Short channeled Ni-Co/SBA-15 catalysts for highly selective hydrogenation of biomass-derived furfural to tetrahydrofurfuryl alcohol

Short channeled Ni-Co/SBA-15 catalysts for highly selective hydrogenation of biomass-derived furfural to tetrahydrofurfuryl alcohol
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用于生物质糠醛高选择性加氢制四氢糠醇的短通道Ni-Co/SBA-15催化剂

DOI:
10.1016/j.micromeso.2017.11.027
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发表时间:
2018-05-15
影响因子:
5.2
通讯作者:
Xiao, Guomin
Xiao, Guomin
中科院分区:
材料科学2区
文献类型:
--
作者:
Li, Shuai;Wang, Yuan;Xiao, Guomin

文献摘要

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采用无贵金属、无毒的双金属镍钴催化剂,进行了糠醛(FFR)加氢一步液相反应制四氢糠醇(THFA)的研究。以短孔道SBA-15为载体,采用浸渍法制备了不同Ni/Co摩尔比的Ni-Co催化剂和Ni、Co两种单金属催化剂。其中Ni-Co/SBA-15催化剂具有较高的FFR加氢选择性。研究了Ni/Co摩尔比的影响,其中在裸载体中具有固定的Ni负载(10重量%)。采用N2吸附、XRD、XPS、H2-TPR、SEM、TEM和CO化学吸附等手段对样品进行了表征。结果表明,适量的尖晶石型NiCo 2 O 4氧化物有利于Ni-0和CoO在短孔道SBA-15上的均匀、高分散,有利于提高催化剂的催化性能。在催化剂活性方面,以MCM-41、MCM-4、MCF-2和普通SBA-15为载体,考察了反应温度、氢气初始压力、反应时间和催化剂重复使用性能等对催化剂活性的影响。当Ni与Co的摩尔比为0.67时,在90 ℃、初始H2为50 bar、反应时间为2.0 h的条件下,催化剂Ni-Co/SBA-15的FFR转化率为100%,四氢叶酸选择性为92.1%。
Liquid phase and one-step reaction for furfural (FFR) hydrogenated to tetrahydrofurfuryl alcohol (THFA) was conducted by employing noble metal-absence and toxicity-free, bimetallic Ni-Co catalysts. The bimetallic Ni-Co catalysts with different molar ratio of Ni to Co and two monometallic catalysts (Ni, Co) were synthesized by conventional incipient-wetness impregnation method with short channeled SBA-15 as support. Among these catalysts, highly selective hydrogenation of FFR to THFA was attained over Ni-Co/SBA-15 catalysts. The impact of molar ratio of Ni/Co was studied with a fixed Ni loading (10 wt %) in bare support. The samples were characterized by N-2 sorption, XRD, XPS, H-2-TPR, SEM, TEM and CO chemisorpdon. The results confirmed that the reducibility of Ni-catalysts can be improved by incorporating Co metal and revealed that appropriate amount of spinel NiCo2O4 oxides is favorable to uniform and high dispersion of Ni-0 and CoO over short channeled SBA-15, which would be benefit for the catalytic performance. For catalytic activity investigation, other four mesoporous SiO2 materials (MCM-41, MCM-4, MCF-2 and common SBA-15) were employed as supports to investigate the effect on the hydrogenation of FFR and the reaction parameters including the reaction temperature, initial of H-2 pressure, reaction time and the reusability of the catalysts were also studied. 100% of FFR conversion and 92.1% of THFA selectivity were achieved at 90 degrees C, 50 bar of initial H-2 and 2.0 h over catalyst Ni-Co/SBA-15 when the molar ratio of Ni to Co was 0.67.