Catalytic oxidative/extractive desulfurization of model and untreated diesel using hybrid based zinc-substituted polyoxometalates

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• 作者：Susana O. Ribeiro^a ; Diana Juliã ; o^a ; Luí ; s Cunha-Silva^a ; Valentina F. Domingues^b ; Rita Valenç ; a^c ; Jorge C. Ribeiro^c ; Baltazar de Castro^a ; Salete S. Balula^a ; ^{sbalula@fc.up.pt" class="auth_mail" title="E-mail the corresponding author}
• 关键词：Oxidative/extractive desulfurization ; Zinc substituted polyoxometalates ; Hybrid polyoxometalates ; Real diesel
• 刊名：Fuel
• 出版年：2016
• 出版时间：15 February 2016
• 年：2016
• 卷：166
• 期：Complete
• 页码：268-275
• 全文大小：694 K

文摘

The desulfurization efficiency of various hybrid zinc-substituted polyoxometalates ([PW₁₁Zn(H₂O)O₃₉]⁵⁻, abbreviated as PW₁₁Zn) was here investigated for the first time and optimized using sustainable systems conciliating successfully the liquid–liquid extraction and the oxidative catalytic process. Initially, the desulfurization studies were performed using a model diesel containing a mixture of the most refractory sulfur compounds and later extended to an untreated real diesel. In both cases, acetonitrile was used as extraction solvent and aqueous H₂O₂ as oxidant. High level of desulfurization was achieved using model and untreated diesels after few hours. The quaternary ammonium catalysts (TBAPW₁₁Zn and ODAPW₁₁Zn) showed higher catalytic desulfurization efficiency than the ionic liquid catalyst (BMIPW₁₁Zn). The TBAPW₁₁Zn behaved as a homogeneous catalyst immobilized in the extraction solvent, while the ODAPW₁₁Zn with the long carbon chain behaved as a heterogeneous catalyst capable to be recovered from the system. Both quaternary ammonium catalysts showed to be successfully reused/recycled for various consecutive desulfurization cycles.