Transfer dynamics and reaction control mechanism over methanation catalyst particles in transport bed

CHENG Yonggang; LIU Jiao; HAN Zhennan; SHI Lei; XU Guangwen

doi:10.11949/0438-1157.20190052

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Transfer dynamics and reaction control mechanism over methanation catalyst particles in transport bed

更新时间：2026-07-24

- Transfer dynamics and reaction control mechanism over methanation catalyst particles in transport bed
- CIESC Journal Vol. 70, Issue 8, Pages: 2876-2887(2019)
- 作者机构：
  
  1.中国科学院过程工程研究所，北京 100190
  2.沈阳化工大学, 辽宁沈阳 110142
  3.中国科学院大学, 北京 100049
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20190052
  CLC： TQ 032
- Received：16 January 2019，
  
  Revised：2019-04-02，
  
  Online First：24 July 2026，
  
  Published：05 August 2019
- 稿件说明：
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程永刚, 刘姣, 韩振南, 石磊, 许光文. 输送床甲烷化催化剂颗粒的热质传递行为与反应机制[J]. 化工学报, 2019, 70(8): 2876-2887

CHENG Yonggang, LIU Jiao, HAN Zhennan, SHI Lei, XU Guangwen. Transfer dynamics and reaction control mechanism over methanation catalyst particles in transport bed[J]. CIESC Journal, 2019, 70(8): 2876-2887
程永刚, 刘姣, 韩振南, 石磊, 许光文. 输送床甲烷化催化剂颗粒的热质传递行为与反应机制[J]. 化工学报, 2019, 70(8): 2876-2887 DOI： 10.11949/0438-1157.20190052.

CHENG Yonggang, LIU Jiao, HAN Zhennan, SHI Lei, XU Guangwen. Transfer dynamics and reaction control mechanism over methanation catalyst particles in transport bed[J]. CIESC Journal, 2019, 70(8): 2876-2887 DOI： 10.11949/0438-1157.20190052.

摘要

采用数值模拟对输送床甲烷化的粒径100 μm级单颗粒催化剂的反应与热传递行为进行了研究，揭示了反应热在单颗粒催化剂上的动态传递规律和典型条件下的反应控制机制。在输送床反应器中，热传递效率高，进入反应器的单个催化剂颗粒温度一般在0.1 s左右即可达到稳态。稳态的100 μm级催化剂颗粒表面、中心、流体之间的温差很小，但催化剂颗粒的径向温度表现为由表面向中心逐渐升高的分布，证明了甲烷化反应热升高了催化剂颗粒温度，建立了温度升高的催化剂颗粒与反应气氛之间的热传递平衡。模拟甲烷化反应速率与组分气体在催化剂颗粒内的分布，揭示了在加压和较高气速反应条件下，反应物向催化剂颗粒的扩散加快，催化剂颗粒的局部甲烷化反应受动力学控制，反应速率由中心向表面逐步减低。反之，常压与低气速条件使得催化剂颗粒的甲烷化反应受气体扩散控制，反应速率自表面向中心逐渐降低。

Abstract

Numerical simulation based on COMSOL Multiphysics was conducted to understand the heat transfer dynamics and reaction control mechanism over methanation catalyst particles in size of about 100 μm under conditions of transport bed. The high heat transfer efficiency in transport bed makes the catalyst particle into the bed quickly approach its steady state at about 0.1 s

a really very short transient period. For the catalyst particle at steady state there are temperatures sharing little difference among particle center

particle surface and gas flow bulk. However

it was clear that the temperature is still gradually lower from the center to surface of the particle

and on particle surface its temperature is higher than that in gas bulk. This clarifies that the exothermic heat of methanation reaction first heats catalyst particle

and the temperature-raised particle then reaches a balance of heat transfer with its surrounding gas. Calculating the radial profiles of temperature

gas components and reaction rate inside the catalyst particle clarified that for methanation at higher gas bulk temperature and elevated pressure (2 MPa here) the mass transfer into particles is quicker and the CO consumption rate becomes gradually lower from the center to surface of the particle. On the contrary

for atmospheric methanation at lower gas velocity

the reaction rate was conversely lower at the particle center. It demonstrates that the methanation reaction is subject to kinetic control for the former but to mass transfer for the latter.

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Keywords

references

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