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Selective hydrodeoxygenation of bio-oil derived products: ketones to olefins

机译：生物油衍生产品的选择性加氢脱氧：酮酮

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The hydrodeoxygenation (HDO) of various ketones (acetone, methyl ethyl ketone and cyclohexanone) to olefins via hydrogenation-dehydration was conducted in a fixed bed reactor at 373-573 K under H-2. A ketone can be hydrogenated over the metal function to an alcohol intermediate that is subsequently dehydrated to an olefin over the acidic function. A preliminary study on hydrogenation of acetone to 2-propanol over metal/SiO2 catalysts (Cr, Fe, Co, Ni, Cu and Pd) shows that Ni and Cu are active at >373 K. Although Ni possesses an activity higher than that of Cu, it promotes olefin hydrogenation and alcohol hydrogenolysis at >473 K. Hydrogenolysis of alcohol intermediate is suppressed over the Ni-Cu alloy catalyst. An optimum conversion with 100% selectivity to alcohol, can be obtained at 448 and 473 K for Ni and Cu, respectively. The dehydration of 2-propanol to propylene over proton zeolites (ZSM-5, Y, Mordenite and beta) can be achieved at >398 K. The zeolites with three-dimensional pore structure (beta and Y) provide relatively higher activity (>90% conversion). However, a bimolecular dehydration to ether is also promoted. Only HZSM-5 shows excellent selectivity to propylene (98%). Hydrodeoxygenation of ketones was tested with (i) a double bed of 5% Ni/SiO2 and HZSM-5 (Si/Al similar to 13), (ii) a physical mixed bed of 5% Cu/SiO2 and HZSM-5 (Si/Al similar to 13) and (iii) a bi-functional catalyst of 5% Cu/HZSM-5 (Si/Al similar to 250). It was found that high alkene selectivity was readily obtained at 448 K. While, over the physical mixed bed and bi-functional catalyst, the hydrogenation activity was enhanced as the alcohol intermediate was removed from the system. The reactivity of the ketone depends on its adsorption on the metal surface and steric hindrance, i.e. acetone > cyclohexanone > methyl ethyl ketone.
机译：在H-2下，在373-573 K的固定床反应器中，在H-2下，在固定床反应器中进行了各种酮（丙酮，甲基乙基酮和环己酮）的氢脱氧（HDO）。酮可以在金属函数上氢化为酒精中间体，该中间体随后在酸性功能上脱水至烯烃。一项关于金属/SIO2催化剂（CR，FE，CO，Ni，Cu和Pd）丙酮氢化至2-丙醇的初步研究，表明Ni和Cu在> 373 K上具有活性。尽管Ni的活性高于高于的活性Cu，它在> 473 K处促进烯烃氢化和酒精氢解。在Ni-Cu合金催化剂上，酒精中间体的氢解会抑制。对于Ni和Cu，可以在448 K和473 K下获得100％选择性的最佳转化率。在质子沸石（ZSM-5，Y，冬日纪和β）上，2-丙二醇向丙烯脱水在> 398 K时可以实现。具有三维孔结构（β和Y）的沸石可提供相对较高的活性（> 90> 90 ％ 转换）。然而，还促进了向醚的双分子脱水。仅HZSM-5对丙烯的选择性极佳（98％）。用（i）5％Ni/siO2和HZSM-5（Si/Al类似于13）的双床测试了酮的氢氧合，（ii）5％CU/SIO2和HZSM-5的物理混合床（SI） /Al类似于13）和（iii）5％CU/HZSM-5（Si/Al类似于250）的双功能催化剂。发现在448 K处很容易获得高烯烃选择性。而在物理混合床和双功能催化剂上，随着酒精中间体从系统中除去，氢化活性得到了增强。酮的反应性取决于其在金属表面和空间障碍上的吸附，即丙酮>环己酮>甲基乙基酮。

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