4.8 Article

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

Journal

NATURE CHEMISTRY
Volume 8, Issue 6, Pages 585-590

Publisher

NATURE PORTFOLIO
DOI: 10.1038/NCHEM.2494

Keywords

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Funding

  1. US National Science Foundation [CBET-1160217, CHE-1012395]
  2. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Sciences Program [DE-FG02-12ER16364]
  3. Div Of Chem, Bioeng, Env, & Transp Sys
  4. Directorate For Engineering [1160217] Funding Source: National Science Foundation

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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 similar to 1% CO, which must be removed for many applications. Methanation (CO + 3H(2) -> CH4 + H2O) 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/Al2O3 catalyst can remove CO to below 10 ppm and still maintain an O-2-to-CO2 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.

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