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深入了解活性双金属Ni(Co)/Al₂O₃干重整催化剂上的双金属效应和积炭物种。

An in-depth understanding of the bimetallic effects and coked carbon species on an active bimetallic Ni(Co)/Al2O3 dry reforming catalyst.

作者信息

Liao Xin, Gerdts Rihards, Parker Stewart F, Chi Lina, Zhao Yongxiang, Hill Martyn, Guo Junqiu, Jones Martin O, Jiang Zheng

机构信息

Faculty of Engineering and the Environment, University of Southampton, Highfield, Southampton, SO17 1BJ, UK.

ISIS Facility, STFC Rutherford Appleton Laboratory, Chilton, Didcot, OX11 0QX, UK.

出版信息

Phys Chem Chem Phys. 2016 Jun 29;18(26):17311-9. doi: 10.1039/c6cp01089j.

Abstract

Ni/Al2O3, Co/Al2O3 and bimetallic Ni(Co)/Al2O3 catalysts were prepared using an impregnation method and employed in CO2 dry reforming of methane under coking-favored conditions. The spent catalysts were carefully characterized using typical characterization technologies and inelastic neutron scattering spectroscopy. The bimetallic catalyst exhibited a superior activity and anti-coking performance compared to Ni/Al2O3, while the most resistant to coking behavior was Co/Al2O3. The enhanced activity of the Ni(Co)/Al2O3 bimetallic catalyst is attributed to the reduced particle size of metallic species and resistance to forming stable filamentous carbon. The overall carbon deposition on the spent bimetallic catalyst is comparable to that of the spent Ni/Al2O3 catalyst, whereas the carbon deposited on the bimetallic catalyst is mainly less-stable carbonaceous species as confirmed by SEM, TPO, Raman and INS characterization. This study provides an in depth understanding of alloy effects in catalysts, the chemical nature of coked carbon on spent Ni-based catalysts and, hopefully, inspires the creative design of a new bimetallic catalyst for dry reforming reactions.

摘要

采用浸渍法制备了Ni/Al2O3、Co/Al2O3和双金属Ni(Co)/Al2O3催化剂,并将其用于有利于结焦条件下的甲烷二氧化碳干重整反应。使用典型的表征技术和非弹性中子散射光谱对失活催化剂进行了仔细表征。与Ni/Al2O3相比,双金属催化剂表现出优异的活性和抗结焦性能,而最耐结焦的是Co/Al2O3。Ni(Co)/Al2O3双金属催化剂活性的提高归因于金属物种粒径的减小以及对形成稳定丝状碳的抗性。失活双金属催化剂上的总积碳量与失活Ni/Al2O3催化剂相当,而通过扫描电子显微镜(SEM)、程序升温氧化(TPO)、拉曼光谱和非弹性中子散射(INS)表征证实,沉积在双金属催化剂上的碳主要是稳定性较差的含碳物种。本研究深入了解了催化剂中的合金效应、失活镍基催化剂上积碳的化学性质,并有望激发用于干重整反应的新型双金属催化剂的创新设计。

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