Controlling the Selectivity of Supported Ru Nanoparticles During Glycerol Hydrogenolysis: C-O vs C-C Cleavage
Controlling the Selectivity of Supported Ru Nanoparticles During Glycerol Hydrogenolysis: C-O vs C-C Cleavage
复制标题
控制甘油氢解过程中负载 Ru 纳米粒子的选择性：C-O 与 C-C 裂解
DOI：
10.1002/cctc.202001881
复制
发表时间：
2021
期刊：
影响因子：
4.5
通讯作者：
Guadix-Montero S
中科院分区：
文献类型：
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作者：
Guadix-Montero S
通过合理设计催化剂来控制反应的选择性是催化研究中的一个重要而富有挑战性的课题。在这篇文章中，我们报告了一种策略，以调整产品的选择性在水相氢解甘油使用气态H2。Ru/TiO 2是甘油氢解的活性催化剂，但它促进了C-C键的氢解，导致大量的C2和C1产物。另一方面，Pd/TiO 2和Pt/TiO 2催化剂对C-O键的氢解具有很高的选择性，主要产生C3产物（1，2和1，3丙二醇），但与Ru催化剂相比，它们的活性要低得多。在这篇文章中，我们报告说，通过将Ru与Pt或Pd结合在纳米颗粒中，我们可以开发出对C−O氢解既有活性又有选择性的新催化剂。两种单金属催化剂的物理混合物并没有表现出这种增强的C-O氢解选择性，证明了纳米颗粒中两种金属的紧密混合对于调节选择性至关重要。所有的monoclonal和monoclonal催化剂已经通过显微镜和光谱方法进行了表征，以了解它们的结构特征。DFT的研究也进行了合理化的monoclonal和monoclonal催化剂之间的催化性能的观察到的差异。
Controlling the selectivity of a reaction by rational designing of catalyst is an important and challenging topic in catalysis research. In this article, we report a strategy to tune the product selectivity during aqueous phase hydrogenolysis of glycerol using gaseous H2. Ru/TiO2is an active catalyst for the hydrogenolysis of glycerol, however it promotes the hydrogenolysis of C−C bonds resulting in large quantities of C2 and C1 products. On the other hand, Pd/TiO2and Pt/TiO2catalysts are very selective for the hydrogenolysis of C−O bonds producing mainly C3 products (1,2 and 1,3 propanediols), however they are much less active compared to the Ru catalysts. In this article, we report that by combining Ru with Pt or Pd in a bimetallic nanoparticle, we can develop new catalysts that are both active and selective for C−O hydrogenolysis. A physical mixture of two monometallic catalysts does not show this enhanced selectivity for C−O hydrogenolysis, proving that intimate mixing of the two metals in a nanoparticle is crucial to tune the selectivity. All the monometallic and bimetallic catalysts have been characterised by microscopic and spectroscopic methods to understand their structural features. DFT studies were also done to rationalise the observed difference in the catalytic properties between monometallic and bimetallic catalysts.