Reaction rate simulation and mechanism analysis of methane steam reforming

HUANG Xing; LIANG Jiabao; MA Qiang; YAO Xin; LIU Yang; YAN Hongyan

doi:10.12434/j.issn.2097-2547.20240156

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Reaction rate simulation and mechanism analysis of methane steam reforming

- Reaction rate simulation and mechanism analysis of methane steam reforming
- Vol. 49, Issue 9, Pages: 12-18(2024)
- 作者机构：
  
  华北理工大学冶金与能源学院，河北唐山 063210
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20240156
  CLC： TE64
- Published：25 September 2024，
  
  Received：14 April 2024，
  
  Revised：30 April 2024，
- 稿件说明：
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黄兴,梁家宝,马强等.甲烷水蒸气重整反应速率模拟与机理分析[J].低碳化学与化工,2024,49(09):12-18.

HUANG Xing,LIANG Jiabao,MA Qiang,et al.Reaction rate simulation and mechanism analysis of methane steam reforming[J].Low-carbon Chemistry and Chemical Engineering,2024,49(09):12-18.
黄兴,梁家宝,马强等.甲烷水蒸气重整反应速率模拟与机理分析[J].低碳化学与化工,2024,49(09):12-18. DOI： 10.12434/j.issn.2097-2547.20240156.

HUANG Xing,LIANG Jiabao,MA Qiang,et al.Reaction rate simulation and mechanism analysis of methane steam reforming[J].Low-carbon Chemistry and Chemical Engineering,2024,49(09):12-18. DOI： 10.12434/j.issn.2097-2547.20240156.

摘要

氢能作为清洁能源，具有巨大的发展潜力。甲烷水蒸气重整技术是一种经济且环保的制氢方式，可产出高纯度氢并减少碳排放。但在该反应的链转移过程中，由于反应速率变化较快，目前反应机理尚不明确。采用CHEMKIN模拟软件，将甲烷水蒸气重整反应动力学模型与平推流反应器（PFR）进行耦合，在温度为1200 K、水碳比（物质的量比）为3.0和气体入口质量流量为0.01 g/s的反应条件下进行模拟。通过分析CH

、H

O及中间产物CH

基元反应速率，确定了影响反应的主要物质，进而对反应机理（主要指反应路径）进行了深入分析。结果表明，水蒸气和CH

在催化剂表面发生的吸附和解吸附反应以及H

O(s)（s代表吸附态）和CH

(s)在催化剂表面发生的解离反应对甲烷水蒸气重整反应的影响较大；CH

(s)在催化剂表面的两种解离反应分别为直接解离和与O(s)发生反应解离，且与O(s)发生反应的解离速率要高于直接解离速率。CH

(s)在催化剂表面的反应路径为CH

(g) → CH

(s) → CH

(s) → CH(s) → C(s)，其中CH

(g) → CH

(s) → CH

(s)对反应的影响最大。H

O(g)同样吸附在催化剂表面，其反应路径为H

O(g) → H

O(s) → OH(s) → H(s)。

Abstract

As clean energy

hydrogen energy has great potential for development. Methane steam reforming is an economical and environmentally friendly hydrogen production method

which can produce high-purity hydrogen and reduce carbon emissions. However

due to the rapid change of the reaction rate during the chain transfer process of the reaction

the reaction mechanism is still unclear. CHEMKIN simulation software was used to couple the methane steam reforming reaction kinetic model with the Plug Flow Reactor (PFR). The simulation was carried out under the reaction conditions of the temperature of 1200 K

water-carbon ratio (molar ratio) of 3.0

and gas inlet mass flow rate of 0.01 g/s. By analyzing the elementary reaction rates of CH

O and intermediate product CH

the main substances involved in the reaction were determined

and the reaction mechanism (mainly refers to the reaction pathways) was further analyzed. The results show that the adsorption and desorption reaction of water vapor and methane on the catalyst surface

and the dissociation reaction of H

O(s) (s represents adsorbed state) and CH

(s) on the catalyst has a great influence on methane steam reforming reaction. The two dissociation reactions of CH

(s) on the catalyst surface are direct dissociation and reactive dissociation with O(s)

and the reaction rate with O(s) is higher than the direct dissociation rate. The reaction pathway of CH

(s) on the catalyst surface is CH

(g) → CH

(s) → CH

(s) → CH(s) → C(s)

and CH

(g) → CH

(s) → CH

(s) has the greatest influence on the reaction. H

O(g) is also adsorbed on the surface of catalysts

and the reaction pathway is H

O(g) → H

O(s) → OH(s) → H(s).

关键词

甲烷水蒸气重整反应速率反应机理

Keywords

methane steam reformingreaction ratereaction mechanism

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