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• W2131924274 abstract "Spillover of reactants from one active site to another is important in heterogeneous catalysis but is notoriously hard to detect or control, especially for hydrogen. The hydrogen spillover pathway on a Pd–Cu alloy can now be controlled by reversible adsorption of a spectator molecule. This effect observed during a surface catalysed reaction should prove useful for controlling uptake and release of hydrogen in a model storage system. Spillover of reactants from one active site to another is important in heterogeneous catalysis and has recently been shown to enhance hydrogen storage in a variety of materials1,2,3,4,5,6,7. The spillover of hydrogen is notoriously hard to detect or control1,2,4,5,6. We report herein that the hydrogen spillover pathway on a Pd/Cu alloy can be controlled by reversible adsorption of a spectator molecule. Pd atoms in the Cu surface serve as hydrogen dissociation sites from which H atoms can spillover onto surrounding Cu regions. Selective adsorption of CO at these atomic Pd sites is shown to either prevent the uptake of hydrogen on, or inhibit its desorption from, the surface. In this way, the hydrogen coverage on the whole surface can be controlled by molecular adsorption at a minority site, which we term a ‘molecular cork’ effect. We show that the molecular cork effect is present during a surface catalysed hydrogenation reaction and illustrate how it can be used as a method for controlling uptake and release of hydrogen in a model storage system1,2,4,5,6,8." @default.
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• W2131924274 date "2013-04-21" @default.
• W2131924274 modified "2023-10-17" @default.
• W2131924274 title "Controlling a spillover pathway with the molecular cork effect" @default.
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• W2131924274 doi "https://doi.org/10.1038/nmat3620" @default.
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