Selective synthesis of furfuryl acetate over solid acid catalysts and active site exploration using density functional theory,Catalysis Science & Technology

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Selective synthesis of furfuryl acetate over solid acid catalysts and active site exploration using density functional theory
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2022-05-30 , DOI: 10.1039/d2cy00334a
B. J. Vaishnavi _{1,

2} , S. Sujith ₁ , K. M. Rajashekhar Vaibhava ₃ , P. Jyothi Bhat ₁ , Rajappan Vetrivel ₃ , Ganapati V. Shanbhag _{1,

3}

Affiliation

Furfuryl acetate is obtained from the esterification of biomass derivative furfuryl alcohol which has potential applications as a biofuel additive, fragrance, and flavoring agent. For acid catalyzed reactions such as esterification, the integration of experimental outcomes with DFT studies to develop a method to derive a general correlation between active site energetics with catalytic activity is needed. Herein, various catalysts such as zeolites, mesoporous materials, ion-exchanged macro reticular resin, and silicoalumino phosphates with diverse physicochemical properties such as porosity, strength and amount of acidity, topology, and material stability were investigated for this transformation. The catalysts were characterized by PXRD, FTIR spectroscopy, ICP-OES, N₂ sorption study, NH₃-TPD, and SEM measurements to correlate the physicochemical properties with catalytic performance. Sulfated zirconia was the best performing catalyst which exhibited the highest furfuryl acetate yield of 95% at a low catalyst loading and reactant mole ratio with good recyclability. The excellent catalytic activity of the three top-performing catalysts (sulfated zirconia, SAPO-11 and Al-SBA-15) was explained using adsorption energies of various species on the catalyst by density functional theory (DFT) studies. Importantly, a new method of correlation was developed with respect to the hydrogen removal energy of the catalysts obtained from DFT which correlated well with the catalytic performance of distinctly different solid catalysts.

中文翻译：

固体酸催化剂上乙酸糠酯的选择性合成及利用密度泛函理论探索活性位点

醋酸糠酯是由生物质衍生物糠醇酯化得到的，糠醇具有作为生物燃料添加剂、香料和调味剂的潜在应用。对于酯化等酸催化反应，需要将实验结果与 DFT 研究相结合，以开发一种方法来推导活性位点能量学与催化活性之间的一般相关性。在此，研究了各种催化剂，如沸石、介孔材料、离子交换大网状树脂和磷酸硅铝，它们具有不同的物理化学性质，如孔隙率、强度和酸度、拓扑结构和材料稳定性。通过PXRD、FTIR光谱、ICP-OES、N ₂吸附研究、NH _{3对催化剂进行了表征}-TPD 和 SEM 测量将物理化学性质与催化性能相关联。硫酸化氧化锆是性能最好的催化剂，在低催化剂负载和反应物摩尔比下表现出最高的 95% 的乙酸糠酯产率，并具有良好的可回收性。通过密度泛函理论 (DFT) 研究，利用催化剂上各种物质的吸附能解释了三种性能最佳的催化剂（硫酸化氧化锆、SAPO-11 和 Al-SBA-15）的优异催化活性。重要的是，针对从 DFT 获得的催化剂的除氢能量开发了一种新的相关方法，该方法与明显不同的固体催化剂的催化性能密切相关。

更新日期：2022-05-30

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