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Pd-based catalyst for catalytic oxidation of methane under water-containing condition and preparation method of Pd-based catalyst

A technology of methane catalysis and catalyst, which is applied in the field of Pd-based catalyst and its preparation, can solve the problems of activity loss and catalyst deactivation, and achieve the effects of improving water resistance, improving performance, good catalytic activity and stability

Active Publication Date: 2020-11-13
CHINA NUCLEAR POWER TECH RES INST CO LTD +3
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Monai prepared Pd@ZrO2 / Si-Al2O3 catalyst, which improved the water resistance of the catalyst, but its activity was also lost (ACS Catalysis, 2014, 4(11): 3902-3909.)
Zou used PdO as the shell and NiO as the core to design a core-shell structure NiO@PdO / Al2O3 catalyst, which can complete the full conversion at 460°C under the condition of water vapor , but after a 12h stability test, the catalyst was obviously deactivated, and the conversion rate dropped from 100% to 80%

Method used

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  • Pd-based catalyst for catalytic oxidation of methane under water-containing condition and preparation method of Pd-based catalyst
  • Pd-based catalyst for catalytic oxidation of methane under water-containing condition and preparation method of Pd-based catalyst

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preparation example Construction

[0030] The preparation method of Pd-based catalyst of the present invention may comprise the following steps:

[0031] S1. Preparation of core-shell structure NO@HZ.

[0032] The preparation of NO@HZ is as follows: using NO nitrate, sodium metaaluminate, silica sol and template as raw materials, NO@HZ with core-shell structure was prepared by one-step hydrothermal synthesis.

[0033] S2. Disperse the core-shell structure NO@HZ in the first solvent, add the precursor solution of MO, and proceed through stirring, centrifugation, drying and roasting in sequence to synthesize MO / NO@HZ.

[0034] The first solvent can be deionized water. The precursor of MO is one of nitrate, acetate and hydrochloride.

[0035] S3. Dispersing MO / NO@HZ in the second solvent to form a mixed solution, adding PdO precursor solution, stirring, centrifuging, drying and roasting in sequence to synthesize PdO-MO / NO@HZ.

[0036]Wherein, the precursor of PdO is one of nitrate, hydrochloride, acetate and ac...

Embodiment 1

[0040] Preparation of core-shell structure: use tetrapropylammonium hydroxide as a template to combine silica-alumina ZSM-5 molecular sieve, and the ratio of each raw material and its mass is 1.0SiO 2 :0.O4Al 2 o 3 :0.1NaOH:0.1TPAOH:20H 2 O.

[0041] Add 10g of sodium hydroxide solution into the flask at room temperature, add the corresponding mass of silica sol after it is completely dissolved, stir until it is completely hydrolyzed, and then add the corresponding amount of NaAlO 4 solution, stirred for 1 h to obtain a mixed solution. The Zr precursor solution was added dropwise to the mixed solution, wherein the molar ratio Zr:Al=1:10, stirred for 30 minutes, transferred to a high-pressure hydrothermal kettle, and placed in an oven at 170°C for 96h. The solid product treated by the hydrothermal method was centrifuged, washed 5 times with water and ethanol, and then dried overnight in an oven at 80° C. to obtain a solid powder. The solid powder was calcined at 550°C in s...

Embodiment 2

[0044] Identical to embodiment 1 makes ZrO 2 @ZSM-5 powder.

[0045] ZrO 2 @ZSM-5 is used as a carrier, ferric nitrate is used as a precursor, the catalyst is prepared in the same way as in Example 1, and PdO-FeOx / ZrO is obtained by centrifugation, drying, roasting, and sieving 2 @ZSM-5 Catalyst.

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Abstract

The invention discloses a Pd-based catalyst for catalytic oxidation of methane under a water-containing condition and a preparation method of the Pd-based catalyst. The Pd-based catalyst is PdO-MO / NO@HZ, wherein NO@HZ is of a hydrophobic core-shell structure, NO is a shell, and HZ is a core; MO and NO are different metal oxides; and HZ is a molecular sieve. The Pd-based catalyst disclosed by the invention is used for catalytic oxidation of methane under a water-containing condition, and still has good catalytic activity and stability in the presence of water vapor, so the water resistance of the catalyst is effectively improved, and the performance of the catalyst is improved.

Description

technical field [0001] The invention relates to the technical field of catalysts, in particular to a Pd-based catalyst for catalytic oxidation of methane under water-containing conditions and a preparation method thereof. Background technique [0002] Methane is used as natural gas, shale gas, biogas, etc. C 1 The main component of resources has the characteristics of abundant reserves and renewable properties. According to the "China Mineral Resources Report (2019)" data, my country's natural gas reserves are as high as 5,793.608 billion cubic meters, and shale gas reserves have also reached 216.02 billion cubic meters. With the continuous development and exploration of the utilization of methane resources, it has been applied in the production of methanol and its derivatives from methane, the synthesis of ammonia and urea from methane; in addition, methane is also mostly used in city gas, industrial fuel and automobile transportation power fuel. [0003] When methane is ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/46B01D53/86B01D53/72
CPCB01J29/46B01D53/864B01D2257/7025Y02C20/20
Inventor 王超郭耘白杉王丽葛云瑞赵瑞玲顾林峰韩玉峰
Owner CHINA NUCLEAR POWER TECH RES INST CO LTD