Kinetic Modeling of Deep Oxidative Desulfurization over Functionalized UiO-66 from a Model Fuel Using Complex Reaction Theory

利用复杂反应理论对功能化UiO-66催化剂上模型燃料的深度氧化脱硫进行动力学建模

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Abstract

This study proposes a systematic and straightforward approach for determining basic reaction routes and overall reactions using the theory of complex kinetics for an oxidative desulfurization (ODS) reaction using solvothermally synthesized metalorganic framework (MOF), UiO-66-NO(2) as a catalyst to remove the dibenzothiophene (DBT) from a model fuel in the temperature range of 20-100 °C. The intermediates are organized in a ″matrix of intermediates″ that simplifies the elementary reactions combination to form overall reactions. Adsorption, oxidation, and desorption were taken into consideration in 11 basic reaction steps that comprised the suggested ODS mechanism. The model's kinetic parameters were optimized by MATLAB program and described by the reparametrized Arrhenius equation. Markov chain Monte Carlo (MCMC) modeling was used to investigate the dependability of the estimated parameters and model predictions. The experimental results were satisfactorily in agreement with the model predictions, as the complex reaction was utilized for the first time to investigate the ODS reaction over MOFs.

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