基于Gibbs自由能最小原理分析CO_2重整CH_4  

Analysis on carbon dioxide reforming of methane with free energy minimization approach

作　　者：李延兵[1] 肖睿[1] 金保升[1] 邓中乙[1] 

机构地区：[1]东南大学洁净煤发电及燃烧技术教育部重点实验室,南京210096

出　　处：《东南大学学报（自然科学版）》2006年第5期769-773,共5页Journal of Southeast University：Natural Science Edition

基　　金：国家重点基础研究发展计划(973计划)资助项目(2005CB221202-03)

摘　　要：运用G ibbs自由能最小方法,研究了重整反应器的操作参数(温度、压力、反应气配比等)对CO2重整反应中CH4转化率和产物分布的影响,以及甲烷氧化反应与CO2重整反应间的能量耦合.研究结果表明:反应压力P不变(P=101.325 kPa),随温度升高CH4和CO2转化率增大,在900 K左右产生的H2O(g)的量达到极大值,在1 200 K以上CH4转化率接近100%;反应温度T不变(T=973 K),随压力升高CH4和CO2转化率降低,H2O(g)的选择性略微增加;T=973 K,P=101.325 kPa,原料气中nCH4/nCO2(摩尔比)从0.65增加到2.0时,CH4转化率从85%降到45%,nH2/nCO(摩尔比)从0.77增加到0.95;反应器中加入适量O2,可以提供CO2重整反应所需的能量,同时可调节产物中CO与H2的摩尔比.The minimum of Gibbs free energy is applied to study the influence of operating parameters （temperature, pressure and composition of feed gas, et al） on the methane conversion, products distribution, and energy coupling between methane oxidation and carbon dioxide reforming methane. The results show： the CH4 and CO2 conversions increase with temperature at 0. 1 MPa. At about 900 K, the amount of steam reaches the maximum. Above 1 200 K, the CH4 conversion is near 100%. The CH4 and CO2 conversions decrease and the steam selection rises slightly with pressure at 973 K. Under conditions of 973 K and 0. 1 MPa, the CH4 conversion decreases from 85% to 45% but nH2/nCO ratio increase from 0. 77 to 0. 95 with the increase of nCH4/nCO2 ratios in the range of 0.65 - 2. 0. By introducing oxygen, energy balance in the carbon dioxide reforming methane reactor oxidation can be realized, and the molar ratio of CO to H2can be adjusted as well.

关 键 词：煤基多联产 CO2重整CH4 自由能最小 热力学平衡 

分 类 号：TQ013.1[化学工程]