CIESC Journal ›› 2021, Vol. 72 ›› Issue (5): 2626-2637.DOI: 10.11949/0438-1157.20210192

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

Study on hydrodeoxygenation performance of hierarchical Pt-Ni/ZSM-5 for lignin derivatives

LI Xiaoxue1,2(),NIU Xiaopo1,2,WANG Qingfa1,2()   

  1. 1.Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
    2.Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin 300072, China
  • Received:2021-01-31 Revised:2021-03-22 Online:2021-05-05 Published:2021-05-05
  • Contact: WANG Qingfa

级孔Pt-Ni/ZSM-5对木质素衍生物加氢脱氧性能研究

李晓雪1,2(),牛晓坡1,2,王庆法1,2()   

  1. 1.天津大学化工学院绿色合成与转化教育部重点实验室,天津 300072
    2.天津化学化工协同创新中心,天津 300072
  • 通讯作者: 王庆法
  • 作者简介:李晓雪(1997—),女,硕士研究生,lixiaoxue@tju.edu.cn
  • 基金资助:
    国家自然科学基金项目(21476169)

Abstract:

The Pt-Ni bimetallic catalyst supported on the graded pore ZSM-5 zeolite was prepared by the equal volume co-impregnation method, and the effect of different Pt/Ni ratios on hydrodeoxygenation performance of guaiacol and dibenzofuran was systematically studied. The physicochemical properties of the as-synthesized Pt-Ni catalysts were characterized via XRD, N2-BET, SEM, TEM and H2-TPR. The results showed that when the loading amount of Ni was small (1% and 3%,mass ratio), it was beneficial to promote the dispersion of active metals and enhance synergistic effect between Pt-Ni bimetals. However, the active metals would agglomerate with the increase of Ni loading to 5%(mass). Compared with the Pt/HZ-75 catalyst, all the Pt-Ni/ZSM-5 catalysts exhibited excellent hydrodeoxygenation catalytic activity, and the introduction of Ni significantly improved the conversion rate and enhanced the selectivity to bicyclohexane. Furthermore, with the decrease of Pt/Ni ratio in Pt-Ni/ZSM-5 catalyst, the catalytic activity of Pt-Ni catalysts gradually increased, while the selectivity to bicyclohexane first increased and then decreased. The Pt-3Ni/HZ-75 catalyst showed the best catalytic activity and bicyclohexane selectivity at 3 MPa and 260℃. After 4 h of reaction, the conversion rate reached 100% and the bicyclohexane selectivity reached 43%.

Key words: catalysis, binary mixture, moleclar sieves, lignin, hydrodeoxygenation, hierarchical ZSM-5, bimetal

摘要:

利用等体积共浸渍法制备了级孔ZSM-5分子筛负载Pt-Ni双金属催化剂,并系统研究了不同Pt/Ni比对愈创木酚和二苯并呋喃二元混合物加氢脱氧反应性能的影响。采用XRD、N2-BET、SEM、TEM和H2-TPR对Pt-Ni催化剂的形貌和结构进行了表征。Ni掺入量较少时(1%和3%,质量分数),有利于促进活性金属的分散,增强Pt-Ni双金属之间的协同作用;当Ni掺入量增加到5%时,活性金属出现较严重的团聚。二元混合物加氢脱氧实验结果表明与单金属Pt/HZ-75相比,双金属Pt-Ni/ZSM-5催化剂均表现出优异的加氢脱氧催化活性,Ni的引入显著提高了反应转化速率,并提高了产物中联环己烷的选择性。随着Pt/Ni比的降低,Pt-Ni催化剂的活性逐渐增加,而联环己烷选择性先升高后降低。Pt-3Ni/HZ-75催化剂在3 MPa、260℃下表现出最佳的催化活性和联环己烷选择性,反应4 h后转化率达到100%,联环己烷选择性达到43%。

关键词: 催化, 二元混合物, 分子筛, 木质素, 加氢脱氧, 级孔ZSM-5, 双金属

CLC Number: