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Methanol steam reforming over Ni-CeO2 model and powder catalysts: Pathways to high stability and selectivity for H2/CO2 production
Catalysis Today ( IF 5.3 ) Pub Date : 2017-08-25 , DOI: 10.1016/j.cattod.2017.08.041
Zongyuan Liu , Siyu Yao , Aaron Johnston-Peck , Wenqian Xu , José A. Rodriguez , Sanjaya D. Senanayake

Nickel-ceria has been reported as a very good catalysts for the reforming of methane. Here, the methanol steam reforming reaction on both powder (Ni-CeO2) and model (Ni-CeO2-x(111)) catalysts was investigated. The active phase evolution and surface species transformation on powder catalysts were studied via in situ X-ray diffraction (XRD) and diffuse reflectance infrared transform spectroscopy (DRIFTS). Phase transitions of NiO → NiC → Ni and CeO2 → CeO2-x were observed during the reaction. The simultaneous production of H2/CO2 demonstrates that the active phase of the catalysts contains metallic Ni supported over partially reduced ceria. The DRIFTS experiments indicate that a methoxy to formate transition is associated with the reduction of ceria whereas the formation of carbonate species results from the presence of metallic Ni. A study of the reaction of methanol with Ni-CeO2-x(111) by X-ray photoelectron spectroscopy (XPS) points to the essential role of metal-support interactions in an oxygen transfer from ceria to Ni that contributes to the high selectivity of the catalysts.



中文翻译:

甲醇水蒸汽重整在Ni-的CeO 2模型和粉末催化剂:通往高稳定性和选择性用于h 2 / CO 2的生产

据报道,二氧化铈是甲烷重整的非常好的催化剂。在此,研究了在粉末(Ni-CeO 2)和模型(Ni-CeO 2-x(111))催化剂上的甲醇蒸汽重整反应。通过原位X射线衍射(XRD)和漫反射红外光谱(DRIFTS)研究了粉末催化剂上的活性相演化和表面物种转化。反应期间观察到NiO→NiC→Ni和CeO 2  →CeO 2-x的相变。同时生产H 2 / CO 2证明了催化剂的活性相含有负载在部分还原的二氧化铈上的金属Ni。DRIFTS实验表明,甲氧基到甲酸的过渡与二氧化铈的还原有关,而碳酸盐物种的形成是由于金属镍的存在而引起的。X射线光电子能谱(XPS)对甲醇与Ni-CeO 2-x(111)反应的研究表明,金属-载体相互作用在二氧化铈向Ni的氧转移中起着重要的作用,这有助于高选择性的催化剂。

更新日期:2017-08-25
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