化工进展

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La-Ni-Mo-B非晶态催化剂高温催化苯酚加氢脱氧及失活性能

胡 韬,杨运泉,王威燕,刘文英,贺 恒,陈来福   

  1. 湘潭大学化工学院,湖南 湘潭 411105
  • 出版日期:2010-12-05 发布日期:2010-12-05

La-Ni-Mo-B amorphous catalyst deactivation in phenol hydrodeoxygention at high temperature

HU Tao,YANG Yunquan,WANG Weiyan,LIU Wenying,HE Heng,CHEN Laifu   

  1. School of Chemical Engineering,Xiangtan University,Xiangtan 411105,Hunan,China
  • Online:2010-12-05 Published:2010-12-05

摘要:

(NH4)6Mo24Ni(NO3)2La(NO3)3为原料,NaBH4为还原剂,采用化学还原法制备出非晶态催化剂La-Ni-Mo-B,以苯酚为模型化合物研究其加氢脱氧性能。结果表明,非晶态催化剂具有较高的加氢脱氧活性,而在548 K时苯酚转化率降低至58.5%。主要原因是该非晶态催化剂在548 K下,颗粒发生明显团聚,比表面积显著下降,非晶态Ni活性中心发生晶化,电子转移减少,抑制了催化剂的加氢活性,使反应路径偏向直接脱氧的方式进行,从而导致经过高温热处理的La-Ni-Mo-BC)在523 K时,苯酚转化率下降至37.5%,芳香烃苯的含量增加至22.3%

Abstract:

La-Ni-Mo-B amorphous catalyst was prepared by chemical reduction of ammonium heptamolydatenickel nitrate and lanthanum nitrate with sodium borohydride aqueous solution. The hydrodeoxygenationHDOperformance was tested using phenol as a model compound. Results showed that the amorphous catalyst exhibited high HDO activitybut the phenol conversion was decreased to 58.5% when the reaction temperature was increased to 548 K. The deactivation was mainly attributed to the serious agglomeration of catalyst particlesthe significant reduction in specific surface areathe transformation of Ni active site from amorphous structure to crystalline structure and the decrease in electron transfer under the condition of temperature 548 K. The hydrogenation activity of the catalyst was inhibited and then the reaction route proceeded with the direct deoxygenation routewhich lead to the phenol conversion decreased to 37.5% and aromatic benzene content increased to 22.3% at the temperature 523 K over La-Ni-Mo-BC.

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