Metathesis of ethylene and butylene-2 to propylene with Mo on Hβ-Al2O3 catalysts

Metathesis of ethylene and butylene-2 to propylene with Mo on Hβ-Al2O3 catalysts
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DOI:
10.1016/j.cattod.2004.06.062
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发表时间:
2004-09
期刊:
影响因子:
5.3
通讯作者:
Shenglin Liu;Shengjun Huang;Wenjie Xin;Bai Jie;Sujuan Xie;Longya Xu
Shenglin Liu;Shengjun Huang;Wenjie Xin;Bai Jie;Sujuan Xie;Longya Xu
中科院分区:
化学2区
文献类型:
--
作者:
Shenglin Liu;Shengjun Huang;Wenjie Xin;Bai Jie;Sujuan Xie;Longya Xu

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采用TPR和NH3-TPD技术,在流动反应器中考察了不同负载型钼催化剂在乙烯和丁烯-2歧化反应中的反应性能、酸碱性质和还原性能。Mo/(Hβ-Al 2 O3)催化剂的稳定性除受温度、空速和压力的影响外,还受Mo负载量、焙烧温度和水热处理条件的影响。NH3-TPD结果表明,在Hβ-Al_2O_3上负载适量的钼有利于催化剂的稳定性。Mo/(Hβ-Al 2 O 3)催化剂的最佳制备条件为:Mo含量3 wt.%,分别在550°C下水热处理2 h和700°C下煅烧2 h。结果表明,在N2/C2 H4 =1.5,C2 H4/C4 H8 -2=3/1,WHSV(C2 H4 + C4 H8 -2)=1h-1,T=120°C,P=1.0MPa的条件下,3 Mo/(Hβ-Al 2 O3)催化剂(编号为3 Mo/Hβ5502700)在22 h的反应时间内,C4 H8 -2的转化率保持在8 - 2%左右。此外,合适的压力(0.5-1.0MPa)和低温(35°C)有利于保持3 Mo/Hβ5502700催化剂的稳定性。
Reaction performance, acidic and basic properties, as well as reduction properties of various supported molybdenum catalysts for the metathesis of ethylene and butylene-2 to propylene were investigated by TPR and NH3-TPD techniques in a flow-reactor. Besides temperature, space velocity and pressure, the stability of a Mo/(Hβ-Al2O3) catalyst is strongly affected by the Mo loading, the calcination temperature and the hydrothermal treatment conditions. A suitable molybdenum loading on Hβ-Al2O3is favorable to the stability of the catalyst that possesses suitable amount of acidity, which was determined by NH3-TPD measurements. The optimum preparation conditions of the Mo/(Hβ-Al2O3) catalyst are as follows: molybdenum content 3wt.%, hydrothermal treatment and calcination at 550°C for 2h and 700°C for 2h, respectively. Thus, the optimal catalyst of 3Mo/(Hβ-Al2O3), designated as 3Mo/Hβ5502700, could keep a conversion of C4H8-2 at about 82% during 22h of reaction time-on-stream under the following conditions: N2/C2H4=1.5, C2H4/C4H8-2=3/1, WHSV(C2H4+C4H8-2)=1h−1, T=120°C, and P=1.0MPa. In addition, a suitable pressure, such as 0.5–1.0MPa, and a low temperature, such as 35°C, are beneficial for keeping the stability of the 3Mo/Hβ5502700 catalyst.