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高碳糠基甲烷在铼改性的铱催化剂上催化加氢脱氧生成可再生喷气燃料范围烷烃。

Catalytic Hydrodeoxygenation of High Carbon Furylmethanes to Renewable Jet-fuel Ranged Alkanes over a Rhenium-Modified Iridium Catalyst.

机构信息

Catalysis Center for Energy Innovation, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA.

出版信息

ChemSusChem. 2017 Aug 24;10(16):3225-3234. doi: 10.1002/cssc.201700863. Epub 2017 Jul 27.

Abstract

Renewable jet-fuel-range alkanes are synthesized by hydrodeoxygenation of lignocellulose-derived high-carbon furylmethanes over ReO -modified Ir/SiO catalysts under mild reaction conditions. Ir-ReO /SiO with a Re/Ir molar ratio of 2:1 exhibits the best performance, achieving a combined alkanes yield of 82-99 % from C -C furylmethanes. The catalyst can be regenerated in three consecutive cycles with only about 12 % loss in the combined alkanes yield. Mechanistically, the furan moieties of furylmethanes undergo simultaneous ring saturation and ring opening to form a mixture of complex oxygenates consisting of saturated furan rings, mono-keto groups, and mono-hydroxy groups. Then, these oxygenates undergo a cascade of hydrogenolysis reactions to alkanes. The high activity of Ir-ReO /SiO arises from a synergy between Ir and ReO , whereby the acidic sites of partially reduced ReO activate the C-O bonds of the saturated furans and alcoholic groups while the Ir sites are responsible for hydrogenation with H .

摘要

通过在温和的反应条件下,用 ReO -修饰的 Ir/SiO 催化剂将木质纤维素衍生的高碳糠基甲烷加氢脱氧,合成可再生喷气燃料范围的链烷烃。Re/Ir 摩尔比为 2:1 的 Ir-ReO /SiO 表现出最佳性能,从 C -C 糠基甲烷中获得 82-99%的组合链烷烃产率。该催化剂可在三个连续循环中再生,组合链烷烃产率仅损失约 12%。从机理上讲,糠基甲烷中的呋喃部分同时进行环饱和和开环反应,形成由饱和呋喃环、单酮基和单羟基组成的复杂含氧物混合物。然后,这些含氧化合物经历一系列氢解反应生成链烷烃。Ir-ReO /SiO 的高活性源于 Ir 和 ReO 之间的协同作用,其中部分还原的 ReO 的酸性位激活饱和呋喃和醇基的 C-O 键,而 Ir 位负责与 H 进行加氢反应。

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