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Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures
Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures
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Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures
Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures

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Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures
Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures
Journal Article

Maximizing the catalytic function of hydrogen spillover in platinum-encapsulated aluminosilicates with controlled nanostructures

2014
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Overview
Hydrogen spillover has been studied for several decades, but its nature, catalytic functions and even its existence remain topics of vigorous debate. This is a consequence of the lack of model catalysts that can provide direct evidences of the existence of hydrogen spillover and simplify the catalytic interpretation. Here we use platinum encapsulated in a dense aluminosilicate matrix with controlled diffusional properties and surface hydroxyl concentrations to elucidate the catalytic functions of hydrogen spillover. The catalytic investigation and theoretical modelling show that surface hydroxyls, presumably Brønsted acids, are crucial for utilizing the catalytic functions of hydrogen spillover on the aluminosilicate surface. The catalysts with optimized nanostructure show remarkable activities in hydro-/dehydrogenation, but virtually no activity for hydrogenolysis. This distinct chemoselectivity may be beneficial in industrially important hydroconversions such as propane dehydrogenation to propylene because the undesired hydrogenolysis pathway producing light hydrocarbons of low value (methane and ethane) is greatly suppressed. The hydrogen spillover mechanism has been studied for several decades, although its exact elucidation has been hampered by the lack of suitable model catalyst systems. Here, the authors combine experimental and computational techniques to probe the role of surface hydroxyls in the mechanism.