Ternary Cobalt–Copper–Niobium Catalysts for the Selective CO Hydrogenation to Higher Alcohols

Ternary Cobalt–Copper–Niobium Catalysts for the Selective CO Hydrogenation to Higher Alcohols
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三元钴-铜-铌催化剂用于 CO 选择性加氢生成高级醇

DOI:
10.1021/acscatal.5b00388
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发表时间:
2015
期刊:
影响因子:
12.9
通讯作者:
Kruse, Norbert
Kruse, Norbert
中科院分区:
化学1区
文献类型:
--
作者:
Xiang, Yizhi;Barbosa, Roland;Li, Xiaonian;Kruse, Norbert

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设计了具有双峰纳米颗粒结构的新型“CoCuNb”三元催化剂,在没有通用载体材料的情况下,并成功地在CO加氢制备高级醇中进行了测试。优化后的C2-C5体系对伯醇的选择性通常超过50 wt %,CO转化率在15%~ 20%之间时,对1-醇/1-烯烃的综合选择性可达173 wt %.通过草酸盐共沉淀实现的双峰纳米尺寸的颗粒分布,含有尺寸范围为25至40 nm的Co-Cu颗粒。在4和8 nm之间的较小颗粒被鉴定为Nb氧化物,并且起到结构分散剂(“间隔物”)和1-醇/1-烯烃生产的促进剂的作用。X-射线光电子能谱显示NbOxto含有大量的4+氧化态的Nb物种。
Novel “CoCuNb” ternary catalysts with bimodal nanosized particle structure, in the absence of a generic support material, were designed and successfully tested in higher alcohol production via CO hydrogenation. The selectivities to primary alcohols with an optimized C2–C5slate usually exceeded the 50 wt % level, and the combined selectivities to 1-alcohols/1-alkenes reached up to ∼73 wt % for CO conversions ranging between ∼5% and nearly 20%. The bimodal nanosized particle distribution, achieved through oxalate coprecipitation, contained Co–Cu particles with sizes ranging from 25 to 40 nm. Smaller particles between 4 and 8 nm were identified as Nb oxides and played the role of a structural dispersant (“spacer”) and promoter of 1-alcohol/1-olefin production. X-ray photoelectron spectroscopy revealed NbOxto contain major amounts of species with Nb in the 4+ oxidation state.