物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2013年
6期
1281-1288
,共8页
张金贵%骞伟中*%汤效平%沈葵%王彤%黄晓凡%魏飞
張金貴%鶱偉中*%湯效平%瀋葵%王彤%黃曉凡%魏飛
장금귀%건위중*%탕효평%침규%왕동%황효범%위비
甲醇%ZSM-5分子筛%芳构化%脱烷基%烷基化%异构化
甲醇%ZSM-5分子篩%芳構化%脫烷基%烷基化%異構化
갑순%ZSM-5분자사%방구화%탈완기%완기화%이구화
Methanol%ZSM-5 zeolite%Aromatization%Dealkylation%Alkylation%Isomerization
在Zn/P/ZSM-5催化剂上研究了甲醇、二甲苯、甲苯和甲醇等不同进料下芳烃产品分布随反应积碳的变化,发现催化剂积碳对芳构化反应、脱烷基反应和烷基化反应的影响不同.在不同硅铝摩尔比(Si/Al比)和Zn负载量的Zn/P/ZSM-5催化剂上进行甲醇转化,考察催化剂酸性位点强度、密度和类型与芳烃收率和产品分布之间的关系,发现当强酸位点酸密度下降时,脱烷基反应最先被抑制,其次是芳构化反应和异构化反应,而烷基化反应却不受影响.在Si/Al比为14,3%(w) Zn负载量的Zn/P/ZSM-5催化剂上可得到75%左右的芳烃收率,二甲苯收率在35%左右,具有重要的工业应用前景.
在Zn/P/ZSM-5催化劑上研究瞭甲醇、二甲苯、甲苯和甲醇等不同進料下芳烴產品分佈隨反應積碳的變化,髮現催化劑積碳對芳構化反應、脫烷基反應和烷基化反應的影響不同.在不同硅鋁摩爾比(Si/Al比)和Zn負載量的Zn/P/ZSM-5催化劑上進行甲醇轉化,攷察催化劑痠性位點彊度、密度和類型與芳烴收率和產品分佈之間的關繫,髮現噹彊痠位點痠密度下降時,脫烷基反應最先被抑製,其次是芳構化反應和異構化反應,而烷基化反應卻不受影響.在Si/Al比為14,3%(w) Zn負載量的Zn/P/ZSM-5催化劑上可得到75%左右的芳烴收率,二甲苯收率在35%左右,具有重要的工業應用前景.
재Zn/P/ZSM-5최화제상연구료갑순、이갑분、갑분화갑순등불동진료하방경산품분포수반응적탄적변화,발현최화제적탄대방구화반응、탈완기반응화완기화반응적영향불동.재불동규려마이비(Si/Al비)화Zn부재량적Zn/P/ZSM-5최화제상진행갑순전화,고찰최화제산성위점강도、밀도화류형여방경수솔화산품분포지간적관계,발현당강산위점산밀도하강시,탈완기반응최선피억제,기차시방구화반응화이구화반응,이완기화반응각불수영향.재Si/Al비위14,3%(w) Zn부재량적Zn/P/ZSM-5최화제상가득도75%좌우적방경수솔,이갑분수솔재35%좌우,구유중요적공업응용전경.
@@@@Relationship between aromatics distribution, in the process of methanol to aromatics (MTA), and the conversion of methanol and the catalyst acidity was investigated over a series of Zn/P/ZSM-5 catalysts with different Si/Al molar ratios and zinc loading. To understand the contribution of aromatization, isomerization, dealkylation and alkylation reactivity of the catalyst to the aromatics distribution, coke deposition degree of Zn/P/ZSM-5 catalyst was tailored as using different feedstocks including methanol, xylene or the mixture of methanol and toluene. With the coke deposition, the amount of different types of acidic sites of catalyst varied significantly, characterized by NH3-temperature programmed desorption (NH3-TPD) and pyridine-infrared methods. Aromatization, dealkylation, alkylation, and isomerization showed sensitivity to a reduction in the density of strongly acidic sites. Dealkylation reaction was preferential y inhibited just by slightly decreasing the density of strong acid sites. However, aromatization and isomerization reaction were inhibited only when the density of strong acid sites was significantly decreased. In al cases, alkylation was found to be uninfluenced by acidic site density. A Zn/P/ZSM-5 catalyst with Si/Al molar ratio of 14 and 3% (w) Zn loading exhibited aromatics yields of 75% and xylene yields of about 35%, indicating potential for industrial application.