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‘Surface Contrast’ NMR Reveals Non‐innocent Role of Support in Pd/CeO2 Catalyzed Phenol Hydrogenation
ChemCatChem ( IF 4.5 ) Pub Date : 2020-05-08 , DOI: 10.1002/cctc.202000608
Timothy K. Egner 1 , Pranjali Naik 1, 2 , Yeongseo An 1 , Amrit Venkatesh 1 , Aaron J. Rossini 1, 2 , Igor I. Slowing 1, 2 , Vincenzo Venditti 1, 3
Affiliation  

Ceria (CeO2)‐supported metals are widely used as catalysts because of their exceptional redox properties. Here, we use surface contrast NMR methods to investigate the hydrogenation of phenol by Pd supported on ceria nanoparticles. We show that the rigid and planar binding of phenol to Pd is mediated by a weak and highly mobile association of the small molecule to ceria. Interestingly, while addition of phosphate to the mixture does not perturb the adsorption of phenol on Pd, it destabilizes its interaction with ceria and proportionally decreases the rate of catalytic conversion. Our data provide strong experimental evidence that weak interactions between adsorbate and ceria are catalytically competent and explain the exceptional performance of Pd/CeO2 for reductive conversions under mild reaction conditions.

中文翻译:

“表面对比” NMR揭示了载体在Pd / CeO2催化的苯酚加氢中的重要作用

二氧化铈(CeO 2)负载的金属因其卓越的氧化还原特性而被广泛用作催化剂。在这里,我们使用表面对比核磁共振方法来研究二氧化铈纳米颗粒上负载的钯对苯酚的氢化作用。我们表明苯酚对Pd的刚性和平面结合是由小分子与二氧化铈的弱且高度移动的缔合介导的。有趣的是,虽然向混合物中添加磷酸盐不会干扰苯酚在Pd上的吸附,但会破坏其与二氧化铈的相互作用并成比例地降低催化转化率。我们的数据提供了有力的实验证据,表明吸附质和二氧化铈之间的弱相互作用具有催化能力,并可以解释Pd / CeO 2的优异性能。 在温和的反应条件下进行还原转化。
更新日期:2020-05-08
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