二氧化碳-甲烷干气重整反应及其积炭控制的热力学分析

Thermodynamic analysis of carbon dioxide-methane dry reforming and its carbon deposition control

二氧化碳-甲烷干气重整(DRM)反应制合成气(H_(2)+CO)是二氧化碳(CO_(2))资源化利用的重要研究方向,关键问题在于积炭的控制。利用FactSage软件,基于吉布斯自由能最小法,对DRM反应及其积炭控制进行了热力学计算分析。结果显示,高温(600~1200℃)、进料比(n(CH_(4))/n(CO_(2)))为1.00、常压等单因素条件下,有利于DRM反应进行,可以实现较好的反应转化速率;以炭的残余量为0.01%(物质的量分数)作为积炭区与非积炭区的临界点,设定反应压力为0.10 MPa、反应温度为900℃,当进料比小于等于0.95时,反应处于非积炭区。研究结果对优化DRM反应的操作条件及催化剂设计具有一定的指导意义。

The carbon dioxide-methane dry reforming(DRM)reaction for the synthesis of syngas(H_(2)+CO)is an important research direction for the resourceful utilization of carbon dioxide(CO_(2)),with a key focus on carbon deposition control.Using FactSage software and employing the Gibbs free energy minimization method,a thermodynamic computational analysis of the DRM reaction and its carbon deposition control was conducted.The results indicate that under single-factor conditions such as high temperature(600°C to 1200°C),a feed ratio(n(CH_(4))/n(CO_(2)))of 1.00,and atmospheric pressure,favorable conditions for the DRM reaction can be achieved,leading to improved reaction conversion rates.By setting a carbon residue threshold at 0.01%(mole fraction),the critical conditions distinguishing between the carbon deposition and non-deposition zones are determined:a reaction pressure of 0.10 MPa,a reaction temperature of 900°C,and the reaction falling within the non-carbon deposition zone when the feed molar ratio is less than or equal to 0.95.The research outcomes hold significant guidance for optimizing the operational parameters of DRM reactions and catalyst design.