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Guaiacol Hydrodeoxygenation over Pd Catalyst with Mesoporous ZSM-5 Support Synthesized by Solid-State Crystallization
Catalysis Today ( IF 5.2 ) Pub Date : 2020-03-06 , DOI: 10.1016/j.cattod.2020.03.009
Yuxin Wang , Huijiang Huang , Nathan C. Baxter , Yixin Liao , Yujun Zhao , Shengnian Wang

Mesoporous structure is important to promote mass transport and active site utilization of zeolites when used in reactions involving bulky molecules. However, their conventional hydrothermal synthesis is energy and labor intensive, requiring high-pressure operation, and lengthy heating a huge amount of alkaline liquid. We successfully synthesized new mesoporous zeolites, Meso-ZSM-5, via solid-state crystallization of dry aluminosilicate nanogels. Neighbor developing nanocrystals further joint at edges, creating connected, inter-lattice mesoscale pathway in the finished single crystalline zeolites. Palladium was further loaded on these zeolites to form a bi-functional catalyst (Pd/Meso-ZSM-5). When used in the hydrodeoxygenation (HDO) of guaiacol, a major bio-oil compound with disappointing conversion and severe coking issue over many HDO catalysts, Pd/Meso-ZSM-5 exhibits superior guaiacol conversion and product distribution when compared with those supported on conventional microporous ZSM-5 counterparts. This is attributed to the improved diffusion and accessibility of active sites inside Meso-ZSM-5 with its unique hierarchically porous structure. Ring saturated hydrocarbons are largely produced at 200 °C when hydrogenation dominates while alkaylated aromatics become major HDO products as deoxygenation becomes favorable at 250 °C. These encouraging results may ignite the wide use of these mesoporous zeolites in many other reactions in both traditional fossil fuel and emerging renewable energy fields.



中文翻译:

固态结晶合成介孔ZSM-5载体在Pd催化剂上的愈创木酚加氢脱氧

当用于涉及大分子的反应中时,中孔结构对于促进沸石的传质和活性位点利用很重要。然而,它们常规的水热合成是能量和劳动密集的,需要高压操作,并且长时间加热大量的碱性液体。我们通过固态结晶干燥铝硅酸盐纳米凝胶成功地合成了新的介孔沸石Meso-ZSM-5。相邻的纳米晶体在边缘进一步接合,在完成的单晶沸石中形成连接的晶格间介观途径。将钯进一步负载在这些沸石上以形成双官能催化剂(Pd / Meso-ZSM-5)。当用于愈创木酚的加氢脱氧(HDO)时,一种主要的生物油化合物,其转化率令人失望,并且在许多HDO催化剂上存在严重的焦化问题,与传统的微孔ZSM-5对应物相比,Pd / Meso-ZSM-5表现出优异的愈创木酚转化率和产物分布。这归因于Meso-ZSM-5内部具有独特的分层多孔结构的活性位点具有更好的扩散性和可及性。当氢化作用占主导地位时,在200°C时会大量生成环状饱和烃,而在250°C时脱氧变得有利时,烷基化的芳族化合物将成为主要的HDO产品。这些令人鼓舞的结果可能会点燃这些中孔沸石在传统化石燃料和新兴可再生能源领域的许多其他反应中的广泛使用。这归因于Meso-ZSM-5内部具有独特的分层多孔结构的活性位点具有更好的扩散性和可及性。当氢化作用占主导地位时,在200°C时会大量生成环状饱和烃,而在250°C时脱氧变得有利时,烷基化的芳族化合物将成为主要的HDO产品。这些令人鼓舞的结果可能会点燃这些中孔沸石在传统化石燃料和新兴可再生能源领域的许多其他反应中的广泛使用。这归因于Meso-ZSM-5内部具有独特的分层多孔结构的活性位点具有更好的扩散性和可及性。当氢化作用占主导地位时,在200°C时会大量生成环状饱和烃,而在250°C时脱氧变得有利时,烷基化的芳族化合物将成为主要的HDO产品。这些令人鼓舞的结果可能会点燃这些中孔沸石在传统化石燃料和新兴可再生能源领域的许多其他反应中的广泛使用。

更新日期:2020-03-06
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