Controlling activity and selectivity using water in the Au-catalysed preferential oxidation of CO in H2

Industrial hydrogen production through methane steam reforming exceeds 50 million tons annually and accounts for 2–5% of global energy consumption. The hydrogen product, even after processing by the water–gas shift, still typically contains ∼1% CO, which must be removed for many applications. Methan...

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Veröffentlicht in:Nature chemistry 2016-06, Vol.8 (6), p.584-589
Hauptverfasser: Saavedra, Johnny, Whittaker, Todd, Chen, Zhifeng, Pursell, Christopher J., Rioux, Robert M., Chandler, Bert D.
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Sprache:eng
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Zusammenfassung:Industrial hydrogen production through methane steam reforming exceeds 50 million tons annually and accounts for 2–5% of global energy consumption. The hydrogen product, even after processing by the water–gas shift, still typically contains ∼1% CO, which must be removed for many applications. Methanation (CO + 3H 2  → CH 4  + H 2 O) is an effective solution to this problem, but consumes 5–15% of the generated hydrogen. The preferential oxidation (PROX) of CO with O 2 in hydrogen represents a more-efficient solution. Supported gold nanoparticles, with their high CO-oxidation activity and notoriously low hydrogenation activity, have long been examined as PROX catalysts, but have shown disappointingly low activity and selectivity. Here we show that, under the proper conditions, a commercial Au/Al 2 O 3 catalyst can remove CO to below 10 ppm and still maintain an O 2 -to-CO 2 selectivity of 80–90%. The key to maximizing the catalyst activity and selectivity is to carefully control the feed-flow rate and maintain one to two monolayers of water (a key CO-oxidation co-catalyst) on the catalyst surface. The preferential oxidation of CO is a potentially efficient means of purifying industrial hydrogen, however, no catalytic systems are known with sufficiently high activity and selectivity. Now Au/Al 2 O 3 catalysts are shown to have outstanding activity and selectivity when both the feed flow-rate and the amount of surface water are carefully controlled.
ISSN:1755-4330
1755-4349
DOI:10.1038/nchem.2494