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首页> 外文期刊>Catalysis science & technology >Carbon nanofibres-supported KCoMo catalysts for syngas conversion into higher alcohols
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Carbon nanofibres-supported KCoMo catalysts for syngas conversion into higher alcohols

机译：碳nanofibres-supported KCoMo催化剂合成气转化为更高的醇

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摘要

The development of industrially-viable heterogeneous catalysts for higher alcohol (HA) synthesis via direct syngas conversion is hindered by the limited understanding of structural and electronic descriptors of their performance. Here, K-promoted CoMo(5 wt%)-based catalysts were investigated to shed light onto property- function relations. Evaluation of impregnated oxides and C-based materials identified a higher HA selectivity for the catalyst supported on carbon nanofibres obtained by the simultaneous addition of all metals. Using this carrier, additional solids were synthesised via ball milling as well as a sol-gel method with citric acid, which enhanced the CO conversion. After confirming the positive influence of K and a unitary Co/Mo ratio, the impact of temperature (573-773 K) and pressure (0.1-5 MPa) upon activation through reduction by hydrogen was investigated. A combination of two steps, one at 723 K and ambient pressure, fostering the HA selectivity (22%), and a second, more extended, at 573 K and 5 MPa, boosting the CO conversion (14%), maximised the space time yield of HA, which matches that of the best comparable CoMo system reported in the literature (ca. 0.12 gHA g(cat)(-1) h(-1)) in spite of the 13-times lower metal loading. Characterisation by X-ray diffraction, temperature-programmed reduction by H-2, X-ray photoelectron spectroscopy, operando infrared spectroscopy and electron microscopy uncovered that this originated from the atomic intermixing of Co and Mo in binary oxide phases and their high dispersion, enabling proximity and an effective reduction to low oxidation states of the metal sites (0 and + 2 for Mo and 0 for Co) upon activation and reaction.
机译：industrially-viable的发展异构催化剂更高的酒精(HA)通过直接合成合成气转换阻碍了有限的理解结构和电子的描述符的性能。催化剂进行了解释到属性函数关系。浸渍氧化物和基于c的材料确定了HA的选择性高催化剂支持碳纳米纤维同时添加所有金属。这个载体,合成更多的固体通过球磨以及溶胶-凝胶法柠檬酸、增强公司的转换。确认后K和积极的影响统一的公司/ Mo比,温度的影响(573 - 773 K)和压力(0.1 - 5 MPa)激活通过氢还原调查。723 K和环境压力,促进HA选择性(22%),其次,更多的扩展,在573 K和5 MPa,促进公司转换(14%),最大化的时空产生哈,匹配的可比科莫最好系统在文献中报道(gHA ca。0.12h g(猫)(1)(1)尽管低13倍金属加载。衍射,程序升温还原2、x射线光电子能谱、operando红外光谱和电子显微镜发现,这起源于原子混合的Co和莫二元氧化物阶段和高色散,使邻近一个有效的降低低氧化态的金属网站为密苏里州和0 (0,+ 2 Co)在激活和反应。

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