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Zr-Incorporating SBA-15 for conversion of the ethanol–acetaldehyde mixture to butadiene
Reaction Chemistry & Engineering ( IF 3.9 ) Pub Date : 2020-07-25 , DOI: 10.1039/d0re00160k
Guochao Yang 1, 2, 3, 4, 5 , Lingtao Wang 1, 2, 3, 4, 5 , Haoxi Jiang 1, 2, 3, 4, 5
Affiliation  

Upgrading bio-ethanol into high value chemicals is an important issue in biomass conversion, and conversion of ethanol into butadiene is one of the most feasible methods. Here Zr-incorporating mesoporous SBA-15 (Zr–SBA-15) materials with different Si/Zr ratios were successfully synthesized by a one-pot method and were employed as catalysts for the conversion of the ethanol (EtOH)–acetaldehyde (AcH) mixture to butadiene. The textural structure and acidity of Zr–SBA-15 were investigated by using XRD, N2 adsorption, TEM, FT-IR, UV-vis, XPS, NH3-TPD and Py-IR, and the results of these characterizations indicated the mesoporosity of Zr–SBA-15 and confirmed the incorporation of Zr into the framework. Zr–O–Si bonds were formed by the incorporation and exhibited Lewis acidity predominantly. The influence of the Si/Zr ratio and reaction conditions (temperature, EtOH/AcH ratio and WHSV) showed that a suitable Si/Zr ratio was needed to balance the butadiene selectivity, by-product selectivity and total conversion. Amongst the prepared catalysts, Zr–SBA-15-20 achieved the best butadiene selectivity of 74.0% at a relatively low temperature (275 °C). The good catalytic performance could be attributed to the homogeneous dispersion of Zr species and Zr–O–Si bond generated by Zr incorporation. Furthermore, EtOH-TPD and AcH-TPD experiments proved the essential role of acetaldehyde addition and the well-accepted reaction pathway.

中文翻译:

掺Zr的SBA-15可将乙醇-乙醛混合物转化为丁二烯

将生物乙醇转化为高价值化学品是生物质转化的重要问题,而将乙醇转化为丁二烯是最可行的方法之一。在这里,通过一锅法成功地合成了具有不同Si / Zr比的掺Zr介孔SBA-15(Zr–SBA-15)材料,并将其用作转化乙醇(EtOH)-乙醛(AcH)的催化剂混合成丁二烯。通过XRD,N 2吸附,TEM,FT-IR,UV-vis,XPS,NH 3考察了Zr–SBA-15的织构和酸度。-TPD和Py-IR,以及这些表征的结果表明Zr–SBA-15具有介孔性,并证实Zr已掺入框架中。Zr-O-Si键是通过结合形成的,主要表现出路易斯酸度。Si / Zr比和反应条件(温度,EtOH / AcH比和WHSV)的影响表明,需要合适的Si / Zr比来平衡丁二烯的选择性,副产物的选择性和总转化率。在制备的催化剂中,Zr–SBA-15-20在相对较低的温度(275°C)下达到了74.0%的最佳丁二烯选择性。良好的催化性能可以归因于Zr物种的均匀分散和Zr掺入产生的Zr–O–Si键。此外,
更新日期:2020-08-25
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