燃料化学学报2011，Vol.39Issue(8)：633-640,8.
甲烷自热重整制氢的热力学和动力学分析
Thermodynamic and kinetic analyses for hydrogen production via methane autothermal reforming
摘要
Abstract
A systemic thermodynamic analysis was conducted for the autothermal reforming of natural gas to produce hydrogen. A kinetic modeling was made for the autothermal reforming by employing the pre-mixed laminar model included in CHEMKIN package that incorporates the mechanisms of CH4 oxidation, steam reforming and dry reforming; kinetic parameters for methane reforming over Ni-based catalyst, widely used in the natural gas reforming industry, were adopted. The results show that the equilibrium composition of outflow gases is depended on the reaction temperature, the air-fuel ratio and water-fuel ratio. The pressure has a limited impact on the product distribution but has a remarkable impact on the time needed to reach the equilibrium. Under 715 ℃ ~ 730 ℃, 0. 7 Mpa ~ 1. 0 Mpa, O2/CH4 of 0. 60 ~ 0. 70, and H2O/CH4 of 3. 15 ~ 3. 25, the fraction of H2 in the product is higher than 68% , while CO does not exceed 10% (dry basis) and the carbon deposition is close to 0. The kinetic analysis suggests two distinct stages during the autothermal reforming process. The initial stage is a rapid oxidation zone, where H2O and CO2 are the main products. The second stage is a slow conversion zone, where methane steam reforming reaction as well as water gas shift reaction and slight dry reforming take place, with H2, CO and CO2 being the main products. Adding H2O in the feed gas is a visible measure for avoiding hot spot in the reactor and controlling the formation of CO.关键词
自热重整/甲烷/热力学/层流预混合/动力学Key words
autothermal reforming/methane/thermodynamic/premixed laminar/kinetic分类
化学化工引用本文复制引用
陈玉民,赵永椿,张军营,郑楚光..甲烷自热重整制氢的热力学和动力学分析[J].燃料化学学报,2011,39(8):633-640,8.基金项目
国家自然科学基金(40972102,50906031) （40972102,50906031）
国家重点基础研究发展规划(973计划,2010CB227003). （973计划,2010CB227003）
