K改性NiMoS/ZnAl氧化物负载型催化剂合成气制低碳醇性能研究OACSTPCD
K-modified NiMoS/ZnAl oxide catalysts for higher alcohols synthesis from syngas
采用共沉淀法和浸渍法,以ZnAl混合金属氧化物为载体,制备了系列不同K/Mo物质的量比的高分散K改性NiMoS/ZnAl催化剂,并对其合成气转化制低碳醇性能进行了研究.结果表明,K的引入可以调变MoS2片层的堆积程度和尺寸,提高NiSx 和NiMoS之间的协同作用,促进低碳醇合成(HAS)过程中CHx 的插入和非解离CO的插入能力,有效抑制烃类和CO2的生成.其中,K/Mo物质的量比为0.6的KNiMoS/ZnAl催化剂具有最多的双层MoS2结构(33.7%)和适宜的NiS,与NiMoS协同作用,产物中总醇选择性达到69.8%,低碳醇空时产率为78.6 mg/(g·h).
Improving the C2+alcohols yield is highly desirable for the direct synthesis of higher alcohols from syngas.In this work,a series of highly dispersed K-modified NiMoS catalysts with different K contents on ZnAl-mixed oxide support were prepared by the combination of co-precipitation and impregnation method.And their performance in higher alcohols synthesis(HAS)from syngas was investigated.The results show that the introduction of K can modulate the stacking degree of MoS2 slabs,and improve the interaction between NiSx and NiMoS phases.The as-prepared catalyst is conducive to promote the insertion of CHx and non-dissociative CO in HAS,and effectively suppress the generation of hydrocarbons and CO2.The 0.6KNiMoS/ZnAl catalyst exhibits the most double-layer MoS2 slabs(33.7%)and highly synergetic effects between NiSx and NiMoS to achieve the total alcohols selectivity(69.8%)and space-time yield(78.6 mg/(g·h))of C2+alcohols.
曹轶华;张鑫;阴雪利;甘永豪;代小平
中国石油大学(北京)化学工程与环境学院 重质油国家重点实验室,北京 102249
化学
NiMoS/ZnAl催化剂K改性合成气低碳醇协同效应
NiMoS/ZnAl catalystsK modificationsynthesis gashigher alcoholssynergetic effect
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The project was supported by the National Natural Science Foundation of China(21576288).国家自然科学基金(21576288)资助
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