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Selective Hydrogenation of Dimethyl Terephthalate to 1,4-Cyclohexane Dicarboxylate by Highly Dispersed Bimetallic Ru–Re/AC Catalysts
Journal of Nanoscience and Nanotechnology Pub Date : 2020-02-01 , DOI: 10.1166/jnn.2020.16965 Enhui Qu 1 , Jingjie Luo 1 , Xin Di 2 , Chuang Li 2 , Changhai Liang 1
Journal of Nanoscience and Nanotechnology Pub Date : 2020-02-01 , DOI: 10.1166/jnn.2020.16965 Enhui Qu 1 , Jingjie Luo 1 , Xin Di 2 , Chuang Li 2 , Changhai Liang 1
Affiliation
The fabrication of bimetallic catalysts has been taken great focus in the concept of heterogeneous catalysis due to their high efficiency and economic concerns. In this work, a series of bimetallic Ru-Re catalysts were designed and synthesized for the selective hydrogenation of dimethyl terephthalate (DMT) to 1,4-cyclohexane dicarboxylate (DMCD) under mild condition. Characterization techniques including the XRD, TEM, STEM-HAADF EDX elemental mapping, H2-TPR, and XPS were used to study the surface chemical property, the morphology, as well as the catalytic behavior of different samples. It was revealed that the monometallic Ru catalyst already has the capacity to activate and transform DMT into DMCD. Whilst the promotion effect can be optimized to a maximum with only small amount of Re, with the mass ratio of Ru/Re as 10:1. It was also revealed that the addition of Re could largely enhance the distribution of surface active metal species, facilitate the charge transfer between Ru and Re, as well as strengthen the Ru-Re synergistic interaction, which further led to the modification of the redox ability and the catalytic performances of samples. However, excessive addition of Re caused strong interaction between Ru and Re, and further limited the H₂ activation and the seasonable release of the active reducible metal species, which was responsible for the depressed catalytic performances in the presence of higher Re loading. The Ru1.25Re0.13/AC catalyst displayed the DMT conversion of 82% with DMCD selectivity of 96% under mild condition of 70 °C at 3 MPa. The specific rate of Ru1.25Re0.13/AC based on per gram of Ru was 0.44 mol·g-1 Ru·h-1.
中文翻译:
高度分散的双金属Ru-Re / AC催化剂将对苯二甲酸二甲酯选择性加氢成1,4-环己烷二甲酸
由于双金属催化剂的高效率和经济问题,其制备已在非均相催化概念中得到了极大的关注。在这项工作中,设计并合成了一系列双金属Ru-Re催化剂,用于在温和条件下将对苯二甲酸二甲酯(DMT)选择性加氢为1,4-环己烷二甲酸(DMCD)。XRD,TEM,STEM-HAADF EDX元素图谱,H2-TPR和XPS等表征技术用于研究不同样品的表面化学性质,形态以及催化行为。据揭示,单金属Ru催化剂已经具有活化DMT并将其转化为DMCD的能力。尽管仅需少量的Re,Ru / Re的质量比为10:1即可将促进效果最大化。研究还表明,添加Re可以大大提高表面活性金属的分布,促进Ru和Re之间的电荷转移,并增强Ru-Re的协同作用,进而导致氧化还原能力的改变。以及样品的催化性能。然而,过量的Re的加入引起Ru和Re之间的强相互作用,并进一步限制了H 2的活化和活性可还原金属物质的及时释放,这导致在较高的Re载量下催化性能下降。Ru1.25Re0.13 / AC催化剂在70℃和3 MPa的温和条件下显示出82%的DMT转化率和DMCD选择性为96%。相对于每克Ru,Ru1.25Re0.13 / AC的比值为0.44mol·g-1 Ru·h-1。
更新日期:2020-02-01
中文翻译:
高度分散的双金属Ru-Re / AC催化剂将对苯二甲酸二甲酯选择性加氢成1,4-环己烷二甲酸
由于双金属催化剂的高效率和经济问题,其制备已在非均相催化概念中得到了极大的关注。在这项工作中,设计并合成了一系列双金属Ru-Re催化剂,用于在温和条件下将对苯二甲酸二甲酯(DMT)选择性加氢为1,4-环己烷二甲酸(DMCD)。XRD,TEM,STEM-HAADF EDX元素图谱,H2-TPR和XPS等表征技术用于研究不同样品的表面化学性质,形态以及催化行为。据揭示,单金属Ru催化剂已经具有活化DMT并将其转化为DMCD的能力。尽管仅需少量的Re,Ru / Re的质量比为10:1即可将促进效果最大化。研究还表明,添加Re可以大大提高表面活性金属的分布,促进Ru和Re之间的电荷转移,并增强Ru-Re的协同作用,进而导致氧化还原能力的改变。以及样品的催化性能。然而,过量的Re的加入引起Ru和Re之间的强相互作用,并进一步限制了H 2的活化和活性可还原金属物质的及时释放,这导致在较高的Re载量下催化性能下降。Ru1.25Re0.13 / AC催化剂在70℃和3 MPa的温和条件下显示出82%的DMT转化率和DMCD选择性为96%。相对于每克Ru,Ru1.25Re0.13 / AC的比值为0.44mol·g-1 Ru·h-1。