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Method for improving surface oxygen vacancy concentration of CeO2 catalyst and application

A catalyst, surface oxygen technology, applied in physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, chemical instruments and methods, etc. The effect of surface oxygen vacancy concentration, simple operation

Pending Publication Date: 2022-07-12
KUNMING UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Thus, it can be seen that the above method does not make CeO 2 Oxygen vacancies are significantly enhanced

Method used

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  • Method for improving surface oxygen vacancy concentration of CeO2 catalyst and application
  • Method for improving surface oxygen vacancy concentration of CeO2 catalyst and application
  • Method for improving surface oxygen vacancy concentration of CeO2 catalyst and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0022] Example 1: Spherical ceria (CeO 2 -NS) catalysts were separated by H 2 -H 2 S mixture and H 2 In-situ XPS (In-situ XPS) characterization after atmosphere treatment

[0023] CeO was prepared by hydrothermal synthesis 2 -NS: 2g of cerium nitrate hexahydrate was dissolved in 2mL of deionized water, and then 2mL of glacial acetic acid was added. After the solution was evenly mixed, 52mL of ethylene glycol was added and stirred for 30min; Put it into a stainless steel reaction kettle of vinyl fluoride, and then put it into an oven at 180 ° C for 200 minutes; after the above process is over, take the sediment in the reaction kettle for centrifugal cleaning (deionized water three times, and absolute ethanol three times); The cleaned product was dried in an oven at 60°C for 12h; then the dried product was put into a crucible and calcined at 400°C for 4h in a muffle furnace to obtain spherical ceria CeO 2 -NS.

[0024] CeO 2 Ce on catalyst 3+ and active adsorbed oxygen s...

Embodiment 2

[0027] Example 2: CeO without any treatment 2 -NS catalyst and via H 2 -H 2 CeO treated with S mixed gas 2 -NS catalyst for low concentration H 2 Preparation of Syngas from Methane and Carbon Dioxide in S Atmosphere

[0028] Take the CeO without any pretreatment in Example 1 2 -NS catalyst is put into the tube furnace reactor after tableting treatment, and the reaction gas is CH 4 Concentration is 25%, CO 2 The concentration is 25%, and the balance gas is N 2 ; The reaction space velocity is 60000mL / g·h, and the reaction temperature is 800℃;

[0029] At the same time, the H 2 -H 2 S mixed gas (H 2 10%, H 2 S100ppm, carrier gas N 2 ) CeO after reduction treatment for 1h 2 -NS catalyst is put into the tube furnace reactor after tableting treatment, and the reaction gas introduced is: CH 4 Concentration is 25%, CO 2 Concentration is 25%, H 2 The concentration of S is 100ppm, and the balance gas is N 2 ; The reaction space velocity is 60000mL / g·h, and the reaction...

Embodiment 3

[0031] Example 3: CeO without any treatment 2 -NS catalyst and via H 2 -H 2 CeO treated with S mixed gas 2 -NS catalyst for low concentration H 2 Preparation of Syngas and Propylene from Propane and Carbon Dioxide in S Atmosphere

[0032] The unpretreated CeO prepared in Example 1 was 2 -NS catalyst is put into the tube furnace reactor after tableting treatment, and the reaction gas introduced is: C 3 H 8 Concentration is 25%, CO 2 The concentration is 25%, and the balance gas is N 2 . The reaction space velocity is 24000mL / g·h, and the reaction temperature is 550℃;

[0033] At the same time, the H 2 -H 2 S mixed gas (H 2 10%, H 2 S100ppm, carrier gas N 2 ) CeO after reduction treatment for 1h 2 -NS catalyst is put into the tube furnace reactor after tableting treatment, and the reaction gas introduced is: C 3 H 8 Concentration is 25%, CO 2 Concentration is 25%, H 2 The concentration of S is 100ppm, and the balance gas is N 2 . The reaction space velocity ...

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Abstract

The invention discloses a method for improving the surface oxygen vacancy concentration of a CeO2 catalyst, which comprises the following steps: carrying out synergistic reduction treatment on CeO2 at 500-800 DEG C by using H2-H2S mixed gas to prepare the CeO2 catalyst with high oxygen vacancy concentration, the CeO2 catalyst prepared by the method disclosed by the invention is applied to preparation of synthesis gas by catalyzing low-carbon alkane and carbon dioxide, and experimental results show that the CeO2 catalyst subjected to H2S and H2 co-treatment not only generates more oxygen vacancies for activating reactant molecules to promote forward proceeding of the reaction, so that the conversion rate of the low-carbon alkane and the carbon dioxide is obviously improved; h2S fed in the reaction does not cause sulfur poisoning and inactivation of the catalyst, which shows that the CeO2 catalyst cooperatively treated by H2S and H2 has excellent sulfur resistance; the method disclosed by the invention is simple, efficient, stable, simple and safe to operate and good in application prospect; the method is suitable for industrial production and market popularization and application.

Description

technical field [0001] The invention belongs to the technical field of energy functional materials, and in particular relates to a method for improving CeO 2 Method for the concentration of oxygen vacancies on the catalyst surface. Background technique [0002] CeO 2 Abundant crystalline oxygen defects (oxygen vacancies) and high oxygen storage capacity have attracted extensive attention from academia and industry. It relies on the rapid redox cycling ability of its own cerium ions to create "oxygen vacancies", as shown in reaction formula I. Oxygen vacancies can store and release oxygen, Ce in a reducing gas 4+ ions are reduced to Ce 3+ The ions in turn release oxygen, and in the oxidizing gas Ce 3+ ions are oxidized to Ce 4+ The ions in turn store oxygen. In recent years, CeO with oxygen vacancies 2 It can be widely used as catalyst or catalyst carrier for CO oxidation, CO 2 Heterogeneous catalysis fields such as reduction, solid oxide fuel cells, electrocatalysis...

Claims

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Application Information

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IPC IPC(8): B01J23/10B01J37/18C01B3/40C07C5/42C07C11/06
CPCB01J23/10B01J37/18C01B3/40C07C5/42C07C11/06Y02P20/52Y02E60/50
Inventor 何德东严俊凯罗永明梅毅张磊陈定凯
Owner KUNMING UNIV OF SCI & TECH
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