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Electrostatic Stabilization of Single-Atom Catalysts by Ionic Liquids
Chem ( IF 23.5 ) Pub Date : 2019-11-04 , DOI: 10.1016/j.chempr.2019.10.007
Shipeng Ding , Yalin Guo , Max J. Hülsey , Bin Zhang , Hiroyuki Asakura , Lingmei Liu , Yu Han , Min Gao , Jun-ya Hasegawa , Botao Qiao , Tao Zhang , Ning Yan

In single-atom catalysts (SACs), the isolated metal atoms on solid support are often charged. Taking advantage of this common feature, we establish ionic liquid-stabilized single-atom catalysts (ILSSACs) employing electrostatic interaction as a general stabilization strategy. While Pt nanoparticles were formed on hydroxyapatite after reaction when unprotected, Pt remained atomically dispersed on ionic liquid-stabilized samples. Density functional theory calculations reveal that the activation energy for the transformation of two isolated Pt atoms to a Pt dimer increases remarkably from 0.11 to 0.72 eV with the protection of [Bmim][BF4]. The presence of ILs also tunes the electronic state of Pt1, inducing an order-of-magnitude hydrogenation activity increase. The simple stabilization strategy is easily extended to SACs comprising various metal atom-support combinations. For instance, ILs significantly improved the stability and selectivity of a Pd1 catalyst for the hydrogenation of acetylene, thus outperforming unprotected SACs.



中文翻译:

离子液体对单原子催化剂的静电稳定作用

在单原子催化剂(SAC)中,固体载体上的孤立金属原子通常带电。利用此共同特征,我们建立了利用静电相互作用作为一般稳定策略的离子液体稳定单原子催化剂(ILSSAC)。当未保护时,Pt纳米粒子在反应后在羟基磷灰石上形成,而Pt仍然原子分散在离子液体稳定的样品上。密度泛函理论计算表明,在[Bmim] [BF 4 ]的保护下,两个孤立的Pt原子转变为Pt二聚体的活化能从0.11 eV显着增加到0.72 eV 。IL的存在还可以调节Pt 1的电子状态,导致氢化活性增加了一个数量级。简单的稳定策略很容易扩展到包含各种金属原子-载体组合的SAC。例如,离子液体显着提高了Pd 1催化剂用于乙炔加氢的稳定性和选择性,从而胜过了未保护的SAC。

更新日期:2019-11-04
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