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Diethyl Ether Conversion to Ethene and Ethanol Catalyzed by Heteropoly Acids
ACS Omega ( IF 3.7 ) Pub Date : 2021-03-23 , DOI: 10.1021/acsomega.1c00958 Rawan Al-Faze 1, 2 , Elena F. Kozhevnikova 1 , Ivan V. Kozhevnikov 1
ACS Omega ( IF 3.7 ) Pub Date : 2021-03-23 , DOI: 10.1021/acsomega.1c00958 Rawan Al-Faze 1, 2 , Elena F. Kozhevnikova 1 , Ivan V. Kozhevnikov 1
Affiliation
The conversion of diethyl ether (DEE) to ethene and ethanol was studied at a gas–solid interface over bulk and supported Brønsted solid acid catalysts based on tungsten Keggin heteropoly acids (HPAs) at 130–250 °C and ambient pressure. The yield of ethene increased with increasing reaction temperature and reached 98% at 220–250 °C (WHSV = 2.2 h–1). The most active HPA catalysts were silica-supported H3PW12O40 and H4SiW12O40 and the bulk heteropoly salt Cs2.5H0.5PW12O40. The HPA catalysts outperformed zeolites HZSM-5 and USY reported elsewhere. A correlation between catalyst activity and catalyst acid strength was established, which indicates that Brønsted acid sites play an important role in DEE elimination over HPA catalysts. The results point to the reaction occurring through the consecutive reaction pathway: DEE → C2H4 + EtOH followed by EtOH → C2H4 + H2O, where ethene is both a primary product of DEE elimination and a secondary product via dehydration of the primary product EtOH. Evidence is provided that DEE elimination over bulk HPA and high-loaded HPA/SiO2 catalysts proceeds via the surface-type mechanism.
中文翻译:
杂多酸催化二乙基醚转化为乙烯和乙醇
在130-250°C和环境压力下,在基于气态Keggin杂多酸(HPA)的块状和负载Brønsted固体酸催化剂的气-固界面上研究了乙醚(DEE)向乙烯和乙醇的转化。乙烯的产率随反应温度的升高而增加,在220–250°C(WHSV = 2.2 h –1)时达到98%。最具活性的HPA催化剂是二氧化硅负载的H 3 PW 12 O 40和H 4 SiW 12 O 40以及本体杂多盐Cs 2。5 H 0。5 PW 12 O 40。HPA催化剂的性能优于HZSM-5和USY沸石。建立了催化剂活性与催化剂酸强度之间的相关性,这表明布朗斯台德酸位点在消除HPE催化剂的DEE中起着重要作用。结果表明反应是通过以下连续反应路径发生的:DEE→C 2 H 4 + EtOH,然后是EtOH→C 2 H 4 + H 2 O,其中乙烯既是DEE消除的主要产物,又是脱水产生的次级产物。初级产品EtOH的含量。有证据表明,通过表面型机理消除了大体积HPA和高负载HPA / SiO 2催化剂上的DEE 。
更新日期:2021-04-06
中文翻译:
杂多酸催化二乙基醚转化为乙烯和乙醇
在130-250°C和环境压力下,在基于气态Keggin杂多酸(HPA)的块状和负载Brønsted固体酸催化剂的气-固界面上研究了乙醚(DEE)向乙烯和乙醇的转化。乙烯的产率随反应温度的升高而增加,在220–250°C(WHSV = 2.2 h –1)时达到98%。最具活性的HPA催化剂是二氧化硅负载的H 3 PW 12 O 40和H 4 SiW 12 O 40以及本体杂多盐Cs 2。5 H 0。5 PW 12 O 40。HPA催化剂的性能优于HZSM-5和USY沸石。建立了催化剂活性与催化剂酸强度之间的相关性,这表明布朗斯台德酸位点在消除HPE催化剂的DEE中起着重要作用。结果表明反应是通过以下连续反应路径发生的:DEE→C 2 H 4 + EtOH,然后是EtOH→C 2 H 4 + H 2 O,其中乙烯既是DEE消除的主要产物,又是脱水产生的次级产物。初级产品EtOH的含量。有证据表明,通过表面型机理消除了大体积HPA和高负载HPA / SiO 2催化剂上的DEE 。