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Covalent-bonding to irreducible SiO2 leads to high-loading and atomically dispersed metal catalysts
Journal of Catalysis ( IF 6.5 ) Pub Date : 2017-08-17 , DOI: 10.1016/j.jcat.2017.07.030
Yifeng Zhu , Xiao Kong , Junqing Yin , Rui You , Bin Zhang , Hongyan Zheng , Xiaodong Wen , Yulei Zhu , Yong-Wang Li

Being a suitable way for achieving the maximum efficiency of atoms, the atomically dispersed metals are playing an ever-increasingly important role in bridging heterogeneous and homogeneous catalysis. It is extremely challenging for dispersing metals in atomic-scales as the applicable high-loading catalysts for industry. The reducible and defective supports or metal surfaces are commonly chosen for anchoring the metals. We here report that atomically-dispersed but high-loading (15 wt%) metals were achieved by covalent-bonding to irreducible SiO2 (though silanol groups) which is realized by a simple urea hydrolysis assistant hydrothermal-deposition method. The CuOSi bonding tailors the structural and electronic states of catalyst by maximum of atom efficiency and tuning electronic effects. The intrinsic performance of CO hydrogenation was thus boosted by one- to two- orders-of-magnitude in comparison with impregnated and precipitated catalysts. The choices of metals include Cu, Zn, Ni, Co and Mn, showing potentials for a category of applied materials.



中文翻译:

共价键合至不可还原的SiO 2导致高负载和原子分散的金属催化剂

作为实现原子最大效率的一种合适方法,原子分散的金属在弥合非均相和均相催化中起着越来越重要的作用。作为适用于工业的高负载催化剂,以原子级分散金属是极具挑战性的。通常选择可还原和有缺陷的支撑物或金属表面来锚定金属。我们在这里报道,通过共价键合到不可还原的SiO 2(尽管有硅烷醇基),可以实现原子分散但高负载(15 wt%)的金属,这是通过简单的尿素水解助剂水热沉积方法实现的。铜Ø硅键合通过最大程度地提高原子效率和调节电子效应来调整催化剂的结构和电子状态。因此,与浸渍和沉淀的催化剂相比,CO氢化的内在性能提高了一到两个数量级。金属的选择包括Cu,Zn,Ni,Co和Mn,显示出适用于一类应用材料的潜力。

更新日期:2017-08-17
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