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基于热力学分析的甲烷干重整反应积炭抑制策略及反应条件优化

孙浩然 杨涛 李超 张萌 刘仲毅 韩怡卓

低碳化学与化工2026,Vol.51Issue(3):21-31,11.
低碳化学与化工2026,Vol.51Issue(3):21-31,11.DOI:10.12434/j.issn.2097-2547.20250176

基于热力学分析的甲烷干重整反应积炭抑制策略及反应条件优化

Suppression strategies of carbon deposit and optimization of reaction conditions for dry reforming of methane based on thermodynamic analysis

孙浩然 1杨涛 1李超 2张萌 1刘仲毅 3韩怡卓4

作者信息

  • 1. 郑州大学 化学学院,河南 郑州 450001
  • 2. 中国科学院 山西煤炭化学研究所 煤炭高效低碳利用全国重点实验室,山西 太原 030001||中国科学院大学,北京 100049
  • 3. 郑州大学 化学学院,河南 郑州 450001||郑州大学 炼焦煤资源绿色开发全国重点实验室,河南 郑州 450001
  • 4. 中国科学院 山西煤炭化学研究所 煤炭高效低碳利用全国重点实验室,山西 太原 030001
  • 折叠

摘要

Abstract

Dry reforming of methane(DRM)can convert greenhouse gases CH4 and CO2 into high-value syngas,with dual benefits of environmental mitigation and energy upgrading.However,this reaction usually needs to be carried out above 700℃,leading to high energy consumption and catalyst deactivation due to metal sintering and carbon deposit.The equilibrium compositions in the DRM system were systematically evaluated based on thermodynamic analysis,and the effects of reaction temperatures,inert gas contents,reaction pressures and feed ratios of raw gas(n(CH4):n(CO2))on the catalytic performances and carbon deposit behaviors of catalysts were discussed.The deviations between actual reaction results reported in the literature and the theoretical equilibrium predictions were also thoroughly analyzed.The results show that reducing n(CH4):n(CO2)to 1:2 can lower the complete conversion temperature by 200℃and effectively suppress carbon deposit formation at above 700 ℃.In addition,changing the inert gas dilution ratio n(CH4):n(CO2):n(inert gas)to 1:1:2 can remarkably suppress carbon deposit from 500℃to 800℃.However,high-pressure operations suitable for the industrial applications are not conducive to raw material conversion and can promote carbon deposit.It is more reasonable to evaluate the actual reaction results in the low-temperature zone(<600℃)and high-temperature zone(>800℃)using the no carbon deposit formation model,while the actual reaction results from 600℃to 800℃need to be evaluated in conjunction with the carbon deposit equilibrium model.This research clearly defines the operational boundaries and suppression strategies of carbon deposit for DRM based on thermodynamic analysis,in order to provide an essential theoretical basis for catalyst design and catalytic performance evaluation and optimization.

关键词

甲烷干重整/热力学计算/平衡组成/反应条件/积炭

Key words

dry reforming of methane/thermodynamic calculation/equilibrium compositions/reaction conditions/carbon deposit

分类

化学化工

引用本文复制引用

孙浩然,杨涛,李超,张萌,刘仲毅,韩怡卓..基于热力学分析的甲烷干重整反应积炭抑制策略及反应条件优化[J].低碳化学与化工,2026,51(3):21-31,11.

基金项目

国家自然科学基金(22408348) (22408348)

河南省自然科学基金(242300421599). (242300421599)

低碳化学与化工

1001-9219

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