Nickel-based composite catalyst for methane reforming with carbon dioxide to produce synthesis gas under pressurization

A composite catalyst and carbon dioxide technology, applied in metal/metal oxide/metal hydroxide catalyst, physical/chemical process catalyst, hydrogen/synthesis gas production, etc., can solve the problem that the reforming methane reaction cannot continue and is difficult to achieve commercialization Application, rapid catalyst deactivation and other problems, to achieve the effect of inhibiting carbon deposition, increasing dispersion and surface active metal content, and improving catalytic activity and stability

Active Publication Date: 2018-10-09
SHAANXI NORMAL UNIV
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] Catalyst systems for reforming methane with carbon dioxide are mainly divided into two categories, one is catalysts with noble metals (Pt, Rh, Ru, Pd, Ir) as active components, although such catalysts have high activity, selectivity and stability, but Its sources are limited, expensive, and difficult to achieve commercial application
[0005] The inventor's research group (Ind.Eng.Chem.Res.2014,53,19077-19086; Int.J.ofHydrogen Energy 2014,39,11592-11605) used carboxylic acid or amino acid as complexing agent, and used combustion decomposition Ni/SiO 2 The catalyst is used for the pressurized carbon dioxide reforming methane reaction. When the reaction pressure is increased from 1.0atm to 10atm, after 20 hours of reaction, the carbon d

Method used

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  • Nickel-based composite catalyst for methane reforming with carbon dioxide to produce synthesis gas under pressurization

Examples

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Example Embodiment

[0021] Example 1

[0022] According to CeO 2 -La 2 O 3 CeO in composite oxide 2 with La 2 O 3 The mass ratio of 0.986g (0.17mmol) P123 with a number average molecular weight of 5800 and 2.5471g (5.867mmol) cerium nitrate hexahydrate, 1.7894g (4.132mmol) lanthanum nitrate hexahydrate were added to 20mL of absolute ethanol , stirred at room temperature for 5 hours to completely dissolve the solid, and the resulting mixture was transferred to a petri dish, covered with a perforated PE film, and then transferred to a forced air oven at 40 °C for solvent evaporation for 48 hours, followed by evaporation at 100 °C for 24 hours. Finally, the obtained xerogel was heated to 450 °C at a heating rate of 1 °C / min under the air atmosphere flowing in the tube furnace, calcined at a constant temperature for 4 hours, cooled to room temperature naturally, and ground into powder to obtain the desired CeO2 -La 2 O 3 complex oxide.

[0023] According to the catalyst composition, it is 10%...

Example Embodiment

[0024] Example 2

[0025] According to CeO 2 -Sm 2 O 3 CeO in composite oxide 2 with Sm 2 O 3 The mass ratio of 0.986g (0.17mmol) P123 with a number average molecular weight of 5800 and 2.4946g (5.746mmol) cerium nitrate hexahydrate, 1.8907g (4.254mmol) samarium nitrate hexahydrate were added to 20mL of absolute ethanol , stirred at room temperature for 5 hours to completely dissolve the solid, and the resulting mixture was transferred to a petri dish, covered with a perforated PE film, and then transferred to a forced air oven at 40 °C for solvent evaporation for 48 hours, followed by evaporation at 100 °C for 24 hours. Finally, the obtained xerogel was heated to 450 °C at a heating rate of 1 °C / min under the air atmosphere flowing in the tube furnace, calcined at a constant temperature for 4 hours, cooled to room temperature naturally, and ground into powder to obtain CeO 2 -Sm 2 O 3 complex oxide.

[0026] According to the catalyst composition, it is 10%Ni-4%CeO 2...

Example Embodiment

[0027] Example 3

[0028] According to CeO 2 -Pr 6 O 11 CeO in composite oxide 2 with Pr 6 O 11 The mass ratio of 0.986g (0.17mmol) P123 with a number average molecular weight of 5800 and 2.8836g (6.642mmol) cerium nitrate hexahydrate, 1.4606g (3.3576mmol) praseodymium nitrate hexahydrate were added to 20mL of absolute ethanol , stirred at room temperature for 5 hours to completely dissolve the solid, and the resulting mixture was transferred to a petri dish, covered with a perforated PE film, and then transferred to a forced air oven at 40 °C for solvent evaporation for 48 hours, followed by evaporation at 100 °C for 24 hours. Finally, the obtained xerogel was heated to 450 °C at a heating rate of 1 °C / min under the air atmosphere flowing in the tube furnace, calcined at a constant temperature for 4 hours, cooled to room temperature naturally, and ground into powder to obtain CeO 2 -Pr 6 O 11 complex oxide.

[0029] According to the catalyst composition, it is 10%Ni-...

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Abstract

The invention discloses a nickel-based composite catalyst for methane reforming with carbon dioxide to produce a synthesis gas under pressurization. A carrier of the catalyst is at least one selectedfrom SiO2, Al2O3 and TiO2, an active component is Ni, Ni-Fe or Ni-Co, and an auxiliary agent is one selected from composite oxides such as CeO2-La2O3, CeO2-Sm2O3, CeO2-Pr6O11, CeO2-Nd2O3 and CeO2-Y2O3; based on a mass of the catalyst of 100%, the catalyst comprises 5%-15% of the active component, 3%-15% of the auxiliary agent, and the balance of the carrier; and the catalyst is prepared by adopting a coordination-decomposition method with glycine, alanine, threonine, citric acid and oxalic acid as a coordination-combustion improver. The catalyst disclosed by the invention has a simple preparation process and lower costs, and is economic and environmentally friendly; and the catalyst has a higher methane and carbon dioxide conversion rate for methane reforming with the carbon dioxide underthe pressurization, exhibits high activity, high stability and extremely high resistance to carbon deposition and sintering.

Description

technical field [0001] The invention belongs to the technical field of catalysts, and in particular relates to a nickel-based composite catalyst used for carbon dioxide reforming methane to produce synthesis gas under pressurized conditions. Background technique [0002] In recent years, with the deepening of people's understanding of the greenhouse effect, CO, one of the strongest greenhouse gases, 2 The capture of and its applications have attracted increasing attention. Carbon dioxide reforming of methane can simultaneously utilize CO 2 and CH 4 The two major greenhouse gases are of great significance to the reduction of greenhouse gas emissions, and the H of syngas 2 / CO≤1, it can be used as raw material gas for the synthesis of carbonyl and organic oxygen-containing compounds. Since Ashcroft et al. (Nat.Chem., 1991, 352:225-226) reported the research on reforming methane with carbon dioxide, reforming methane with carbon dioxide has attracted extensive attention of ...

Claims

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Application Information

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IPC IPC(8): B01J23/83C01B3/40
CPCB01J23/002B01J23/83B01J2523/00C01B3/40C01B2203/0238C01B2203/1058B01J2523/3706B01J2523/3712B01J2523/41B01J2523/3737B01J2523/3718B01J2523/3725B01J2523/36Y02P20/52
Inventor 刘忠文肖勇山宋永红李婷石先莹刘昭铁
Owner SHAANXI NORMAL UNIV
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