Pt3Mn/SiO2 + ZSM-5 Bifunctional Catalyst for Ethane Dehydroaromatization

IF 4.7 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2024-06-04 DOI:10.3390/catal14060365
Shan Jiang, Che-Wei Chang, William A Swann, Christina W. Li, Jeffrey T. Miller
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Abstract

Ethane dehydroaromatization (EDA) is a potentially attractive process for converting ethane to valuable aromatics such as benzene, toluene, and xylene (BTX). In this study, a Pt3Mn/SiO2 + ZSM-5 bifunctional catalyst was used to investigate the effect of dehydrogenation and the Brønsted acid catalyst ratio, hydrogen partial pressure, and reaction temperature on the product distributions for EDA. Pt3Mn/SiO2 + ZSM-5 with a 1/1 weight ratio showed the highest ethane conversion rate and BTX formation rate. Ethylene is initially formed by dehydrogenation by the Pt3Mn catalyst, which undergoes secondary reactions on ZSM-5, forming C3+ reaction intermediates. The latter form final products of CH4 and BTX. At conversions from 15 to 30%, the BTX selectivities are 82–90%. For all bifunctional catalysts, the ethane conversion significantly exceeds the ethane–ethylene equilibrium conversion due to reaction to secondary products. Low H2 partial pressures did not significantly alter the product selectivity or conversion. However, higher H2 partial pressures resulted in increased methane and decreased BTX selectivity. The excess hydrogen saturated the olefin intermediates to form alkanes, which produced methane by monomolecular cracking on ZSM-5. With an increasing reaction temperature from 550 °C to 650 °C, the benzene selectivity increased, while the highest BTX selectivity was obtained at 600 to 650 °C.
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用于乙烷脱氢芳构化的 Pt3Mn/SiO2 + ZSM-5 双功能催化剂
乙烷脱氢芳构化(EDA)是将乙烷转化为苯、甲苯和二甲苯(BTX)等有价值芳烃的一种具有潜在吸引力的工艺。本研究使用 Pt3Mn/SiO2 + ZSM-5 双功能催化剂研究了脱氢、布氏酸催化剂比例、氢分压和反应温度对 EDA 产物分布的影响。重量比为 1/1 的 Pt3Mn/SiO2 + ZSM-5 的乙烷转化率和 BTX 生成率最高。乙烯最初由 Pt3Mn 催化剂脱氢生成,在 ZSM-5 上发生二次反应,形成 C3+ 反应中间产物。后者形成 CH4 和 BTX 的最终产物。当转化率为 15% 至 30% 时,BTX 的选择性为 82%-90%。对于所有双官能催化剂,乙烷转化率都大大超过乙烷-乙烯平衡转化率,原因是反应生成了副产品。较低的 H2 分压不会显著改变产品选择性或转化率。然而,较高的氢气分压导致甲烷增加,BTX 选择性降低。过量的氢使烯烃中间体饱和,形成烷烃,在 ZSM-5 上通过单分子裂解产生甲烷。随着反应温度从 550 ℃ 升至 650 ℃,苯的选择性增加,而在 600 至 650 ℃ 时,BTX 的选择性最高。
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来源期刊
CiteScore
7.20
自引率
4.30%
发文量
567
期刊介绍: ACS Applied Electronic Materials is an interdisciplinary journal publishing original research covering all aspects of electronic materials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials science, engineering, optics, physics, and chemistry into important applications of electronic materials. Sample research topics that span the journal's scope are inorganic, organic, ionic and polymeric materials with properties that include conducting, semiconducting, superconducting, insulating, dielectric, magnetic, optoelectronic, piezoelectric, ferroelectric and thermoelectric. Indexed/​Abstracted: Web of Science SCIE Scopus CAS INSPEC Portico
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