Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
School of Chemistry, Cardiff University, Cardiff CF10 3AT, UK.
Philos Trans A Math Phys Eng Sci. 2020 Jul 24;378(2176):20200055. doi: 10.1098/rsta.2020.0055. Epub 2020 Jul 6.
We report the role of the acidity of support during the selectivity hydrogenolysis of glycerol over supported bimetallic palladium-ruthenium (PdRu) catalysts. The PdRu nanoparticles were supported on a series of metal oxides and zeolitic supports via the modified impregnation method and tested for the liquid-phase hydrogenolysis of glycerol using gaseous hydrogen. The relative acid site densities of selected catalysts were determined by ammonia temperature-programmed desorption and pyridine desorption experiments. Based on these studies, we report a direct correlation between the catalytic activity (conversion and 1,2 propane diol yield) and two different acid sites (strong acid sites and very strong acid sites). Besides zeolite-supported catalysts, TiO supported PdRu nanoparticles exhibit moderate catalytic activity; however, this catalyst shows high selectivity for the desired C-O bond cleavage to produce C3 products over the undesired C-C bond cleavage to produce < C3 products. This article is part of a discussion meeting issue 'Science to enable the circular economy'.
我们研究了在负载型双金属钯-钌（PdRu）催化剂上选择性催化甘油氢解过程中载体酸度的作用。PdRu 纳米颗粒通过改良浸渍法负载在一系列金属氧化物和沸石载体上，并使用氢气进行液相甘油氢解测试。通过氨程序升温脱附和吡啶解吸实验来确定所选催化剂的相对酸位密度。基于这些研究，我们报告了催化活性（转化率和 1,2-丙二醇收率）与两种不同酸位（强酸位和超强酸位）之间的直接相关性。除了沸石负载的催化剂外，TiO2 负载的 PdRu 纳米颗粒表现出适度的催化活性；然而，该催化剂在所需的 C-O 键断裂生成 C3 产物方面表现出较高的选择性，而在不希望的 C-C 键断裂生成 <C3 产物方面则表现出较低的选择性。本文是“科学助力循环经济”讨论专题的一部分。
