Multifunctional Catalysts for Direct Conversion of Alcohols to Long-Chain Hydrocarbons via Deoxygenative Olefination

被引：4

作者：

Ainembabazi, Diana ^{[1
]}

Horlyck, Jonathan ^{[1
]}

Dolan, Darren ^{[1
]}

Finn, Matthew ^{[1
,2
]}

Lee, Adam Fraser ^{[3
]}

Wilson, Karen ^{[3
]}

Voutchkova-Kostal, Adelina ^{[1
]}

机构：

[1] George Washington Univ, Chem Dept, Washington, DC 20052 USA

[2] Naval Res Lab, Washington, DC 20375 USA

[3] RMIT Univ, Sch Sci, Melbourne, Vic 3001, Australia

来源：

ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2021年 / 9卷 / 44期

基金：

美国国家科学基金会;

关键词：

Fuels from renewable alcohols; Decarbonylation; Olefination; Dehydrogenation; Palladium; Alumina; Magnesium oxide; Hydrotalcite; PD NANOPARTICLES; TRANSITION-METAL; N-BUTANOL; HYDROTALCITE; ETHANOL; HYDROGENATION; SUPPORT; DECARBONYLATION; CONDENSATION; SPECIATION;

D O I：

10.1021/acssuschemeng.1c05436

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Multistep H-2-free upgrading of alcohols to liquid hydrocarbons is highly desirable for producing drop-in fuel substitutes, but the limited reports of this process for select substrates require multiple catalysts , OH and bases, resulting in limited applicability. Direct conversion processes that rely on multifunctional catalysts and do not require base are yet to be reported. Here we describe such a Pd-catalyzed deoxygenative coupling of heptanol with heterogeneous catalysts composed of Pd immobilized on acid- base supports, which actively participate in the reaction cascade. The supports include primarily basic MgO, acidic gamma-Al2O3, and Mg-Al hydrotalcite (HT), with a combination of Lewis acidic and basic sites. Pd-HTs with 1% and 5 wt % Pd loading afforded the highest overall activity in the multistep cascade, yielding 30% hydrocarbons (tridecene 6-E-tridecene and tridecane) from a neat reaction with heptanol with 0.2 mol % Pd loading. Heterogeneity tests suggest that Pd-HT is operationally heterogeneous. The impact of support selection on the activity and selectivity offers insights into the design principles for next-generation catalysts for this process and related transformations.

引用

页码：14657 / 14662

页数：6