One-Step Ethanol Conversion for 1,3-Butadiene Synthesis over Two-Dimensional VMT-SiO2 Nanomesh Loaded with Magnesium and Copper Oxide

纳米网 乙醇 1,3-丁二烯 氧化物 材料科学 化学 无机化学 催化作用 冶金 有机化学 石墨烯 纳米技术
作者
Yaqi Qin,Kegong Fang,Wenbin Li,Hongfang Jiu
出处
期刊:Chemistry [MDPI AG]
卷期号:6 (3): 361-375
标识
DOI:10.3390/chemistry6030021
摘要

A two-dimensional porous silica nanomesh (VMT-SiO2) was used as a carrier to prepare MgO-CuO-based catalysts and tested for one-step ethanol conversion to 1,3-butadiene. The effects of catalyst composition and different calcination temperatures on the reaction performances of the catalysts were mainly investigated. Combining various characterization techniques, such as HRTEM, XRD, FT-IR, and TPD, it was found that the dispersion state of MgO and CuO on the catalyst surface was related to the calcination temperature, which further induced changes in the acid–base properties. A small number of acidic centers and a proper proportion of medium–strong alkaline centers maintained a subtle balance, affecting catalytic performance. A lower total acid/base ratio is more conducive to ethanol conversion and 1,3-butadiene formation. At the same time, the synergistic effect of CuO and MgO promotes the transformation of the intermediate acetaldehyde product, which is the key to ensuring the subsequent aldol condensation and then 1,3-butadiene formation. Among the investigated samples, the CuO/MgO-VMT-SiO2 catalyst calcined at 500 °C exhibited the best catalytic performance, with an impressive ethanol conversion of 47.8% and 1,3-butadiene formation (42.6% selectivity and a space-time yield of 182.0 gC4H6·kgcat−1·h−1).
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