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Highly active ternary oxide ZrCeZnOx combined with SAPO-34 zeolite for direct conversion of syngas into light olefins
Catalysis Today ( IF 5.2 ) Pub Date : 2020-03-17 , DOI: 10.1016/j.cattod.2020.03.023
Fanhui Meng , Xiaojing Li , Peng Zhang , Langlang Yang , Guinan Yang , Pengchuan Ma , Zhong Li

Direct conversion of syngas into light olefins over bifunctional catalysts (metal oxide and zeolite) has attracted great attention in recent years. For this reaction, the adsorption and activation of CO and H2 occur on metal oxide surface, thus the design of metal oxide is crucial. In this study, ternary oxides ZrCeZnOx with various CeO2 contents were prepared by parallel coprecipitation method, and SAPO-34 zeolite (Si/Al = 0.125) was hydrothermally synthesized. The metal oxides were characterized by XRD, BET, TEM, SEM, XPS, CO-TPD, H2-TPD, TGA and in-situ DRIFTS. The addition of CeO2 into Zr-Zn oxide shifted the diffraction peaks to lower values, and formed the Ce0.5Zr0.5O2 solid solution as the Zr/Ce/Zn atomic ratio reached 4/4/1. As the CeO2 content rose, the BET surface area increased while the metal oxide particle size decreased. Moreover, the addition of CeO2 greatly enhanced the concentration of oxygen vacancies and the adsorption ability of CO and H2. The in-situ DRIFTS confirmed that CH3O* was the intermediate. By optimizing the reaction conditions, ZrCeZnOx/SAPO-34 catalyst exhibited high CO conversion of 25.6 % and light olefins selectivity of 78.6 %. This study will contribute to the design of metal oxide for bifunctional catalyst for light olefins synthesis.



中文翻译:

高活性三元氧化物ZrCeZnO x与SAPO-34沸石结合使用,可将合成气直接转化为轻质烯烃

近年来,通过双功能催化剂(金属氧化物和沸石)将合成气直接转化为轻质烯烃备受关注。对于该反应,CO和H 2的吸附和活化发生在金属氧化物表面上,因此金属氧化物的设计至关重要。在这项研究中,通过平行共沉淀法制备了具有各种CeO 2含量的三元氧化物ZrCeZnO x,并水热合成了SAPO-34沸石(Si / Al = 0.125)。通过XRD,BET,TEM,SEM,XPS,CO-TPD,H 2 -TPD,TGA和原位DRIFTS对金属氧化物进行表征。在Zr-Zn氧化物中添加CeO 2可使衍射峰移至较低值,并形成Ce 0.5的Zr 0.5 ø 2固溶体作Zr / CE /锌的原子比达到4/4/1。随着CeO 2含量的增加,BET表面积增加,而金属氧化物的粒径减小。此外,CeO 2的添加大大提高了氧空位的浓度以及CO和H 2的吸附能力。在原位DRIFTS确认CH 3的O *是中间。通过优化反应条件,ZrCeZnO x / SAPO-34催化剂显示出25.6%的高CO转化率和78.6%的轻烯烃选择性。这项研究将有助于轻烯烃合成双功能催化剂的金属氧化物的设计。

更新日期:2020-03-17
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