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Molybdenum modified nickel phyllosilicates as a high performance bifunctional catalyst for deoxygenation of methyl palmitate to alkanes under mild conditions
Green Chemistry ( IF 9.8 ) Pub Date : 2017-08-17 00:00:00 , DOI: 10.1039/c7gc01720k
Long Yan 1, 2, 3, 4, 5 , Xinxin Liu 1, 2, 3, 4, 5 , Jin Deng 1, 2, 3, 4, 5 , Yao Fu 1, 2, 3, 4, 5
Affiliation  

Deoxygenation is the central challenge in converting bio-derived fatty esters into diesel-range hydrocarbons. A new molybdenum oxide doping nickel phyllosilicate (Mo–Ni@PSi) bifunctional catalyst was synthesized and used for the deoxygenation of methyl palmitate. Compared to impregnated Ni catalysts, Mo–Ni@PSi catalysts showed obviously enhanced catalytic activity for the deoxygenation process. Several structural variations induced by the introduction of Mo species were confirmed by H2-TPR, XRD, FT-IR, TEM, XPS, and NH3-TPD characterization. With these variations, more dispersive Ni nanoparticles (Ni NPs) and acidic sites were explored over the surface of modified Mo–Ni@PSi, which provided high catalytic activity for the deoxygenation of fatty esters. Furthermore, the content of the Mo element and the influences of activation temperature on the catalyst were also investigated. Remarkably, the highest catalytic activity was observed over the 3% Mo–Ni@PSi(B) catalyst with 98.3% yield of hydrocarbons at 220 °C and 1.0 MPa H2, and the catalytic activity decreased with further increase in the Mo content. Then, hydrodeoxygenation and decarbonylation processes were both confirmed in the reaction mechanism study. Additionally, the catalyst also presented good catalytic activity after four recycle reactions. The oxidization of reduced Ni and Mo species was probably the main reason for the deactivation of the catalyst.

中文翻译:

钼改性页硅酸镍作为高性能双功能催化剂,可在温和条件下将棕榈酸甲酯脱氧成烷烃

脱氧是将生物来源的脂肪酯转化为柴油范围的碳氢化合物的主要挑战。合成了一种新型的氧化钼掺杂的页硅酸镍(Mo–Ni @ PSi)双功能催化剂,并将其用于棕榈酸甲酯的脱氧。与浸渍的Ni催化剂相比,Mo–Ni @ PSi催化剂对脱氧过程的催化活性明显增强。H 2 -TPR,XRD,FT-IR,TEM,XPS和NH 3证实了由Mo的引入引起的几种结构变异。-TPD表征。通过这些变化,在改性Mo-Ni @ PSi的表面上探索了更多分散的Ni纳米颗粒(Ni NPs)和酸性位点,这为脂肪酯的脱氧提供了高催化活性。此外,还研究了Mo元素的含量和活化温度对催化剂的影响。值得注意的是,在220°C和1.0 MPa H 2的条件下,在3%Mo–Ni @ PSi(B)催化剂上观察到了最高的催化活性,烃产率为98.3%,并且随着Mo含量的进一步增加,催化活性降低。然后,在反应机理研究中证实了加氢脱氧和脱羰过程。另外,该催化剂在四个循环反应后也表现出良好的催化活性。还原的Ni和Mo物种的氧化可能是催化剂失活的主要原因。
更新日期:2017-09-04
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