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Selective Hydrodeoxygenation of 5-Hydroxymethylfurfuralto 25-Dimethylfuran over Ni Supported on Zirconium Phosphate Catalysts

机译:5-羟基甲基糠醛的选择性加氢脱氧磷酸锆负载的镍上的二氯苯甲酸制备25-二甲基呋喃

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摘要

Crystal α-zirconium phosphate (α-ZrP) was prepared by a hydrothermal method and exfoliated into a layered structure by n-hexylamine (C6H13NH2). Ni-based catalyst (Ni/ZrP) was promoted by loading nickel on the layered α-ZrP via ion exchange. The catalyst was performed to catalyze hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), and a 68.1% yield of DMF and 100% conversion of HMF were achieved at 240 °C, 5 MPa H2, and 20 h. The DMF yield can still retain 52.8% after five cycles. The characteristics of the catalyst were investigated via N2 adsorption–desorption, X-ray diffraction, field emission scanning electron microscopy, high-resolution transmission electron microscopy, pyridine-adsorbed Fourier transform infrared (FTIR) spectra, FTIR spectra, inductively coupled plasma mass spectrometry, and thermogravimetric analysis–mass spectrometry, as well as Raman spectroscopy. A pathway from HMF to DMF was found with MF as the intermediate product, and DMF production was preferable via the −CH2OH group hydrogenolysis of HMF overLewis acidic sites of Ni/ZrP, which is caused by the zirconium vacantorbits.
机译:通过水热法制备晶体α-磷酸锆(α-ZrP),并通过正己胺(C6H13NH2)将其剥离成层状结构。通过离子交换将镍负载在层状α-ZrP上可以促进Ni基催化剂(Ni / ZrP)的生长。进行该催化剂以催化5-羟甲基糠醛(HMF)加氢脱氧为2,5-二甲基呋喃(DMF),在240°C,5 MPa H2和20°C的条件下,DMF的收率为68.1%,HMF的转化率为100%。 H。在五个周期后,DMF产率仍可保持52.8%。通过N2吸附-脱附,X射线衍射,场发射扫描电子显微镜,高分辨率透射电子显微镜,吡啶吸附傅立叶变换红外(FTIR)光谱,FTIR光谱,电感耦合等离子体质谱法研究了催化剂的特性,热重分析,质谱以及拉曼光谱。发现以HMF为中间产物从HMF到DMF的途径,通过HMF的-CH2OH基团氢解反应,DMF的产生是优选的。Ni / ZrP的路易斯酸性位点,这是由锆空位引起的轨道。

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