{"title":"甲苯在不同硅浓度的HSAPO-5上的烷基化反应","authors":"T. Masukawa, T. Komatsu, T. Yashima","doi":"10.1016/S0144-2449(97)00116-4","DOIUrl":null,"url":null,"abstract":"<div><p>HSAPO-5 with various Si concentrations was used as a catalyst for the alkylation of toluene with methanol to investigate weak acid sites. On HSAPO-5 with Si/(Al + P + Si) ≦ 0.026, the conversion of toluene increased with time on stream for a certain period, whereas the conversion decreased monotonously on HSAPO-5 with higher Si concentrations. Pretreatment with methanol on HSAPO-5 with Si/(Al + P + Si) = 0.018 increased the initial conversion of toluene. From the measurement of the amount of coke deposited on HSAPO-5, it is suggested that during the initial stage of the reaction coke is mainly produced by the reaction of methanol by itself at the acid sites on the external surface of HSAPO-5 with low Si concentrations. A small amount of coke thus formed would gradually retard the further self-conversion of methanol into coke. Therefore, the fraction of methanol used for the alkylation could increase, resulting in the increase in toluene conversion. It is suggested that the acid sites on the external surface are stronger than those formed by the substitution of Si for P but are weaker than those formed in aluminosilicate regions existing in HSAPO-5 with high Si concentrations.</p></div>","PeriodicalId":23983,"journal":{"name":"Zeolites","volume":"19 5","pages":"Pages 429-433"},"PeriodicalIF":0.0000,"publicationDate":"1997-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00116-4","citationCount":"10","resultStr":"{\"title\":\"Alkylation of toluene on HSAPO-5 with various Si concentrations\",\"authors\":\"T. Masukawa, T. Komatsu, T. Yashima\",\"doi\":\"10.1016/S0144-2449(97)00116-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>HSAPO-5 with various Si concentrations was used as a catalyst for the alkylation of toluene with methanol to investigate weak acid sites. On HSAPO-5 with Si/(Al + P + Si) ≦ 0.026, the conversion of toluene increased with time on stream for a certain period, whereas the conversion decreased monotonously on HSAPO-5 with higher Si concentrations. Pretreatment with methanol on HSAPO-5 with Si/(Al + P + Si) = 0.018 increased the initial conversion of toluene. From the measurement of the amount of coke deposited on HSAPO-5, it is suggested that during the initial stage of the reaction coke is mainly produced by the reaction of methanol by itself at the acid sites on the external surface of HSAPO-5 with low Si concentrations. A small amount of coke thus formed would gradually retard the further self-conversion of methanol into coke. Therefore, the fraction of methanol used for the alkylation could increase, resulting in the increase in toluene conversion. It is suggested that the acid sites on the external surface are stronger than those formed by the substitution of Si for P but are weaker than those formed in aluminosilicate regions existing in HSAPO-5 with high Si concentrations.</p></div>\",\"PeriodicalId\":23983,\"journal\":{\"name\":\"Zeolites\",\"volume\":\"19 5\",\"pages\":\"Pages 429-433\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"1997-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1016/S0144-2449(97)00116-4\",\"citationCount\":\"10\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Zeolites\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0144244997001164\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Zeolites","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0144244997001164","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 10
摘要
以不同Si浓度的HSAPO-5为催化剂,对甲苯与甲醇的烷基化反应进行了弱酸位点的研究。在Si/(Al + P + Si)≦0.026的HSAPO-5上,甲苯的转化率在一定时间内随时间的增加而增加,而在Si浓度较高的HSAPO-5上,甲苯的转化率单调下降。在Si/(Al + P + Si) = 0.018的HSAPO-5上进行甲醇预处理,提高了甲苯的初始转化率。通过对HSAPO-5表面焦炭沉积量的测定,认为在反应初期,焦炭主要是由甲醇在低Si浓度HSAPO-5表面的酸位上自行反应生成的。这样形成的少量焦炭会逐渐阻碍甲醇进一步自转化为焦炭。因此,烷基化过程中甲醇用量的增加会导致甲苯转化率的增加。结果表明,外表面的酸性位点比Si取代P形成的酸性位点强,但比高Si浓度HSAPO-5中铝硅酸盐区形成的酸性位点弱。
Alkylation of toluene on HSAPO-5 with various Si concentrations
HSAPO-5 with various Si concentrations was used as a catalyst for the alkylation of toluene with methanol to investigate weak acid sites. On HSAPO-5 with Si/(Al + P + Si) ≦ 0.026, the conversion of toluene increased with time on stream for a certain period, whereas the conversion decreased monotonously on HSAPO-5 with higher Si concentrations. Pretreatment with methanol on HSAPO-5 with Si/(Al + P + Si) = 0.018 increased the initial conversion of toluene. From the measurement of the amount of coke deposited on HSAPO-5, it is suggested that during the initial stage of the reaction coke is mainly produced by the reaction of methanol by itself at the acid sites on the external surface of HSAPO-5 with low Si concentrations. A small amount of coke thus formed would gradually retard the further self-conversion of methanol into coke. Therefore, the fraction of methanol used for the alkylation could increase, resulting in the increase in toluene conversion. It is suggested that the acid sites on the external surface are stronger than those formed by the substitution of Si for P but are weaker than those formed in aluminosilicate regions existing in HSAPO-5 with high Si concentrations.