Ammonium Hexafluorosilicate (AHFS) Modified HMCM‐22 As Efficient Catalysts for Alkylation of Phenol with Methanol
Ammonium Hexafluorosilicate (AHFS) Modified HMCM‐22 As Efficient Catalysts for Alkylation of Phenol with Methanol
复制标题
六氟硅酸铵 (AHFS) 改性 HMCM–22 作为苯酚与甲醇烷基化的高效催化剂
DOI：
10.1002/slct.202202974
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发表时间：
2022-12
期刊：
影响因子：
--
通讯作者：
Xue Bing
中科院分区：
文献类型：
--
作者：
Liu Zonghui;Xie Dehua;Ran jianzhou;Wu Jing;Liu Na;Xue Bing
制备了一系列xahfs /HMCM‐22 （x表示AHFS在HMCM‐22上的处理量，AHFS是六氟硅酸铵的缩写），并对苯酚与甲醇烷基化催化合成对甲酚进行了评价。采用n2吸附-解吸、XRD、FT - IR、27Al - MAS NMR、吡啶- IR和NH3 - TPD等表征技术分析了xahfs /HMCM - 22催化剂的理化性质。苯酚的转化率随着xahfs /HMCM‐22催化剂用量的增加而降低；而对甲酚的选择性在x=0.07时达到最大。结果表明，0.07AHFS/HMCM‐22催化剂在325℃，WHSV=2 h−1的条件下，对甲酚的选择性在24 h以上，达到53.3%，远高于HMCM‐22催化剂的37.1%。该催化剂的高甲酚选择性是由于AHFS去除了HMCM - 22外表面的部分酸位，并将酸位保留在沸石的微孔中。相反，催化剂活性的降低是由于总酸位的减少。
A series ofxAHFS/HMCM‐22 (xdenotes the amount of AHFS treatment on HMCM‐22, AHFS is the abbreviation for ammonium hexafluorosilicate) were prepared and evaluated in the catalytic synthesis ofp‐cresol by alkylation of phenol with methanol. Several characterization techniques including N2adsorption‐desorption, XRD, FT‐IR,27Al MAS NMR, Pyridine‐IR, and NH3‐TPD have been used to analyze the physicochemical properties of thexAHFS/HMCM‐22 catalyst. The conversion of phenol decreased with increasingxofxAHFS/HMCM‐22 catalyst; while the selectivity forp‐cresol maximized at x=0.07. The 0.07AHFS/HMCM‐22 catalyst was identified as the most efficient catalyst, showing the highestp‐cresol selectivity (53.3 %) for longer than 24 h under optimized reaction conditions (325 °C, WHSV=2 h−1), which is much higher than that of parent HMCM‐22 catalyst (37.1 %). The highp‐cresol selectivity of the catalyst is attributed to AHFS removing part of the acid sites on the external surface of the HMCM‐22, and preserving the acid sites in the micropores of zeolite. By contrast, the decrease in catalyst activity is due to the decrease in total acid sites.
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