Insights into the production of upgraded biofuels using Mg‐loaded mesoporous ZSM‐5 zeolites,ChemCatChem

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Insights into the production of upgraded biofuels using Mg‐loaded mesoporous ZSM‐5 zeolites
ChemCatChem ( IF 3.8 ) Pub Date : 2020-07-03 , DOI: 10.1002/cctc.202000787
Olga Sanahuja‐Parejo ₁ , Alberto Veses ₁ , José Manuel López ₁ , María Soledad Callén ₁ , Benjamín Solsona ₂ , Nia Richards ₃ , Stuart H. Taylor ₃ , Tomás García ₁

Affiliation

Bio‐oil catalytic upgrading has been performed using mesoporous Mg‐loaded ZSM‐5. The presence of Mg modifies both textural and acidic properties, which do not only depend on the Mg content (1 and 5 wt. %) but also on the Si/Al ratio of the parent zeolite (25 and 40). Mg impregnation over mesoporous acidic zeolites has been shown to be essential for further deoxygenation of the raw bio‐oil. Thus, remarkable deoxygenation rates have been achieved, exceeding 68 % for a 5 wt. % Mg‐loaded ZSM‐5 (Si/Al=25). For this catalyst, decarboxylation reactions at MgO active sites seem to be predominant, promoting the upgrading of phenols towards the formation of phenolic compounds with lower oxygen content. As in the case of acidic mesoporous ZSM‐5, the formation of aromatics for Mg‐loaded mesoporous ZSM‐5 samples could be mainly related to the promotion of decarbonylation reactions of phenolic compounds over Brønsted acidic sites at the external surface. Interestingly, the presence of strong Lewis acidic sites created by the interaction between (Mg²⁺OH⁻)⁺ species and extra framework alumina jointly with the remaining Brønsted acidic sites at the external surface could enhance the formation of aromatics through cascade reactions involving ketonization and further aldol condensation and dehydration reactions.

中文翻译：

对使用负载Mg的中孔ZSM-5沸石生产升级版生物燃料的见解

已使用中孔加载Mg的ZSM-5对生物油进行了催化升级。Mg的存在会改变质构和酸性，这不仅取决于Mg含量（1和5 wt。％），还取决于母体沸石的Si / Al比（25和40）。业已证明，在中孔酸性沸石上浸渍镁对于生化生物油的进一步脱氧至关重要。因此，已经实现了显着的脱氧率，对于5wt。％，超过68％。含镁的ZSM-5（Si / Al = 25）％。对于这种催化剂，MgO活性位点的脱羧反应似乎占主导地位，从而促进了酚类的升级，从而形成了含氧量更低的酚类化合物。与酸性介孔ZSM-5一样，加载Mg的中孔ZSM-5样品中芳族化合物的形成可能主要与促进酚类化合物在外表面的Brønsted酸性位点上的脱羰反应有关。有趣的是，（Mg²⁺ OH ^-）⁺物种和额外的骨架氧化铝以及外表面上剩余的布朗斯台德酸性位点可通过涉及酮化作用以及进一步的羟醛缩合和脱水反应的级联反应增强芳烃的形成。

更新日期：2020-07-03

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