Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene,Catalysis Science & Technology

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Heterogeneous Pt-catalyzed transfer dehydrogenation of long-chain alkanes with ethylene
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-11-09 , DOI: 10.1039/d3cy00370a
Tim de la Croix ₁ , Nathalie Claes ₂ , Samuel Eyley ₃ , Wim Thielemans ₃ , Sara Bals ₂ , Dirk De Vos ₁

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The dehydrogenation of long-chain alkanes to olefins and alkylaromatics is a challenging endothermic reaction, typically requiring harsh conditions which can lead to low selectivity and coking. More favorable thermodynamics can be achieved by using a hydrogen acceptor, such as ethylene. In this work, the potential of heterogeneous platinum catalysts for the transfer dehydrogenation of long-chain alkanes is investigated, using ethylene as a convenient hydrogen acceptor. Pt/C and Pt–Sn/C catalysts were prepared via a simple polyol method and characterized with CO pulse chemisorption, HAADF-STEM, and EDX measurements. Conversion of ethylene was monitored via gas-phase FTIR, and distribution of liquid products was analyzed via GC-FID, GC-MS, and 1H-NMR. Compared to unpromoted Pt/C, Sn-promoted catalysts show lower initial reaction rates, but better resistance to catalyst deactivation, while increasing selectivity towards alkylaromatics. Both reaction products and ethylene were found to inhibit the reaction significantly. At 250 °C for 22 h, TON up to 28 and 86 mol per mol Pt were obtained for Pt/C and PtSn₂/C, respectively, with olefin selectivities of 94% and 53%. The remaining products were mainly unbranched alkylaromatics. These findings show the potential of simple heterogeneous catalysts in alkane transfer dehydrogenation, for the preparation of valuable olefins and alkylaromatics, or as an essential step in various tandem reactions.

中文翻译：

长链烷烃与乙烯的非均相 Pt 催化转移脱氢

长链烷烃脱氢为烯烃和烷基芳烃是一种具有挑战性的吸热反应，通常需要恶劣的条件，这可能导致低选择性和焦化。使用氢受体（例如乙烯）可以实现更有利的热力学。在这项工作中，使用乙烯作为方便的氢受体，研究了非均相铂催化剂在长链烷烃转移脱氢中的潜力。通过简单的多元醇方法制备 Pt/C 和 Pt-Sn/C 催化剂，并通过 CO 脉冲化学吸附、HAADF-STEM 和 EDX 测量进行表征。通过气相 FTIR 监测乙烯的转化率，并通过 GC-FID、GC-MS 和 1H-NMR 分析液体产物的分布。与未促进的 Pt/C 相比，Sn 促进的催化剂表现出较低的初始反应速率，但对催化剂失活的抵抗力更好，同时提高了对烷基芳烃的选择性。发现反应产物和乙烯均对反应有显著抑制作用。在 250 °C 下 22 小时，Pt/C 和 PtSn₂/C 的 TON 分别高达 28 和 86 mol/mol Pt，烯烃选择性分别为 94% 和 53%。其余产物以无支链烷基芳烃为主。这些发现表明，简单的非均相催化剂在烷烃转移脱氢中的潜力，用于制备有价值的烯烃和烷基芳烃，或作为各种串联反应中的重要步骤。

更新日期：2023-11-09

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