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Differentiation of Pt−Fe and Pt−Ni3 Surface Catalytic Mechanisms towards Contrasting Products in Chemoselective Hydrogenation of α,β‐Unsaturated Aldehydes
ChemCatChem ( IF 4.5 ) Pub Date : 2020-11-10 , DOI: 10.1002/cctc.202001482
Liangmin Ning 1 , Mingtao Zhang 1 , Shengyun Liao 2 , Yuting Zhang 1 , Dandan Jia 1 , Yunfang Yan 1 , Wen Gu 1 , Xin Liu 1
Affiliation  

Noble‐metal catalysts serve as an irreplaceable role in pharmaceutical, perfume and fine chemicals fields. However, there still remains a grand challenge in controlling chemoselectivity. Herein, we have synthesized a bimetallic nanostructure supported on porous metal‐organic frameworks (Pt−Fe/UiO‐66, Pt‐Ni3/UiO‐66), in which Pt nanoparticles was modified with non‐noble metal (Fe or Ni) directly. The as‐synthesized catalysts can function as a switch for selective hydrogenation of α,β‐unsaturated aldehydes to afford the potential products on‐demand. In comparison with the conventional Pt‐based catalysts, Pt−Fe/UiO‐66 and Pt‐Ni3/UiO‐66 catalysts exhibit excellently catalytic activity, enhanced selectivity and improved stability for selectivity hydrogenation. The partial charge reconfiguration and electronic coupling effect existing in such distinctive bicomponent nanocatalysts was confirmed by some comprehensive characterization and density functional theory (DFT) calculations. The developed method for precisely modification the composition and interaction between the noble metal and non‐noble metal provides a feasible avenue to design the advanced catalysts.

中文翻译:

α,β-不饱和醛化学选择性加氢中Pt-Fe和Pt-Ni3表面催化机理对不同产物的区别

贵金属催化剂在制药,香料和精细化工领域起着不可替代的作用。但是,在控制化学选择性方面仍然存在巨大挑战。在本文中,我们合成了负载在多孔金属有机骨架上的双金属纳米结构(Pt-Fe / UiO-66,Pt-Ni 3 / UiO-66),其中Pt纳米粒子被非贵金属(Fe或Ni)改性直。合成后的催化剂可以用作α,β-不饱和醛选择性加氢的开关,从而按需提供潜在的产物。与传统的基于Pt的催化剂相比,Pt-Fe / UiO-66和Pt-Ni 3/ UiO-66催化剂具有出色的催化活性,更高的选择性和更高的选择性加氢稳定性。通过一些全面的表征和密度泛函理论(DFT)计算,证实了这种独特的双组分纳米催化剂中存在的部分电荷重配置和电子耦合效应。精确修饰贵金属与非贵金属之间的组成和相互作用的已开发方法为设计高级催化剂提供了可行的途径。
更新日期:2020-11-10
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