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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
Suppression strategies of carbon deposit and optimization of reaction conditions for dry reforming of methane based on thermodynamic analysis
- 低碳化学与化工 2026, 51(3): 21-31.
- 作者机构：
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
3.中国科学院大学，北京 100049
4.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
- 作者简介：
孙浩然（2001—），硕士研究生，研究方向为多相催化，E-mail：sunhaoran123@gs.zzu.edu.cn。
张萌（1991—），博士，副教授，研究方向为工业催化，E-mail：zhangmeng1991@zzu.edu.cn；
韩怡卓（1964—），博士，研究员，研究方向为煤化工，E-mail：hanyz@sxicc.ac.cn。
- 基金信息：国家自然科学基金(22408348);河南省自然科学基金(242300421599)
DOI：10.12434/j.issn.2097-2547.20250176
中图分类号： TQ426收稿：2025-04-11，
修回：2025-05-12，
纸质出版：2026-03-25
- 稿件说明：
移动端阅览
孙浩然,杨涛,李超等.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.
SUN Haoran,YANG Tao,LI Chao,et al.Suppression strategies of carbon deposit and optimization of reaction conditions for dry reforming of methane based on thermodynamic analysis[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(3):21-31.
孙浩然,杨涛,李超等.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. DOI： 10.12434/j.issn.2097-2547.20250176.
SUN Haoran,YANG Tao,LI Chao,et al.Suppression strategies of carbon deposit and optimization of reaction conditions for dry reforming of methane based on thermodynamic analysis[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(3):21-31. DOI： 10.12434/j.issn.2097-2547.20250176.
摘要
甲烷干重整（DRM）反应可以将温室气体CH
4
和CO
2
转化为高附加值的合成气，兼具环境改善与能源升级的双重效益。然而，该反应通常需要在700 ℃以上进行，能耗较高且会导致催化剂因颗粒烧结和表面积炭而失活。基于热力学分析评估了DRM反应体系的平衡组成，探讨了反应温度、惰性气体含量、反应压力和原料气进料比（
n
(CH
4
):
n
(CO
2
)）等对催化剂催化性能和积炭行为的影响，并对文献报道的实际反应结果与理论平衡值的偏离现象进行了深入分析。结果表明，减小
n
(CH
4
):
n
(CO
2
)至1:2可使原料气的完全转化温度降低200 ℃，并有效抑制反应温度700 ℃以上时的积炭生成；若
n
(CH
4
):
n
(CO
2
):
n
(惰性气体)调整至1:1:2也可显著抑制反应温度500~800 ℃时的积炭生成，但是适宜工业应用的高压操作不利于原料转化且会促进积炭生成。低温区（
<
600 ℃）和高温区（
>
800 ℃）的实际反应结果采用无积炭生成模型评估更为合理，而600~800 ℃区间的实际反应结果需结合积炭生成平衡模型进行评估。本研究基于热力学分析明确了DRM反应的操作边界与积炭调控策略，以期为催化剂设计与催化性能评估和优化提供重要理论依据。
Abstract
Dry reforming of methane (DRM) can convert greenhouse gases CH
4
and CO
2
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 carbo
n 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
(CH
4
):
n
(CO
2
)) 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
(CH
4
):
n
(CO
2
) to 1:2 can lower the complete conversion temperature by 200 ℃ and effectively suppress carbon deposit formation at above 700 °C. In addition
changing the inert gas dilution ratio
n
(CH
4
):
n
(CO
2
):
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
Keywords
references
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