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Controllable synthesis of rod-shaped beta-Mo2C and application thereof in reverse water-gas shift reaction

An inverse water vapor shift, rod-shaped technology, applied in the field of carbon dioxide catalytic conversion and utilization, can solve problems such as molybdenum carbide catalyst and non-thermal plasma that have not yet been seen, and achieve the effect of breaking through the limitation of thermodynamic equilibrium, simple preparation method and high CO2 conversion rate

Active Publication Date: 2017-12-22
DALIAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, so far, there has been no report on the application of molybdenum carbide catalysts in combination with non-thermal plasmas for reverse water vapor shift reactions.

Method used

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  • Controllable synthesis of rod-shaped beta-Mo2C and application thereof in reverse water-gas shift reaction
  • Controllable synthesis of rod-shaped beta-Mo2C and application thereof in reverse water-gas shift reaction
  • Controllable synthesis of rod-shaped beta-Mo2C and application thereof in reverse water-gas shift reaction

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0032] Example 1 One-dimensional rod-like β-Mo 2 Preparation of C and Evaluation of Simple Catalytic Activity

[0033] (1) Preparation

[0034] Dissolve 8.4g ammonium paramolybdate in 200ml deionized water and 40ml 65% HNO 3 In the mixed solution, after stirring evenly, transfer the above solution to the reaction kettle, heat at 200°C for 22 hours, and cool down naturally; centrifuge to obtain a precipitate, wash it with water several times to make it neutral, and then dry it in a blast at 60°C Stand in the box for 24 hours to obtain molybdenum trioxide with uniform rod shape.

[0035] Take 0.2g of prepared rod-like MoO 3 (40-60 mesh) samples are placed in a quartz reactor, and 20% CH 4 / H 2 (150mL / min) mixed gas, raised to 300°C at a heating rate of 5°C / min, then raised to the final carbonization temperature of 700°C at 1°C / min, and kept for 2 hours. Then after cooling down to room temperature, in 1% O 2 / Ar atmosphere passivation for 12h to obtain a one-dimensional ro...

Embodiment 2

[0058] Example 2 One-dimensional rod-like β-Mo 2 Evaluation of Catalytic Activity Synergistically with C and Cold Plasma

[0059] The reverse water vapor shift reaction was carried out in a quartz tube fixed-bed reactor with an inner diameter of 8 mm. The flow rate of each gas required for the experiment is regulated and controlled by a mass flow meter, and flows into the reactor after mixing. Weigh 10 mg of one-dimensional rod-shaped molybdenum carbide (40-60 mesh) catalyst and 0.19 g of quartz sand (40-60 mesh) and place them in a quartz tube after being evenly mixed with 15% CH 4 / H 2 The mixed gas pretreated the catalyst at 590°C for 2 hours, and then carried out the activity evaluation under the following conditions: the reaction atmosphere was CO 2 :H 2 =1:2, the gas space velocity is 1,500,000mL / g / h, the dielectric barrier (DBD) discharge center frequency is 30kHz, and the applied voltage is 40V. Under this condition, CO 2 The conversion rate is 33.4%, and the CO ...

Embodiment 3

[0071] Example 3 One-dimensional rod-like β-Mo 2 C and cold plasma synergistically catalyzed inverse water vapor shift stability test

[0072] This embodiment is an 8-hour stability test of a one-dimensional rod-shaped molybdenum carbide catalyst, and the preparation and activity evaluation test conditions of the catalyst during the process are the same as those in Example 2. It can be seen that within 8 h, the reactivity of the catalyst did not decrease significantly, as Figure 5 shown.

[0073] Table 1 shows the block molybdenum carbide (a) prepared in Comparative Example 1.1 and the one-dimensional rod-shaped β-Mo prepared in Example 1 2 The specific surface area comparison of C(b);

[0074] Table 1

[0075]

[0076] Table 2 shows the block molybdenum carbide prepared in ratio 1.1 and the one-dimensional rod-shaped β-Mo prepared in Example 1 2 Under the synergistic catalysis of C and cold plasma, the CO catalyzed inverse water vapor shift reaction at different inpu...

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Abstract

The invention discloses controllable synthesis of one-dimension rod-shaped beta-Mo2C and an application thereof in reverse water-gas shift reaction and belongs to the field of carbon-dioxide catalytic conversion and utilization. A product is CO with high additional value. The controllable synthesis comprises the steps of dissolving ammonium paramolybdate in a mixed solution of deionized water and HNO3 to obtain molybdenum trioxide with uniform and rod-shaped morphology by water heat, carrying out programmed heating and carbonization at the temperature of 590-800 DEG C in 20vt% CH4 / H2 mixed gas at the speed of 100-160ml / min to obtain molybdenum carbide with one-dimension rod-shaped morphology. Compared with molybdenum carbide deposited by nanoparticles, the molybdenum carbide with one-dimension rod-shaped morphology has higher specific surface area and larger active-center number, and has excellent CO2 conversion rate and CO selectivity in reverse water-gas shift reaction no matter under simple catalytic action or the synergistic action of cold plasma and molybdenum carbide.

Description

technical field [0001] The invention belongs to the field of catalytic conversion and utilization of carbon dioxide, and in particular relates to the single catalysis of one-dimensional rod-shaped beta-type molybdenum carbide, and the synergistic catalysis of one-dimensional rod-shaped beta-type molybdenum carbide and cold plasma to prepare carbon monoxide by reverse water-vapor shift reaction. Background technique [0002] With the growth of the global population and the acceleration of industrialization, global carbon dioxide emissions have risen sharply since the last century. In 2016 alone, global CO 2 The emissions are as high as 32.1 billion tons. Environmental problems such as seawater acidification and climate warming caused by massive emissions of carbon dioxide are becoming more and more serious, and have become one of the social problems that need to be solved urgently. At the same time, carbon dioxide is also the most abundant C1 resource in the world. Therefor...

Claims

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Application Information

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IPC IPC(8): C01B32/949C01B32/40B01J27/22
CPCB01J27/22C01P2004/03C01P2004/10
Inventor 石川于涛刘洋张晓赵琦牛量陈冰冰
Owner DALIAN UNIV OF TECH
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