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Hydrogenation of cinnamaldehyde to cinnamyl alcohol with metal phosphides: Catalytic consequences of product and pyridine doping
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2020-06-25 , DOI: 10.1016/j.apcatb.2020.119272
Yolanda Bonita , Varsha Jain , Feiyang Geng , Timothy P. O’Connell , Norbert X. Ramos , Neeraj Rai , Jason C. Hicks

Selective hydrogenation of α,β-unsaturated aldehydes is challenging due to the competition between unsaturated functional groups (C = C and C = O) with the catalyst. This study probes the use of metal phosphides as selective catalysts for cinnamaldehyde hydrogenation. Monometallic phosphides (MP; M = Ni, Co, Ru) showed high affinity to C = C hydrogenation, with 98% selectivity to hydrocinnamaldehyde with both Ni2P and Co2P. Bimetallic RuMoP improved the cinnamyl alcohol (COL) selectivity up to 91%, while bimetallic NiMoP preferred C = C hydrogenation to hydrocinnamaldehyde. Density functional theory (DFT) suggested greater charge transfer between the carbonyl oxygen and Mo sites on the surface leading to a lower activation energy barrier for cinnamaldehyde hydrogenation to COL. Product and pyridine doping studies resulted in an increased selectivity to COL possibly through surface coverage effects. Lastly, diffuse reflectance infrared Fourier transform spectra and DFT provided insights into the CAL adsorption mode and the reaction mechanism that supported the experimental observation.



中文翻译:

金属磷化物将肉桂醛加氢为肉桂醇:产物和吡啶掺杂的催化作用

由于不饱和官能团(C = C和C = O)与催化剂之间的竞争,α,β-不饱和醛的选择性加氢具有挑战性。这项研究探讨了使用金属磷化物作为肉桂醛加氢的选择性催化剂。单金属磷化物(MP; M = Ni,Co,Ru)对C = C的氢化反应显示出高亲和力,同时对Ni 2 P和Co 2的氢化肉桂醛有98%的选择性P.双金属RuMoP将肉桂醇(COL)的选择性提高了91%,而双金属NiMoP优选将C = C氢化为氢肉桂醛。密度泛函理论(DFT)表明,羰基氧和表面Mo位置之间的电荷转移更多,导致肉桂醛加氢生成COL的活化能垒较低。产物和吡啶掺杂研究可能通过表面覆盖效应提高了对COL的选择性。最后,漫反射红外傅里叶变换光谱和DFT提供了对CAL吸附模式和支持实验观察的反应机理的见解。

更新日期:2020-06-25
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