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Methane assisted catalyst synthesis and catalytic conversion of oleic acid
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2022-08-08 , DOI: 10.1039/d2ta04568k
Jack Samuel Jarvis 1 , Zhaofei Li 1 , Shijun Meng 1 , Hua Song 1
Affiliation  

Fatty acid deoxygenation is an important process if we are to realize the use of biocrudes as replacements for fossil fuels. A ZSM-5 support with 40% higher pore volume and increased surface area is realized by assisted synthesis under CH4. The catalyst exhibits a very good performance for deoxygenation of oleic acid (92% by mole) and selectivities towards aromatics (50.8 wt%) and syngas (14.8 wt%) when loaded with 5% Ce, 0.5% Ga, and 0.5% Pt metal particles. CH4 is also employed as the coreactant at mild temperature and pressure (400 °C and 30 bar) in a batch system. CH4 conversion is greatly enhanced over the CH4-synthesized support and is shown by 13CH4 experiments and 13C NMR to directly incorporate into the benzylic sites of the aromatics in the liquid product as well as CO2 in the gas phase. XPS is used to show that metal species (particularly Ce) are partially reduced prior to reaction, resulting from the ejection of CH4 pools trapped in the framework during synthesis, removing the need for a potentially expensive and time-consuming pre-reduction step. DSC and TPD studies also show that this material has a significantly higher capacity for methane adsorption, a potential result of methane imprinting from the synthesis process.

中文翻译:

甲烷辅助催化剂合成及油酸催化转化

如果我们要实现使用生物原油作为化石燃料的替代品,脂肪酸脱氧是一个重要的过程。通过在 CH 4下的辅助合成,实现了孔体积增加 40% 和表面积增加的 ZSM-5 载体。当负载 5% Ce、0.5% Ga 和 0.5% Pt 金属时,该催化剂表现出非常好的油酸脱氧性能(92% 摩尔)和对芳烃(50.8 重量%)和合成气(14.8 重量%)的选择性粒子。CH 4还用作间歇系统中温和温度和压力(400 °C 和 30 bar)下的共反应剂。与 CH 4合成的载体相比, CH 4转化率大大提高,并通过13 个CH 4实验和13 C NMR 直接结合到液体产物中芳烃的苄基位点以及气相中的 CO 2中。XPS 用于显示金属物质(尤其是 Ce)在反应前被部分还原,这是由于合成过程中被困在框架中的 CH 4池的排出而导致的,因此无需进行可能昂贵且耗时的预还原步骤。DSC 和 TPD 研究还表明,这种材料具有显着更高的甲烷吸附能力,这是合成过程中甲烷印记的潜在结果。
更新日期:2022-08-08
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