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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >Tuning Ni-catalyzed CO2 hydrogenation selectivity via Ni-ceria support interactions and Ni-Fe bimetallic formation
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Tuning Ni-catalyzed CO2 hydrogenation selectivity via Ni-ceria support interactions and Ni-Fe bimetallic formation

机译：通过Ni-Ceria支持相互作用和Ni-Fe Bimetallic形成调节Ni催化的CO 2氢化选择性

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摘要

CO2 hydrogenation over Fe-modified Ni/CeO2 catalysts was investigated in a batch reactor using time-resolved in situ FTIR spectroscopy. Low loading of Ni/CeO2 was associated with high selectivity to CO over CH4, while higher Ni loading improved CO2 hydrogenation activity with a reduced CO selectivity. X-ray absorption near edge structure (XANES) analysis revealed Ni to be metallic for all catalysts including the CO-selective low loading 0.5% Ni catalyst, suggesting that the selectivity trend is due to structural rather than oxidation state effects. The loading amount of 1.5% Ni was selected for co-impregnation with Fe, based on the significant shift in product selectivity towards CH4 for that loading amount, in order to shift the selectivity towards CO while maintaining high activity. Temperature programmed reduction (TPR) results indicated bimetallic interactions between Ni and Fe, and XANES analysis showed that about 70% of Fe in the bimetallic catalysts was oxidized. The Ni-Fe catalysts demonstrated improved selectivity towards CO without significantly compromising activity, coupling the high activity of Ni catalysts and the high CO selectivity of Fe. The general trends in Ni loading and bimetallic modification should guide efforts to develop non-precious metal catalysts for the selective production of CO by CO2 hydrogenation.
机译：使用时间分离的原位FTIR光谱研究在分批反应器中研究了Fe改性的Ni / CeO 2催化剂的CO 2氢化。 Ni / CeO 2的低负载与CO 4的高选择性相关，而具有降低的CO选择性的较高Ni加载改善的CO 2氢化活性。边缘结构（XANES）分析附近的X射线吸收显示所有催化剂的Ni是金属，包括共选择低负荷0.5％Ni催化剂，表明选择性趋势是由于结构而不是氧化状态效应。根据产品选择性的显着转变，选择加载1.5％Ni的加载量为1.5％的CH4的加载量，以便在保持高活性的同时改变CO的选择性。温度编程减少（TPR）结果表明Ni和Fe之间的双金属相互作用，Xanes分析显示，约70％的二氧化硅催化剂中的Fe氧化。 Ni-Fe催化剂对CO的选择性改善了无显着损害活性的，偶联Ni催化剂的高活性和Fe的高Co选择性。 Ni负荷和双金属改性的一般趋势应指导开发非贵金属催化剂，用于通过CO 2氢化选择性生产CO。

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