Qiao Ying, Cao Wei, Qian Sheng-Jie, Yao Zhen, Wang Yang-Gang
Department of Chemistry and Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China.
J Chem Phys. 2024 Feb 21;160(7). doi: 10.1063/5.0185491.
The catalytic hydrogenation of biomass-derived chemicals is essential in chemical industry due to the growing demand for sustainable and renewable energy sources. In this study, we present a comprehensive theoretical investigation regarding the hydrogenation of glycolaldehyde to ethylene glycol over a Ru/C catalyst by employing density functional theory and ab initio molecular dynamics simulations. With inclusion of explicit solvation, we have demonstrated that the glycolaldehyde hydrogenation is significantly improved due to the fast proton transfer through the hydrogen bond network. The enhanced activity could be attributed to the participation of the solvent water as the hydrogen source and the highly positively charged state of a Ru cluster in an aqueous phase, which are critical for the activation of aldehyde groups and proton-assisted hydrogenation. Overall, our findings provide valuable insights into glycolaldehyde hydrogenation over Ru/C catalysts in the aqueous phase, highlighting the importance of solvation effects in the biomass conversion.
由于对可持续和可再生能源的需求不断增长，生物质衍生化学品的催化加氢在化学工业中至关重要。在本研究中，我们通过采用密度泛函理论和从头算分子动力学模拟，对乙二醇醛在Ru/C催化剂上催化加氢生成乙二醇进行了全面的理论研究。通过引入明确的溶剂化作用，我们证明了由于质子通过氢键网络的快速转移，乙二醇醛的加氢反应得到了显著改善。活性增强可归因于溶剂水作为氢源的参与以及Ru簇在水相中的高正电荷状态，这对于醛基的活化和质子辅助加氢至关重要。总体而言，我们的研究结果为水相中Ru/C催化剂上的乙二醇醛加氢提供了有价值的见解，突出了溶剂化效应在生物质转化中的重要性。
