and molybdenum sulfide as active components, using titanium oxide and calcium aluminate as carriers and using a rare earth aid as an auxiliary agent through a mixing kneading method. According to the present invention, the active components are not easily lost in the carriers, the structure and the activity stability of the catalystare good, the catalyst can adapt to the conditions of high pressure, high space velocity and low water-gas ratio, the sulfur-tolerant shift reaction and the methanation reaction can be simultaneouslycarried out while the hydrogen gas and the methane product can be simultaneously obtained, the methanation reaction has a low activation temperature, and the preparation method has advantages of simple process and low preparation cost.

Description

technical field [0001] The invention relates to a catalyst for the sulfur-resistant shift methanation reaction of producing synthesis gas from heavy raw materials such as residual oil, heavy oil, petroleum coke, coal, etc., in particular to an integrated sulfur-resistant shift methanation catalyst and a preparation method. Background technique [0002] At present, the generally adopted technological process for producing a small amount of low calorific value fuel gas by-product of coal gasification hydrogen production unit is to set up conversion line and non-transformation line to meet the refinery’s demand for hydrogen and fuel gas respectively, but the investment of the device is large and the fuel gas heat The value is low, and the demand for hydrogen and fuel gas cannot be switched flexibly. If the methanation process is embedded in the conversion section, the non-transformation line is canceled to perform conversion and methanation reactions at the same time, after the...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/051B01J37/08B01J37/20B01J35/10C10L3/08
CPCC10L3/08B01J23/002B01J27/0515B01J35/002B01J35/1019B01J35/1038B01J37/0018B01J37/20B01J2523/00B01J2523/23B01J2523/31B01J2523/3712B01J2523/47B01J2523/3706B01J2523/36
Inventor 赵庆鲁余汉涛田兆明白志敏齐焕东陈依屏李文柱
Owner CHINA PETROLEUM & CHEM CORP
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