水热预处理Zn/HZSM-5催化剂对其催化乙烯芳构化反应性能的影响OA北大核心CSTPCD
The effect of hydrothermal pretreatment on the catalytic performance of Zn/HZSM-5 catalysts for ethylene aromatization reaction
针对用于低碳烯烃芳构化的Zn/HZSM-5 催化剂存在易于结焦失活的问题,采用高温水热的方法对催化剂进行预处理,通过XRD、N2 物理吸附-脱附、NH3-TPD、Py-FTIR、XPS和TG等技术对样品进行表征,并以乙烯芳构化为探针反应考察了高温水热预处理对催化剂反应性能和稳定性的影响.结果表明,Zn/HZSM-5 催化剂经高温水热预处理 48h后表现出优异的催化性能,虽然乙烯转化率略微降低,但是催化剂寿命显著延长,由 72h延长至 216 h,同时芳烃选择性保持在60%以上;水热处理促进了ZnO物种与B酸中心的相互作用及ZnOH+物种的生成,在抑制氢转移反应的同时显著促进了催化剂的脱氢性能,提高了氢气选择性;此外,水热处理后催化剂容碳量明显增加、积炭速率降低,表现出优异的抗结焦积炭特性.
To address the issue of coking and deactivation of Zn/HZSM-5 catalysts used for light olefins aromatization,a high-temperature hydrothermal method was employed for catalyst pretreatment.The catalysts were characterized using XRD,N2 physical adsorption-desorption,NH3-TPD,Py-FTIR,XPS and TG techniques.The effect of high-temperature hydrothermal pretreatment on the catalytic performance and stability of the catalyst was investigated using ethylene aromatization as a probe reaction.The results showed that the Zn/HZSM-5 catalyst exhibited excellent catalytic performance after 48 h of high-temperature hydrothermal pretreatment.Although the conversion of ethylene slightly decreased,the catalyst lifetime was significantly extended,increasing from 72 to 216 h,while the aromatics selectivity remained above 60%.It was suggested that the hydrothermal treatment enhanced the interaction between ZnO species and Brønsted acid sites,promoting the generation of ZnOH+species.This not only suppressed the hydrogen transfer reaction but also significantly enhanced the dehydrogenation performance of the catalyst,improving the selectivity towards hydrogen.Additionally,the catalyst exhibited increased carbon capacity and reduced carbon deposition rate after hydrothermal treatment,demonstrating excellent anti-coking properties.
邵嘉蓓;李柏超;董梅;樊卫斌;秦张峰;王建国
中国科学院山西煤炭化学研究所煤炭高效低碳利用国家重点实验室 山西太原 030001||中国科学院大学 北京 100049中国科学院山西煤炭化学研究所煤炭高效低碳利用国家重点实验室 山西太原 030001中国科学院大学 北京 100049
化学
Zn/HZSM-5水热预处理乙烯芳构化Zn物种
Zn/HZSM-5hydrothermal pretreatmentethylene aromatizationZn species
《燃料化学学报(中英文)》 2024 (008)
1079-1087 / 9
The project was supported by National Key R&D Program of China(2020YFB0606402),National Natural Science Foundation of China(22372189,22322208,U1910203).国家重点研发计划(2020YFB0606402)和国家自然科学基金(22372189,22322208,U1910203)资助
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