Highly stable defect state cerium-zirconium double metal oxide catalyst, preparation method and application thereof

A dual-metal oxide and defect state technology, which is applied in metal/metal oxide/metal hydroxide catalysts, catalyst activation/preparation, physical/chemical process catalysts, etc., can solve kinetic difficulties, complex operations, and energy consumption High-level problems, to achieve high-efficiency methane dehydrogenation coupling, high atom utilization, and reduce environmental pollution

Active Publication Date: 2022-03-18
JILIN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the indirect conversion process requires high energy consumption, complicated operation and high cost.
Thermocatalytic direct conversion of methane to its derivatives such as methanol is thermodynamically feasible but kinetically difficult
In addition, methanol or other derivative chemicals and intermediates in the reaction process are less than CH 4 The reactivity is higher, so the target product needs to be kinetically protected or selectively separated, which brings great difficulties to the actual production

Method used

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  • Highly stable defect state cerium-zirconium double metal oxide catalyst, preparation method and application thereof
  • Highly stable defect state cerium-zirconium double metal oxide catalyst, preparation method and application thereof
  • Highly stable defect state cerium-zirconium double metal oxide catalyst, preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0037] Example 1: Preparation method of cerium-zirconium double metal oxides with different cerium-zirconium ratios and its application in photocatalytic methane dehydrogenation coupling reaction

[0038] (1) Preparation of cerium-zirconium double metal oxide: Weigh commercial cerium nitrate hexahydrate, zirconium oxynitrate hydrate, and glycine in a small beaker with a molar ratio of 3:7:10. After uniformity, the solution was transferred to an evaporating dish, evaporated to dryness at 90°C, and then heated to 170°C, the mixture released heat and spontaneously ignited to obtain a light yellow sample of cerium-zirconium double metal oxide, marked as C 3 Z 7 ; Afterwards, the catalyst is used in the methane dehydrogenation coupling reaction.

[0039] (2) Weigh 50 mg of catalyst into a 10 mL small beaker, disperse it evenly with acetone, place it in a 70°C oven to evaporate the solvent, and obtain a catalyst with a uniform surface, put the catalyst into a quartz reactor, and pl...

Embodiment 2

[0040] Example 2: Preparation method of cerium-zirconium double metal oxides with different cerium-zirconium ratios and its application in photocatalytic methane dehydrogenation coupling reaction

[0041] (1) Preparation of cerium-zirconium double metal oxide: Weigh 4 mmol of commercial cerium nitrate hexahydrate, zirconium oxynitrate hydrate, and glycine in a molar ratio of 4:6:10 in a small beaker, add 10 mL of deionized water, and stir magnetically After uniformity, the solution was transferred to an evaporating dish, evaporated to dryness at 90°C, and then heated to 170°C, the mixture released heat and spontaneously ignited to obtain a light yellow sample of cerium-zirconium double metal oxide, marked as C 4 Z 6 ; Afterwards, the catalyst is used in the methane dehydrogenation coupling reaction.

[0042] (2) Weigh 50 mg of catalyst into a 10 mL small beaker, disperse it evenly with acetone, place it in a 70°C oven to evaporate the solvent, and obtain a catalyst with a uni...

Embodiment 3

[0043] Example 3: Preparation method of cerium-zirconium double metal oxides with different cerium-zirconium ratios and its application in photocatalytic methane dehydrogenation coupling reaction

[0044] (1) Preparation of cerium-zirconium double metal oxide: Weigh commercial cerium nitrate hexahydrate, zirconium oxynitrate hydrate, and glycine in a small beaker with a molar ratio of 5:5:10. After uniformity, the solution was transferred to an evaporating dish, evaporated to dryness at 90°C, and then heated to 170°C, the mixture released heat and spontaneously ignited to obtain a light yellow sample of cerium-zirconium double metal oxide, labeled as CZ; after that, the catalyst was used for methane removal Hydrogen coupling reaction.

[0045] (2) Weigh 50 mg of catalyst into a 10 mL small beaker, disperse it evenly with acetone, place it in a 70°C oven to evaporate the solvent, and obtain a catalyst with a uniform surface, put the catalyst into a quartz reactor, and place the...

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Abstract

A high-stable defect-state cerium-zirconium double metal oxide catalyst, a preparation method and its application in light-driven methane molecular dehydrogenation coupling reactions belong to the technical field of methane dehydrogenation coupling. The present invention utilizes reducing metal powder to treat cerium-zirconium bimetallic oxide in a hydrogen atmosphere, and can obtain strongly basic anion-deficient state cerium-zirconium bimetallic oxide by controlling the ratio of cerium-zirconium bimetallic oxide and reducing metal powder material catalyst. The existence of inherent defects and adjustable strong basic sites can make the cerium-zirconium bimetallic oxide effectively adsorb and weaken the C-H bond in methane molecules, and realize the efficient dehydrogenation coupling of methane molecules driven by light at room temperature. The catalyst of the present invention drives methane activation by light, has high efficiency, energy saving, environmental protection, and high atom utilization rate. The design and construction of nano-catalysts and the modification of catalysts can achieve efficient methane dehydrogenation coupling under mild conditions, which can reduce energy consumption and reduce environmental pollution.

Description

technical field [0001] The invention belongs to the technical field of methane dehydrogenation coupling, and in particular relates to a highly stable defect state cerium-zirconium bimetallic oxide catalyst, a preparation method and its application in light-driven methane molecular dehydrogenation coupling reaction. Background technique [0002] Methane is the main component of natural gas and combustible ice. With the depletion of oil reserves, it will play an increasingly important role in energy upgrading and various chemical production processes; at the same time, the development of hydraulic fracturing technology and the development of shale gas Development and utilization have greatly increased the recoverable reserves and supply of natural gas. Therefore, synthesis processes of high value-added chemicals from methane are becoming more and more economically attractive. However, most of the methane is used to burn heat and generate electricity, the utilization rate of a...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J23/10B01J35/00B01J37/16B01J37/18C07C2/76C07C9/06
CPCB01J23/10B01J23/002B01J37/16B01J37/18B01J35/004C07C2/76C07C9/06
Inventor 李路王光明
Owner JILIN UNIV
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