论文部分内容阅读
采用浸渍法制备一系列以稀土氧化物为载体的NiWP催化剂。在固定床反应装置上考查其在973 K~1123 K温度范围内CO_2重整CH_4的催化活性,发现NiWP/Y_2O_3催化剂催化活性最好,其在1073 K时,CH_4和CO_2的转化率达到了98%和90%。同时考察了以Y_2O_3为载体的Ni,Ni W,Ni P,WP,NiWP的催化剂在固定床反应装置上在1023 K~1123 K温度范围内CO_2重整CH_4的催化活性及其稳定性。并通过XRD,H2-TPR等手段对催化剂进行了表征。结果表明,不同催化活性组分对催化剂NiWP/Y_2O_3有明显的影响,在1073 K时,NiWP/Y_2O_3的催化活性最好,CH_4和CO_2的转化率为98%和90%,其次为Ni/Y_2O_3,其CH_4和CO_2的转化率为88.5%和77%。同时在1073 K下,NiWP/Y_2O_3催化剂的稳定性亦优于其他几种催化剂的稳定性,其在10小时后的CH_4的转化率为95.1%与10小时前CH_4的转化率相差不大。并对积碳后催化剂进行TG-DTG表征,结果表明,不同活性组分催化剂积碳后的积碳量不同,其积碳种类也不尽相同,其中NiWP/Y_2O_3催化剂的积碳率最少为9.74%,其积碳以丝状碳和石墨碳为主;Ni/Y_2O_3和Ni W/Y_2O_3的积碳率相差不大,为14.38%和14.63%,而Ni P/Y_2O_3的积碳率为35.6%,这三者的积碳以丝状碳为主。
A series of NiWP catalysts with rare earth oxides as carrier were prepared by impregnation method. The activity of CO_2 reforming CH_4 in the temperature range of 973 K ~ 1123 K was investigated on a fixed bed reactor. It was found that the catalytic activity of NiWP / Y_2O_3 catalyst was the best. At 1073 K, the conversion of CH_4 and CO_2 reached 98 % And 90%. At the same time, the catalytic activity and stability of CO_2 reforming CH_4 over a fixed bed reactor at temperatures ranging from 1023 K to 1123 K were investigated with catalysts Ni_, Ni W, Ni P, WP and NiW with Y_2O_3 as carriers. The catalysts were characterized by XRD, H2-TPR and other means. The results showed that the catalytic activities of NiWP / Y_2O_3 were obviously influenced by different catalytic active components. The catalytic activity of NiWP / Y_2O_3 was the best at 1073 K with the conversion rates of 98% and 90% for CH_4 and CO_2, followed by Ni / Y_2O_3 , The CH_4 and CO_2 conversion rate of 88.5% and 77%. At the same time, the stability of NiWP / Y_2O_3 catalyst is better than that of other catalysts at 1073 K. The conversion rate of CH_4 after 10 hours is 95.1%, which is similar to that of CH_4 before 10 hours. The results of TG-DTG showed that the carbon deposits of different active components were different after carbon deposition, and their carbon deposition types were also different. The carbon deposition rate of NiWP / Y_2O_3 catalyst was at least 9.74 %, And the carbon deposits are dominated by filiform carbon and graphite carbon. The carbon deposition rates of Ni / Y_2O_3 and Ni W / Y_2O_3 are 14.38% and 14.63%, respectively, while the carbon deposition rate of Ni P / Y_2O_3 is 35.6% , The three are mainly carbon-based carbon deposition.