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Metal Oxide-Promoted Hydrodeoxygenation Activity of Platinum in Pt-MOx/Al2O3 Catalysts for Green Diesel Production
Energy & Fuels ( IF 5.2 ) Pub Date : 2018-12-01 00:00:00 , DOI: 10.1021/acs.energyfuels.8b03588 Sagar Janampelli 1, 2 , Srinivas Darbha 1, 2
Energy & Fuels ( IF 5.2 ) Pub Date : 2018-12-01 00:00:00 , DOI: 10.1021/acs.energyfuels.8b03588 Sagar Janampelli 1, 2 , Srinivas Darbha 1, 2
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Catalytic deoxygenation of fatty acids into renewable hydrocarbons (green diesel) was investigated over 4Pt-8MOx/Al2O3 (M = Mo, Re, W, and Sn) catalysts prepared by the wet impregnation method. Platinum deposited on MOx-modified γ-Al2O3 showed higher catalytic hydrodeoxygenation activity than that of the “neat” Pt/Al2O3 catalyst. The promotional effect of metal oxides (MOx) decreased in the following order: MoOx > ReOx > WOx > SnOx. Characterization studies revealed that metal oxides affect the textural and electronic properties of Pt. Supported Pt facilitated the reduction of these metal oxides. Synergy and electronic contact between Pt and MOx determined the catalytic deoxygenation performance. Fatty acid conversion increased with increasing metallic nature (decreasing binding energy) of Pt. Hydrodeoxygenation product selectivity correlated with the extent of metal oxide reduction. Among the catalysts, 4Pt-8MoOx/Al2O3 had the optimum dispersion, electron-rich Pt, and reduced Mo5+ species, enabling quantitative conversion of oleic acid with 93.5% octadecane selectivity at a temperature as low as 220 °C and 20 bar hydrogen pressure. Metal oxide switched the mechanism of deoxygenation from decarbonylation/decarboxylation to hydrodeoxygenation. Fatty acids, methyl oleate, and vegetable oil were deoxygenated with equal efficiency over this catalyst. Catalysts were reusable in recycling studies only at higher temperature (320 °C) and not at lower temperature (260 °C), perhaps due to strong sticking of reactant molecules at lower temperature on the catalyst surface than at higher temperature.
中文翻译：
Pt-MO x / Al 2 O 3催化剂在绿色柴油生产中的金属氧化物催化铂加氢脱氧活性
在通过湿法浸渍法制备的4Pt-8MO x / Al 2 O 3（M = Mo，Re，W和Sn）催化剂上，研究了将脂肪酸催化脱氧成可再生烃（绿色柴油）的方法。铂沉积在MO X改性的γ-Al 2 ö 3显示出比所述“纯”的Pt /铝的较高的催化加氢脱氧活性2 ö 3催化剂。金属氧化物（MO x）的促进作用按以下顺序降低：MoO x > ReO x > WO x > SnO x。表征研究表明，金属氧化物会影响Pt的质构和电子性能。负载的铂促进了这些金属氧化物的还原。Pt和MO x之间的协同作用和电子接触决定了催化脱氧性能。脂肪酸转化率随着Pt金属性质的增加（结合能的降低）而增加。加氢脱氧产物的选择性与金属氧化物的还原程度有关。在这些催化剂中，4Pt-8MoO x / Al 2 O 3具有最佳分散性，富电子的Pt和还原的Mo 5+物种，可在低至220°C和20 bar氢气压力下以93.5％十八烷选择性对油酸进行定量转化。金属氧化物将脱氧机理从脱羰/脱羧转变为加氢脱氧。在该催化剂上，脂肪酸，油酸甲酯和植物油以相同的效率脱氧。催化剂仅在较高温度（320°C）而不在较低温度（260°C）下才可在循环研究中重复使用，这可能是由于较低温度下的反应物分子与高温下相比在催化剂表面上的强烈粘着。
更新日期：2018-12-01
中文翻译：
Pt-MO x / Al 2 O 3催化剂在绿色柴油生产中的金属氧化物催化铂加氢脱氧活性
在通过湿法浸渍法制备的4Pt-8MO x / Al 2 O 3（M = Mo，Re，W和Sn）催化剂上，研究了将脂肪酸催化脱氧成可再生烃（绿色柴油）的方法。铂沉积在MO X改性的γ-Al 2 ö 3显示出比所述“纯”的Pt /铝的较高的催化加氢脱氧活性2 ö 3催化剂。金属氧化物（MO x）的促进作用按以下顺序降低：MoO x > ReO x > WO x > SnO x。表征研究表明，金属氧化物会影响Pt的质构和电子性能。负载的铂促进了这些金属氧化物的还原。Pt和MO x之间的协同作用和电子接触决定了催化脱氧性能。脂肪酸转化率随着Pt金属性质的增加（结合能的降低）而增加。加氢脱氧产物的选择性与金属氧化物的还原程度有关。在这些催化剂中，4Pt-8MoO x / Al 2 O 3具有最佳分散性，富电子的Pt和还原的Mo 5+物种，可在低至220°C和20 bar氢气压力下以93.5％十八烷选择性对油酸进行定量转化。金属氧化物将脱氧机理从脱羰/脱羧转变为加氢脱氧。在该催化剂上，脂肪酸，油酸甲酯和植物油以相同的效率脱氧。催化剂仅在较高温度（320°C）而不在较低温度（260°C）下才可在循环研究中重复使用，这可能是由于较低温度下的反应物分子与高温下相比在催化剂表面上的强烈粘着。
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