摘要
本文以焦炉气自热转化技术为背景,以自热转化炉为主要研究对象,采用实验和数值模拟相结合的方法对自热转化炉的流场结构和反应特性进行了研究,并运用Aspen Plus对自热转化系统进行了模拟计算。主要研究内容如下：
(1)运用实验和数值模拟相结合的方法系统研究了自热转化炉内的流动特性。自热转化炉内部空间可分为两部分：燃烧空间和催化剂床层。燃烧空间的流动特性通过速度分布、湍流强度和回流比进行表征。结果表明,燃烧空间上部的速度分布和湍流强度不受催化剂床层高度和空隙率的影响,但湍流强度随着喷嘴进口流率的增加而增大；燃烧空间下部接近催化剂床层表面处的轴向速度随着催化剂床层高度、空隙率和喷嘴进口流率的增加而增大；催化剂床层表面处湍流强度随着催化剂床层高度和喷嘴进口流率的增加而增大；燃烧空间回流比的大小与喷嘴进口流率无关。
催化剂床层的流动特性通过非均匀度因子和渗透深度表征：催化剂床层非均匀度因子随着空隙率的减小而降低；渗透深度随着催化剂床层高度的增加而增加。自热转化炉的喷嘴进口流率不影响催化剂床层中流体的均布特性。
(2)采用示踪法研究了自热转化炉的停留时间分布,并考察了催化剂床层高度和喷嘴进口流率对炉内停留时间分布的影响。结果表明,随着催化剂床层高度的增加,停留时间分布密度函数变窄,平均停留时间和无因次方差均减小；喷嘴进口流率增大,平均停留时间减小,无因次方差增大。基于对自热转化炉内部流动特性的认识,采用CSTR、轴向混合模型和平推流相串联的方法建立了自热转化炉停留时间分布的数学模型,并运用拉普拉斯变换和阻尼最小二乘法估算得到相关参数值。
(3)研究了敞开空间焦炉气自由射流火焰的特性。结果表明,火焰长度随焦炉气的流量和弗劳德数的增大而变长,在浮力控制区,火焰长度和弗劳德数(Frf)之间满足线性关系：L=137.07Frf-B。火焰长度随着雷诺数(Re)的增大而增大,但当Re大于8×104～9×104后,火焰长度保持不变,火焰弗劳德数Frf与Re呈线性关系。在实验条件下,当焦炉气的射流速度大于20m/s,火焰出现脱火现象,脱火高度和射流速度呈比例增长关系；当焦炉气的射流速度大于100m/s时,火焰完全熄灭。
(4)通过热模实验平台研究了自热转化炉燃烧空间进料流量变化对出口反应气体组成的影响。研究结果表明,保持氧气流量不变时,随着焦炉气流量的增大,出口气体组成中H2、CO和CH4的含量先增加后略有减小,中间存在一最大值；甲烷转化率则相应下降；CO2的含量随焦炉气的增大而减小。保持焦炉气流量不变时,出口气体组成中H2、CO和CO2的含量随着氧气流量的增加先增加后稳定不变；CH4含量随氧气流量的增大而减小,而甲烷转化率相应增大。
(5)采用数值模拟的方法对自热转化炉内的反应和流动进行了研究,考察了不同操作压力和旋流数对流场的影响,以及不同的水蒸气/焦炉气(kg/Nm3)和氧气/焦炉气(Nm3/Nm3)下,甲烷转化率和有效气产率的变化。结果表明,自热转化炉内轴向速度的衰减比常规双通道直射流快,在靠近轴线的区域出现回流区；自热转化炉内切向速度在径向上先增大后减小,速度最大值出现在燃烧空间回流区的中心位置。燃烧空间内温度分布梯度较大,而催化剂床层内温度分布均匀；相应地,燃烧空间内浓度梯度大于催化剂床层内梯度。炉内压力和旋流数的增大促使炉内组分分布均匀。对甲烷转化率和有效气产率的研究表明,水蒸气/焦炉气和氧气/焦炉气最优值分别为0.1-0.2(kg/Nm3)和0.15～0.2(Nm3/Nm3)。
(6)采用流程模拟软件Aspen Plus对自热转化炉工艺进行模拟计算,考察了操作压力、进料组成、水蒸气/焦炉气(kg/Nm3)和氧气/焦炉气州m3/Nm3)对反应结果的影响。结果表明,随着操作压力的上升,甲烷转化率和有效气产率均有所下降。焦炉气中二氧化碳含量的升高对甲烷转化率没有影响,但使有效气产率升高。水蒸气/焦炉气对甲烷转化率和有效气产率的影响不明显；甲烷转化率随氧气/焦炉气的增加而增加,但有效气产率随氧气/焦炉气的增加而下降。
This article investigated autothermal reformer based on the back ground of Coke Oven Gas autothermal reforming technology. Flow field and reaction characteristics of autothermal reformer were studied by experiment and numerical simulation. Moreover, the process simulation was investigated using Aspen Plus. The detail contents are as follow:
(1) The flow characteristics of autothermal reformer were investigated by experiments and numerical simulation. From the analysis results of flow field, space in the autothermal reformer can be divided into two parts:combustion chamber and catalyst bed. The flow in combustion chamber can be characterized by velocity distribution, turbulence intensity and reflux ratio. Results showed that the velocity distribution and turbulence intensity in chamber upper part were not influenced by catalyst bed height and porosity, but turbulent intensity increased with inlet flow rate. The axial velocity of chamber bottom part was increased with catalyst bed height, porosity and inlet flow rate. The turbulence intensity of chamber bottom part was increased with catalyst bed height and inlet flow rate. The reflux ratio in chamber was not influenced by inlet flow rate.
The flow in catalyst bed can be characterized by maldistribution factor and penetration depth. The maldistribution factor was decreased with catalyst bed porosity, while penetration depth was increased with catalyst bed height. The uniform distribution characteristic of autothermal reformer was not influenced by inlet flow rate.
(2) Resident time distribution of autothermal reformer was studied by impulse response. The influences of catalyst bed height and inlet flow rate on RTD were analyzed. The results showed that the mean residence time, variance residence time decreased as well as distribution functions of RTD narrowing with the catalyst bed height increasing. The mean residence time decreasing and dimensionless variance residence time increasing with inlet flow rate increasing. The RTD model was formed by combination with CSTR, axial dispersion model and PFR based on the flow characteristic of autothermal reformer. Parameters in model were obtained by Laplace transforming and Levenberg-Marquardt.
(3) The characteristic of co-axial jet free diffusion flame of Coke-Oven Gas (COG) was investigated by experiments. The results showed that the flame length was increased with COG flow rate and Froude number (Frf). In the zone of momentum control, the relationship of flame length and Frf is linear:L=137.07Frf-B. The flame length was increased with Re. when the Re is larger than 8×104～9×104, the flame length was constant. The relationship of Frf and Re was linear. When the jet velocity of COG is 20 m/s, flame will be blown off. The height of blow off had a proportional increasing to jet velocity. Flame will be extinct when the velocity of COG larger than 100m/s.
(4) The influences of feed on syngas composition were studied. Results showed that when flow rate of oxygen was constant, the fractions of H2, CO, CH4 in syngas were increased at first and then decreased with COG flow rate increasing. While methane conversion and CO2 fraction are decreased with COG flow rate increasing. When COG flow rate is constant, CH4 concentrations of outlet was decreased with oxygen flow rate increasing, while CO, CO2 and H2 concentrations of outlet were increasing at first and then constant with oxygen flow rate.
(5) The reactions and flow in autothermal reformer were investigated with the numerical simulation. The structure and characteristic of flow field of hot model were analyzed. The influences of operation pressure and swirl number of nozzle on flow field, and the influences of steam/fuel and oxygen/fuel on methane conversion and H2+CO yield were studied. Results showed that the attenuation of swirl velocity is slow than axial velocity. There was back flow zone near the axis area. Along the radial position, the swirl velocity increase at first and then decreased. The peak value of swirl velocity is at central position of back flow zone in chamber. Temperature and concentration gradient of chamber is larger than that of catalyst bed. Operating pressure and large swirl number is good for the species mixing. From the analysis of conversion and effective gas (H2+CO) yield, it can obtain the optimal value of Steam/COG and Oxygen/COG is 0.1～0.2 (kg/Nm3) and 0.15～0.2 (Nm3/Nm3), respectively.
(6) Autothermal process simulation was studied with Aspen Plus. The influences of operating pressure, feed composition, Steam/COG and Oxygen/COG on syngas composition were investigated. Results showed that methane conversion and effective gas yield are decreased with the operating pressure. There is no any effect of CO2 fraction in feed on methane conversion, but effective gas yield is increased with CO2 fraction in feed. The Steam/ COG could not affect methane conversion and effective gas. Methane conversion is increased with Oxygen/COG, while effective gas yield is decreased with increasing of Oxygen/COG.
引文
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