Theoretical Insights on the Synergistic Effect of Dual Metal Sites Supported on MgO(100) Promoting the Hydrogenation Reaction

IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL
Ruifang Xue, Fang-Fang Wang, De-Li Chen, Fumin Zhang, Weidong Zhu
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Abstract

Designing heterogeneous catalysts with dual-functional sites for hydrogenation reactions holds significant potential for improving activity and selectivity. We present catalysts that incorporate two distinct metal sites onto a MgO support, serving as adsorption sites for reactant and H2, respectively. From screening 16 candidates using density functional theory calculations, we identified Pt1Al1/MgO as a promising catalyst for nitroaromatic hydrogenation. The Al–Mg moiety adsorbs 3-nitrostyrene via its nitro group, while the neighboring Pt–O facilitates H2 dissociation through transient frustrated Lewis pairs. The synergistic effect of the Al–O–Pt moiety enhances reaction activity, driven by the appropriate adsorption/desorption of *H at the Pt site and a low diffusion barrier. This study offers valuable insights into the design of transient frustrated Lewis pair catalysts and is pivotal for the development of heterogeneous catalysts with dual-sites for hydrogenation reactions.

Abstract Image

MgO(100)负载双金属位促进加氢反应协同效应的理论见解
设计具有双功能位点的多相催化剂用于加氢反应具有显著的提高活性和选择性的潜力。我们提出了将两个不同的金属位点结合到MgO载体上的催化剂,分别作为反应物和H2的吸附位点。通过密度泛函理论计算筛选16种候选催化剂,我们确定Pt1Al1/MgO是一种很有前景的硝基芳烃加氢催化剂。Al-Mg部分通过硝基吸附3-硝基苯乙烯,而相邻的Pt-O通过瞬态受挫刘易斯对促进H2解离。Al-O-Pt部分的协同作用增强了反应活性,这是由Pt位点上*H的适当吸附/解吸和低扩散势垒驱动的。该研究为瞬态受挫Lewis对催化剂的设计提供了有价值的见解,对开发用于加氢反应的双位点非均相催化剂具有关键意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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