Monometallic and bimetallic catalysts based on Pd, Cu and Ni for hydrogen transfer deoxygenation of a prototypical fatty acid to diesel range hydrocarbons
Monometallic and bimetallic catalysts based on Pd, Cu and Ni for hydrogen transfer deoxygenation of a prototypical fatty acid to diesel range hydrocarbons
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DOI：
10.1016/j.cattod.2019.03.017
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发表时间：
2020-09-15
期刊：
影响因子：
5.3
通讯作者：
Kyriakou, Georgios
中科院分区：
文献类型：
--
作者：
Cheah, Kin Wai;Taylor, Martin J.;Kyriakou, Georgios
通过一种简单、廉价和商业上相关的方法合成了负载在活性炭上的宽组成范围的双金属PdxNi（100-x）和PdxCu（100-x）结构。通过STEM-EDS、TEM、XPS、粉末XRD、N2孔率仪和ICP-OES等测试手段，研究了纳米结构及其单晶对应物的表面和体相性质。单个金属颗粒的XRD图案和EDS元素组成映射之间的密切相关性建立了每个样品中钯-基金属相互作用的程度。以四氢萘为供氢体，考察了不同结构的催化剂对油酸选择性加氢和加氢脱氧反应的催化性能。发现与观察到组成偏析的催化剂相比，显示出真正的氢化物/合金形成的催化剂提高了四氢化萘的转化率。发现PdxNi（100-x）系列在通过四氢萘脱氢的氢生产方面优于PdxCu（100-x）催化剂，反映了PdxCu（100-x）系列比PdxNi（100-x）发生更多的组成偏析的事实。发现油酸在monoclonal和monoclonal催化剂上的氢转移脱氧反映了氢的可用性，这些催化剂释放更多的氢也有利于C-17和C-18烷烃的形成。
Bimetallic PdxNi(100-x) and PdxCu(100-x) structures of a wide compositional range supported on activated carbon were synthesised via a simple, cheap and commercially relevant method. The surface and bulk properties of both the bimetallic structures and their monometallic counterparts were determined via STEM-EDS, TEM, XPS, powder XRD, N-2 porosimetry and ICP-OES. A close correlation between the XRD patterns and EDS elemental composition mapping of individual metal particles established the extent of palladium-base metal interaction in each sample. The performance of the different structures as catalysts for the selective hydrogenation and hydrodeoxygenation of oleic acid, a prototypical fatty acid, was evaluated using tetralin as a hydrogen donor. Catalysts displaying true bimetallic/alloy formation were found to improve the conversion of tetralin as compared to catalysts in which compositional segregation was observed. The PdxNi(100-x) series was found to outperform the PdxCu(100-x) catalysts in terms of hydrogen production via the dehydrogenation of tetralin, mirroring the fact that compositional segregation occurs more for the PdxCu(100-x) series than PdxNi(100-x). The hydrogen transfer deoxygenation of oleic acid over the monometallic and bimetallic catalysts was found to mirror the availability of hydrogen with those catalysts liberating more hydrogen also favouring the formation of C-17 and C-18 alkanes.