Study on intrinsic kinetics of CO<sub>2</sub> methanation on Ni/CeO<sub>2</sub> catalyst

FAN Zhihui; YUE Yanyan; ZHANG Xiaonan; LI Xinli; ZHANG Shaokang; ZHANG Zhenzhou; TU Weifeng; HAN Yifan

doi:10.12434/j.issn.2097-2547.20240104

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Study on intrinsic kinetics of CO₂ methanation on Ni/CeO₂ catalyst

- Study on intrinsic kinetics of CO₂ methanation on Ni/CeO₂ catalyst
- Vol. 49, Issue 8, Pages: 123-130(2024)
- 作者机构：
  
  郑州大学化工学院，河南郑州 450001
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20240104
  CLC： TQ211;TQ426
- Published：25 August 2024，
  
  Received：15 March 2024，
  
  Revised：21 April 2024，
- 稿件说明：
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范志辉,岳燕燕,张笑楠等.Ni/CeO₂催化剂上CO₂甲烷化反应本征动力学研究[J].低碳化学与化工,2024,49(08):123-130.

FAN Zhihui,YUE Yanyan,ZHANG Xiaonan,et al.Study on intrinsic kinetics of CO₂ methanation on Ni/CeO₂ catalyst[J].Low-carbon Chemistry and Chemical Engineering,2024,49(08):123-130.
范志辉,岳燕燕,张笑楠等.Ni/CeO₂催化剂上CO₂甲烷化反应本征动力学研究[J].低碳化学与化工,2024,49(08):123-130. DOI： 10.12434/j.issn.2097-2547.20240104.

FAN Zhihui,YUE Yanyan,ZHANG Xiaonan,et al.Study on intrinsic kinetics of CO₂ methanation on Ni/CeO₂ catalyst[J].Low-carbon Chemistry and Chemical Engineering,2024,49(08):123-130. DOI： 10.12434/j.issn.2097-2547.20240104.

摘要

加氢合成CH

（CO

甲烷化）是CO

高效、清洁转化的重要途径之一。尽管CO

甲烷化的催化体系研究已较深入，但特定条件下CO

甲烷化本征动力学的研究较少。采用燃烧法制备了Ni/CeO

催化剂（Ni质量分数为10%），并通过加入内稀释剂（

-Al

）制备了不同

(

-Al

(Ni/CeO

)的样品。考察了在温度为300 ℃、压力为1 MPa和空速为3 × 10

mL/(g·h)的条件下，

(

-Al

(Ni/CeO

) = 25:1样品（样品A）的CO

甲烷化本征动力学。结合本征动力学测试、漫反射红外光谱、H

-程序升温还原和H

-程序升温脱附等对CO

甲烷化本征反应动力学方程进行了深入分析。结果表明，样品A作用下的CH

生成速率最高可达41.4 mmol/(g·h)（H

分压为400 kPa，CO

分压为120 kPa）。当CO

分压为30~120 kPa时，CH

生成速率随H

分压的增大线性增长，并且不受CO

分压或CO分压变化的影响。在该CO

分压范围内，富氢环境可以显著提高催化剂的CO

甲烷化催化活性。

Abstract

Hydrogenation of CO

to synthesize CH

(CO

methanation) is one of the crucial pathways for the efficient and clean conversion of CO

. Despite extensive researches on the catalytic system for CO

methanation

the intrinsic kinetics of CO

methanation under specific conditions have not been thoroughly investigated. Ni/CeO

catalyst (Ni mass fraction of 10%) was prepared using the combustion method

and samples with varying

(

-Al

(Ni/CeO

) were produced by incorporating

-Al

as the internal diluent. The intrinsic kinetics of CO

methanation of sample A with

(

-Al

(Ni/CeO

) = 25:1 were examined

under the conditions of temperature of 300 ℃

pressure of 1 MPa and gas hourly space velocity of 3 × 10

mL/(g·h). An in-depth analysis of the kinetic equations for the intrinsic CO

methanation reaction was conducted through a combination of intrinsic kinetic tests

diffuse reflection infrared spectrum

-temperature programmed reaction and H

-temperature programmed desorption

etc. The results show that the CH

generation rate under action of sample A can reach up to 41.4 mmol/(g·h)(H

partial pressure is 400 kPa

and CO

partial pressure is 120 kPa). When CO

partial pressure is 30 kPa to 120 kPa

the CH

generation rate exhibits linear increases with the rises of the H

partial pressure

and is not affected by variation of the CO

or CO partial pressure. Within this CO

partial pressure range

the hydrogen-rich environment significantly enhances the catalytic activity of the catalyst for CO

methanation.

关键词

CO2甲烷化Ni/CeO2催化剂本征动力学

Keywords

CO2 methanationNi/CeO2 catalystintrinsic dynamics

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Study on intrinsic kinetics of CO2 methanation on Ni/CeO2 catalyst

DOI：10.12434/j.issn.2097-2547.20240104

摘要

Abstract

关键词

Keywords

references

Study on intrinsic kinetics of CO₂ methanation on Ni/CeO₂ catalyst