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Strong metal-support interaction of palladium carbide in PtPd/C catalysts for enhanced catalytic transfer hydrogenolysis of glycerol
Biomass & Bioenergy ( IF 6 ) Pub Date : 2022-06-23 , DOI: 10.1016/j.biombioe.2022.106507
Dongpei Zhang, Wei Yu, Ze Li, Zhenyang Wang, Bin Yin, Xi Liu, Jian Shen, Chaohe Yang, Wenjuan Yan, Xin Jin

Catalytic transfer hydrogenolysis of glycerol can give 1,2-propanediol under mild condition (200 °C) in the absence of external H2. Most existing studies have been focused on metallic catalysts for tandem H2 generation and hydrogenolysis. In this work, a series of bimetallic PtPd/C catalysts with PdCx as promoting role, were synthesized with different calcination temperatures (300–900 °C) and varied Pt/Pd molar ratio (Pd/Pt: 0.5–2.0), to investigate the structure-activity relationship over the in-situ transfer hydrogenation of glycerol. In particular, PtPd/C-900 catalysts showed the best performance (TOF: 37.6 h−1, 1,2-PDO selectivity: 45.3%). It is evidenced that varied metal particle sizes (2.6–7.0 nm) were obtained, and catalytic transfer hydrogenolysis of glycerol displayed size sensitivity over PtPd/C catalysts. Besides, strong metal-support interaction can promote the formation of palladium carbide (PdCx), thus changing the electronic structure of Pt atoms, and improving the activity of hydrogenation reaction and WGS + Reforming reaction. This study will provide insights for the structural design of catalyst for selective transfer hydrogenation of bio-polyols.



中文翻译:

PtPd/C催化剂中碳化钯的强金属-载体相互作用增强甘油催化转移氢解

在没有外部H 2的温和条件下(200℃),甘油的催化转移氢解可以得到1,2-丙二醇。大多数现有研究都集中在用于串联H 2生成和氢解的金属催化剂上。在这项工作中,在不同的煅烧温度(300-900 ℃)和不同的 Pt/Pd 摩尔比(Pd/Pt:0.5-2.0)下合成了一系列以 PdC x为促进作用的双金​​属 PtPd/C 催化剂,以达到研究甘油原位转移氢化的构效关系。特别是 PtPd/C-900 催化剂表现出最佳性能(TOF:37.6 h -1, 1,2-PDO 选择性:45.3%)。有证据表明,获得了不同的金属颗粒尺寸(2.6-7.0 nm),并且甘油的催化转移氢解在 PtPd/C 催化剂上表现出尺寸敏感性。此外,金属-载体的强相互作用可以促进碳化钯(PdC x)的形成,从而改变Pt原子的电子结构,提高加氢反应和WGS+重整反应的活性。该研究将为生物多元醇选择性转移氢化催化剂的结构设计提供见解。

更新日期:2022-06-23
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