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Catalyst for low-temperature water-gas-shift reaction under hydrogenous reformed gas and preparation method thereof

A technology for converting catalysts and water gas, applied in catalyst activation/preparation, chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, etc., can solve the problems of reducing gold content, catalytic activity reduction, high gold content, etc. , to achieve the effect of increasing the contact interface concentration, reducing the catalytic activity, and improving the catalytic activity

Inactive Publication Date: 2012-12-26
FUZHOU UNIV
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  • Abstract
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  • Application Information

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Problems solved by technology

Due to many defects in the traditional low-temperature water-gas shift catalyst, it is difficult to meet the requirements of fuel cells, so it is necessary to develop a new type of high-efficiency low-temperature water-gas shift catalyst
[0003] Nano-gold catalysts are a new generation of low-temperature water-gas shift catalysts that have been studied more in recent years. The relatively mature ones are Au / Fe 2 o 3 , Au / CeO 2 series of catalysts, but the catalysts of these two systems have many shortcomings: firstly, the gold content is high, and the Au / Fe which has been reported to have better low-temperature water gas catalytic activity 2 o 3 , Au / CeO 2 The gold content of the catalyst is 3-5% (Appl. Catal. B, 2010, 95, 57; Gold. Bull., 2002, 35, 82), and some even reach 8% (CN 1748863A). The cost of the catalyst is mainly The use of a large amount of Au is spent, so the application and promotion of nano-gold catalysts is urgent to reduce the content of gold used to reduce the cost of the catalyst
Secondly when Au / Fe 2 o 3 , Au / CeO 2 When these two catalysts are used in hydrogen-rich reformed gas conditions, the catalytic activity is greatly reduced, and serious deactivation problems will occur (J. Phys. Chem. C, 2007, 111, 16927), so it is difficult to apply to real fuel cell operating environment

Method used

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  • Catalyst for low-temperature water-gas-shift reaction under hydrogenous reformed gas and preparation method thereof
  • Catalyst for low-temperature water-gas-shift reaction under hydrogenous reformed gas and preparation method thereof
  • Catalyst for low-temperature water-gas-shift reaction under hydrogenous reformed gas and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0025] Take 60 mL of 0.4 mol / L Zr(NO 3 ) 4 ·5H 2 O aqueous solution was put into a 100 mL high-pressure polytetrafluoroethylene lining, and then the lining was put into a stainless steel outer lining, and after tightening, it was placed in a blast drying oven. Heating at 130 °C for 24 h. After the hydrothermal kettle is lowered to room temperature, pour out the precipitate in the lining, add a few drops of 25% concentrated ammonia water to the precipitate, adjust the pH of the system to 6, and then centrifugally wash the precipitate several times, and detect the absence of Cl by AgNO3. -1 until. The resulting precipitate was dried at 80 °C for 24 h, and then calcined in a muffle furnace at 200 °C for 6 h to obtain the desired ZrO 2 carrier. Take 2 g ZrO 2 Support preparation Au / ZrO 2 catalyst. First, 0.52 mL of 0.2 mol / L chloroauric acid solution was added dropwise to the ultrasonically dispersed ZrO 2 Carrier emulsion (ZrO 2 The carrier is dispersed in a certain amo...

Embodiment 2

[0027] Take 60 mL of 0.4 mol / L ZrO (NO 3 ) 2 2H 2 O aqueous solution was put into a 100 mL high-pressure polytetrafluoroethylene lining, and then the lining was put into a stainless steel outer lining, and after tightening, it was placed in a blast drying oven. Heat at 190°C for 3 h. After the hydrothermal kettle is lowered to room temperature, pour out the precipitate in the inner lining, add a few drops of 25% concentrated ammonia water to the precipitate, adjust the pH of the system to 10, then centrifugally wash the precipitate several times, and detect the absence of Cl by AgNO3 -1 until. The resulting precipitate was dried at 150 °C for 5 h, and then calcined in a muffle furnace at 550 °C for 2 h to obtain the desired ZrO 2 carrier. Take 2 g ZrO2 Support preparation Au / ZrO 2 catalyst. First, 0.52 mL of 0.2 mol / L chloroauric acid solution was added dropwise to the ultrasonically dispersed ZrO 2 Carrier emulsion (ZrO 2 The carrier is dispersed in a certain amount ...

Embodiment 3

[0029] Take 60 mL of 0.4 mol / L ZrOCl 2 ·8H 2 O aqueous solution was put into a 100 mL high-pressure polytetrafluoroethylene lining, and then the lining was put into a stainless steel outer lining, and after tightening, it was placed in a blast drying oven. Heating at 150 °C for 6 h. After the hydrothermal kettle is lowered to room temperature, pour out the precipitate in the lining, add a few drops of 25% concentrated ammonia water to the precipitate, adjust the pH of the system to 8.8, and then centrifugally wash the precipitate for several times, and detect the absence of Cl by AgNO3 -1 until. The resulting precipitate was dried at 120 °C for 8 h, and then calcined in a muffle furnace at 350 °C for 4 h to obtain the desired ZrO 2 carrier. Take 2 g ZrO 2 Support preparation Au / ZrO 2 catalyst. First, 0.52 mL of 0.2 mol / L chloroauric acid solution was added dropwise to the ultrasonically dispersed ZrO 2 Carrier emulsion (ZrO 2 The carrier is dispersed in a certain amou...

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Abstract

The invention relates to a catalyst for a low-temperature water-gas-shift reaction under a hydrogenous reformed gas and a preparation method thereof. The catalyst of the invention comprises the following component in percentage by weight: 0.1 to 3 percent of aurum (Au) and 97 to 99.9 percent of zirconium oxide (ZrO2), wherein the Au is an active component; and the ZrO2 is a carrier. The ZrO2 carrier prepared by the method has larger specific surface area and larger pore volume, so the active component Au can be dispersed better. The catalyst of the invention still has higher low-temperature water-gas-shift catalytic activity under the condition of lower Au mass content, for example, when the Au weight content reduced to 1 percent, the carbon monoxide (CO) conversion rate of the Au / ZrO2 catalyst is still near the balance conversion rate at the temperature of between 210 and 300 DEG C. The catalyst of the invention has the advantages of wide using conditions and particular suitability for a high airspeed hydrogenous reformed gas atmosphere.

Description

technical field [0001] The invention relates to a low-temperature water-gas shift catalyst, in particular to a low-temperature water-gas shift catalyst applied to hydrogen-rich reformed gas and a preparation method thereof. Background technique [0002] Water-Gas-Shift Reaction (Water-Gas-Shift Reaction, CO + H 2 O → CO + H 2 ) is an important reaction process widely used in the chemical industry. It is mainly used to purify synthesis gas and provide a clean source of hydrogen for ammonia synthesis. The core of water gas shift reaction lies in the research and development of water gas shift catalyst. In recent years, due to the important application of low-temperature water-gas shift reaction in proton membrane fuel cells (PEMFC) and phosphoric acid fuel cells (PAFC), the research and development of new low-temperature water-gas shift catalysts has once again attracted extensive attention of researchers from all over the world. Proton membrane fuel cells have high require...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/52B01J21/06B01J37/18C01B3/58
Inventor 郑起张燕杰曹彦宁詹瑛瑛林性怡陈崇启
Owner FUZHOU UNIV
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