Zeng Liying, Liu Fei, Zhao Tianxiang, Cao Jianxin
School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou 550025, P. R. China.
Key Laboratory of Green Chemical and Clean Energy Technology, Guizhou University, Guiyang, Guizhou 550025, P. R. China.
ACS Omega. 2021 Jul 18;6(29):19067-19075. doi: 10.1021/acsomega.1c02369. eCollection 2021 Jul 27.
This paper proposes a ZSM-5@γ-AlO composite with a core-shell structure for the high-efficiency cocatalytic conversion of a methanol-ethanol system to light olefins. Using ZSM-5 and γ-AlO as sole catalysts for comparison, the effects of physical blending, impregnation, and liquid-phase precipitation coating strategies on the catalytic performance and physicochemical properties of the composite catalysts were systematically investigated. The results indicated that the ZSM-5@γ-AlO composite catalyst prepared by a liquid-phase precipitation coating exhibited excellent catalytic performance. When the ethanol content was 25 wt % and the reaction occurred at 350 °C, the conversion rates of methanol and ethanol were 96.1 and 99.9%, respectively; the selectivity and yield of light olefins reached 92.3 and 89.9%, respectively. The introduction of ethanol into methanol enhanced the selectivity of light olefins as target products. The interfacial composite phase formed by in situ nucleation growth of pseudoboehmite produced distinct Brønsted-Lewis acid synergistic active centers. It also increased the mesopore/micropore ratio in the composite catalyst.
本文提出了一种具有核壳结构的ZSM-5@γ-AlO复合材料,用于甲醇-乙醇体系高效共催化转化为轻质烯烃。以ZSM-5和γ-AlO作为单独的催化剂进行比较,系统研究了物理混合、浸渍和液相沉淀包覆策略对复合催化剂催化性能和物理化学性质的影响。结果表明,通过液相沉淀包覆制备的ZSM-5@γ-AlO复合催化剂表现出优异的催化性能。当乙醇含量为25 wt%且反应在350℃进行时,甲醇和乙醇的转化率分别为96.1%和99.9%;轻质烯烃的选择性和产率分别达到92.3%和89.9%。将乙醇引入甲醇中提高了作为目标产物的轻质烯烃的选择性。由拟薄水铝石原位成核生长形成的界面复合相产生了独特的布朗斯特-路易斯酸协同活性中心。它还增加了复合催化剂中的中孔/微孔比。