CO2-assisted oxidative dehydrogenation of ethane to ethylene over the ZnO-ZrO2 catalyst

Q3 Energy 燃料化学学报 Pub Date : 2023-10-01 DOI:10.1016/S1872-5813(23)60360-3
Duo-hua LIAO, Liang YANG, Geng-zhe SONG, Xue-dong MA, Shuang LI
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Abstract

The ZnO-ZrO2 catalyst was prepared by the deposition-precipitation method using ZrO2 as the carrier obtained from calcining commercial zirconium hydroxide (Zr(OH)4). And the catalytic performance was evaluated at 873 K in CO2-assisted ethane oxidative dehydrogenation reaction (CO2-ODHE). The physical-chemical properties and morphology were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), Raman spectra, High-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectra (XPS), CO2 temperature-programmed desorption (CO2-TPD). The results show that ZnO were doped into the surface lattice of ZrO2 on the 5%ZnO-ZrO2 catalyst, generating highly dispersed ZnO species and oxygen-deficient regions on catalyst surface. 5%ZnO-ZrO2 catalyst could selectively breaking C–H bond instead of C–C bond, delivering excellent catalytic performance. 210 μmol/(gcat·min) of C2H4 formation rate could compare favorably with the data reported on noble metal and transition metal carbides. Additionally, the possible mechanism is discussed.

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ZnO-ZrO2催化剂催化乙烷氧化脱氢制乙烯
ZnO-ZrO2催化剂通过沉积沉淀法制备,使用从煅烧商业氢氧化锆(Zr(OH)4)获得的ZrO2作为载体。并在873K下对CO2辅助乙烷氧化脱氢反应(CO2-ODHE)的催化性能进行了评价。通过X射线衍射(XRD)、扫描电子显微镜(SEM)、拉曼光谱、高分辨率透射电子显微镜(HRTEM)、X射线光电子能谱(XPS)、CO2程序升温脱附(CO2-TPD)对其理化性质和形貌进行了表征。结果表明,在5%ZnO-ZrO2催化剂上,ZnO掺杂到ZrO2的表面晶格中,在催化剂表面产生高度分散的ZnO物种和缺氧区域。5%ZnO-ZrO2催化剂可以选择性地破坏C–H键而不是C–C键,具有优异的催化性能。210μmol/(gcat·min)的C2H4生成速率可以与贵金属和过渡金属碳化物的数据相比较。此外,还讨论了可能的机制。
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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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