摘要
为了强化传质和反应操作,同时实现反应产物与浆液的分离,使用CuCr/CH3ONa催化体系,在鼓泡浆液反应器(BC-SR)、闪蒸塔(FC)和浆液循环泵组成的反应系统(BCSR-FC)中考察了低温甲醇合成的反应性能。初始浆液由铜铬催化剂、甲醇钠溶液、乳化剂OP-10和液相介质二甲苯组成。在BCSR:4.2 MPa^4.6 MPa,110℃~120℃(反应段)100℃~110℃(扩大段),入口气速0.35 cm/s^0.40 cm/s;FC:0.25 MPa^0.40 MPa,80℃~90℃,浆液循环量50 L/h下,100 h实验期间,合成气转化率、CO转化率和H2转化率分别从最高的71.0%、79.1%和67.5%降到17.8%、35.0%和12.1%。催化体系失活的主要原因是CH3ONa和MeF反应生成甲酸钠。液体产物由DME 1.23%、甲醇79.52%、MeF 19.25%组成。甲醇+MeF的选择性大于98%。以系统中催化剂为基准,液体产物的产率则为0.166 g/gcat.h;BCSR中CuCr催化剂的液体产物的产率为0.336 g/gca.th。
In order to promote mass transfer and realize products separation from slurry, reaction performance of CuCr/CH3ONa catalyst used for the low-temperature methanol synthesis was firstly examined in the bubble column slurry reactor with a flash column （BCSR/FC）. The reaction system includes the reaction section of 39 mm id. and 480 0 mm height and the enlarged section of 147 mm id and 120 0 mm height in BCSR, FC of 147 mm id. and 164 0 mm height and a slurry recirculating pump. The initial slurry was composed of the required amounts of sodium methoxide solution and CuCr catalyst and emulsifier OP-10 as well as the balanced liquid xylene medium. The results showed that the BCSR/FC can be operated at 4.2 MPa - 4.6 MPa, 110 ℃ - 120 ℃ （ reaction section） and 100 ℃ - 110 ℃ （ enlarged section）, inlet gas velocity 0.35 cm/s - 0.40 cm/s for BCSR, 0.25 MPa - 0.4 MPa, 80 ℃ - 90 ℃ for FC and slurry recirculation rate of 50 L/h. The results showed that the conversions of CO ＋ H2, CO and H2 were decreased from their highest of 71.0% ,79.1% and 67.5% to 17.8%, 35% and 12.1% during operation test over 100 h respectively. The stability of the catalyst system is poor although its initial activity is quite high. This is probably due to the consumption of CH3ONa caused by the side reaction CH3ONa ＋ HCOOCH3→ CH3OCH3 ＋ HCOONa. Liquid products were composed of DME of 1.23%, methanol of 79.52% and MeF of 19.25%. Selectivity of Methanol ＋ MeF is more than 98%. Its yields were 0. 168g/gcat·h based on all CuCr catalyst in the system and 0.336 g/gcat·h only based on the CuCr catalyst in BCSR.
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2007年第1期56-60,共5页
Journal of Fuel Chemistry and Technology
基金
中国科学院九.五特别支持项目
关键词
甲醇合成
鼓泡浆液反应器
甲酸甲酯
闪蒸分离
methanol synthesis
bubble column slurry reactor
methyl formate
flash-separation
