Reactions of 2-Methyltetrahydropyran on Silica-Supported Nickel Phosphide in Comparison with 2-Methyltetrahydrofuran
Reactions of 2-Methyltetrahydropyran on Silica-Supported Nickel Phosphide in Comparison with 2-Methyltetrahydrofuran
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DOI：
10.1021/acscatal.6b01033
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发表时间：
2016-06
期刊：
影响因子：
12.9
通讯作者：
P. Bui;S. Oyama;Atsushi Takagaki;Brad P. Carrow;K. Nozaki
中科院分区：
文献类型：
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作者：
P. Bui;S. Oyama;Atsushi Takagaki;Brad P. Carrow;K. Nozaki
2-甲基四氢吡喃（2-MTHP, C6H12O）在Ni2P/SiO2上的反应提供了生物质原料中丰富成分环醚与有效加氢处理催化剂过渡金属磷化物之间相互作用的见解。在与快速热解相似的常压低接触时间条件下，2-MTHP与Ni2P/SiO2反应生成的产物中70%为脱氧产物，2-己烯和2-戊烯，具有良好的除氧能力。脱质子、氢解、脱水和脱碳是主要的反应途径。反应顺序从吸附2-MTHP开始，然后在甲基取代侧（路径I）或未取代侧（路径II）开环，产生吸附的醇氧化合物。在路径1中，伯胺醇在α-碳上被氧化生成醛，醛随后被脱碳生成2-戊烯。伯醇醇也可以质子化得到…
The reactions of 2-methyltetrahydropyran (2-MTHP, C6H12O) on Ni2P/SiO2 provide insights on the interactions between a cyclic ether, an abundant component of biomass feedstock, with a transition-metal phosphide, an effective hydrotreating catalyst. At atmospheric pressure and a low contact time, conditions similar to those of a fast pyrolysis process, 70% of products formed from the reaction of 2-MTHP on Ni2P/SiO2 were deoxygenated products, 2-hexene and 2-pentenes, indicating a good oxygen removal capacity. Deprotonation, hydrogenolysis, dehydration, and decarbonylation were the main reaction routes. The reaction sequence started with the adsorption of 2-MTHP, followed by ring-opening steps on either the methyl substituted side (Path I) or the unsubstituted side (Path II) to produce adsorbed alkoxide species. In Path I, a primary alkoxide was oxidized at the α-carbon to produce an aldehyde, which subsequently underwent decarbonylation to 2-pentenes. The primary alkoxide could also be protonated to give a ...