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Ni/HZSM-5 catalyst preparation by deposition-precipitation. Part 2. Catalytic hydrodeoxygenation reactions of lignin model compounds in organic and aqueous systems
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-06-15 , DOI: 10.1016/j.apcata.2018.06.012
R.R. Barton , M. Carrier , C. Segura , J.L.G. Fierro , S. Park , H.H. Lamb , N. Escalona , S.W. Peretti

Nickel metal supported on HZSM-5 (zeolite) is a promising catalyst for lignin depolymerization. In this work, the ability of catalysts prepared via deposition-precipitation (DP) to perform hydrodeoxygenation (HDO) on two lignin model compounds in organic and aqueous solvents was evaluated; guaiacol in dodecane and 2-phenoxy-1-phenylethanol (PPE) in aqueous solutions. All Ni/HZSM-5 catalysts were capable of guaiacol HDO into cyclohexane at 523 K. The role of the HZSM-5 acid sites was confirmed by comparison with Ni/SiO2 (inert support) which exhibited incomplete deoxygenation of guaiacol due to the inability to perform the cyclohexanol dehydration step. The catalyst prepared with 15 wt% Ni, a DP time of 16 h, and a calcination temperature of 673 K (Ni(15)/HZSM-5 DP16_Cal673), performed the guaiacol conversion with the greatest selectivity towards HDO products, with an intrinsic rate ratio (HDO rate to conversion rate) of 0.31, and 90% selectivity to cyclohexane. Catalytic activity and selectivity of Ni/HZSM-5 (15 wt%) in aqueous environments (water and 0.1 M NaOH solution) was confirmed using PPE reactions at 523 K. After 30 min reaction time in water, Ni/HZSM-5 exhibited ∼100% conversion of PPE, and good yield of the desired products; ethylbenzene and phenol (∼35% and 23% of initial carbon, respectively). Ni/HZSM-5 in NaOH solution resulted in significantly higher ring saturation compared to the Ni/HZSM-5 in water or the NaOH solution control.



中文翻译:

通过沉积沉淀法制备Ni / HZSM-5催化剂。第2部分。木质素模型化合物在有机和水性体系中的催化加氢脱氧反应

负载在HZSM-5(沸石)上的镍金属是木质素解聚的有前途的催化剂。在这项工作中,评估了通过沉积沉淀(DP)制备的催化剂在有机和水性溶剂中对两种木质素模型化合物进行加氢脱氧(HDO)的能力。十二烷中的愈创木酚和水溶液中的2-苯氧基-1-苯基乙醇(PPE)。所有Ni / HZSM-5催化剂均能够在523 K下将愈创木酚HDO转化为环己烷。通过与Ni / SiO 2的比较证实了HZSM-5酸位的作用(惰性载体)由于无法进行环己醇脱水步骤而显示出愈创木酚的不完全脱氧。用15 wt%Ni,DP时间为16 h,煅烧温度为673 K(Ni(15)/ HZSM-5 DP16_Cal673)制备的催化剂进行了愈创木酚转化,对HDO产物的选择性最高,具有固有的速率比(HDO率与转化率)为0.31,对环己烷的选择性为90%。Ni / HZSM-5(15 wt%)在水性环境(水和0.1 M NaOH溶液)中的催化活性和选择性通过523 K在PPE反应中得到证实。在水中反应30分钟后,Ni / HZSM-5表现出〜 PPE的100%转化率高,所需产物的收率高;乙苯和苯酚(分别约为起始碳的35%和23%)。

更新日期:2018-06-15
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