Hydrogen Spillover. Facts and Fiction

Prins, R.

doi:10.1021/cr200346z

Cited by 941 publications

(724 citation statements)

References 198 publications

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“…Since the discovery in the early 1960s 1,2 , hydrogen spillover has attracted the attention of many scientists, who have tried not only to explain it but also to exploit it for designing advanced catalysts with enhanced catalytic activity and lifetime [3][4][5] . Historically researchers have agreed on the existence of hydrogen spillover on semiconductors and conductors, because a hydrogen atom can migrate as a proton (H þ ) and electron (e À ) pair.…”

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confidence: 99%

“…Historically researchers have agreed on the existence of hydrogen spillover on semiconductors and conductors, because a hydrogen atom can migrate as a proton (H þ ) and electron (e À ) pair. Protons can migrate over the support surface and electrons can transfer through the conduction band of material framework, which is thermodynamically feasible process 5 . In contrast to the cases of semiconductors and conductors, there have been ongoing debates on the existence of hydrogen spillover on insulating materials (SiO 2 , Al 2 O 3 and zeolite).…”

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confidence: 99%

“…Despite extensive studies on these metal oxides, the nature of spillover species, the migration mechanism, catalytic functions and even its existence remain topics of vigorous debate 5 . For a large part, this is a consequence of the lack of model catalysts that can provide direct evidences on the existence of hydrogen spillover and simplify the catalytic interpretation.…”

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confidence: 99%

“…This was ascribed to hydrogen spillover from the Pt/KA to the NaY or H-ZSM-5 surface where the isobutylene was hydrogenated. Transmission electron micrographs (TEM) investigation showed, however, that some of the Pt particles were much larger than the zeolite cages and that part of the zeolite structure was damaged 5,8 .…”

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

et al. 2014

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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.

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

et al. 2014

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“…catalyst ? support physical mixtures) [27]. This spillover hydrogen contributes to hydrogenation activity [28].…”

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Overcoming the limitations of gold catalysts in hydrogenation: enhanced activity with full hydrogen utilization

Keane

Collado

et al. 2018

Reac Kinet Mech Cat

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Application of nano-scale supported Au in catalytic hydrogenation delivers high chemoselectivity but low activity using (pressurized) H 2 far in excess of stoichiometric requirements. We have tackled the issues of low reaction rate and inefficient hydrogen utilization through a series of approaches taking Au/CeO 2 (mean Au size = 2.8 nm) as a test catalyst. Increased spillover hydrogen (using physical mixtures of Au/CeO 2 with CeO 2 and SiO 2 ) and the promotional effect of water (via catalytic dissociation on surface oxygen vacancies) resulted in a fourfold increase in the selective rate of furfural hydrogenation to furfuryl alcohol. In contrast, Pd/CeO 2 and Ni/CeO 2 promoted decarbonylation (to furan), hydrogenolysis (to 2-methylfuran) and ring reduction (to tetrahydrofurfuryl alcohol). Coupling (2-butanol ? 2-butanone) dehydrogenation over Cu/SiO 2 (mean Cu size = 7.8 nm) with furfural hydrogenation over Au/CeO 2 further increased rate with full utilization of the hydrogen generated in dehydrogenation. The coupling strategy allows ''hydrogen free'' hydrogenation that circumvents the limitation of Au in standard catalytic hydrogenation. This can open new avenues to exploit the ultra-selectivity of Au for continuous production of high value commodity products.

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Hydrogen Storage in Graphene

Li¹,

Chen²

2013

Graphene Chemistry

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Hydrogen Spillover. Facts and Fiction

Cited by 941 publications

References 198 publications

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

Overcoming the limitations of gold catalysts in hydrogenation: enhanced activity with full hydrogen utilization

Hydrogen Storage in Graphene

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