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Turning aluminium into a noble-metal-like catalyst for low-temperature activation of molecular hydrogen

Nature Materials volume 10, pages 884–889 (2011)Cite this article

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A Corrigendum to this article was published on 23 November 2011

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Abstract

Activation of molecular hydrogen is the first step in producing many important industrial chemicals that have so far required expensive noble-metal catalysts and thermal activation. We demonstrate here that aluminium doped with very small amounts of titanium can activate molecular hydrogen at temperatures as low as 90 K. Using an approach that uses CO as a probe molecule, we identify the atomistic arrangement of the catalytically active sites containing Ti on Al(111) surfaces, combining infrared reflection–absorption spectroscopy and first-principles modelling. CO molecules, selectively adsorbed on catalytically active sites, form a complex with activated hydrogen that is removed at remarkably low temperatures (115 K; possibly as a molecule). These results provide the first direct evidence that Ti-doped Al can carry out the essential first step of molecular hydrogen activation under nearly barrierless conditions, thereby challenging the monopoly of noble metals in hydrogen activation.

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Figure 1: Infrared reflection–absorption spectra of CO molecules adsorbed on Al(111) surfaces at 90 K.
Figure 2: Ti surface configurations relevant for hydrogen dissociation.
Figure 3: Catalytic activity as a function of Ti coverage.
Figure 4: Evidence for hydrogen spillover from catalytic site onto bare Al.
Figure 5: Catalytic activity of Ti-doped Al(111) surface.
Figure 6: Evolution of CO–H complex (2,222 cm−1 band) on a 0.1 ML Ti-doped Al(111) surface.

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  • 21 October 2011

    In the version of this Article originally published, the first sentence of the Acknowledgements should have read that the work performed at the University of Texas at Dallas was fully supported by the Office of Basic Energy Sciences, U.S. Department of Energy, under contract no. DE-AC02-98CH10886. This error has been corrected in the HTML and PDF versions of the Article.

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Acknowledgements

The experimental work performed at the University of Texas at Dallas was fully supported by the Office of Basic Energy Sciences, U.S. Department of Energy, under contract no. DE-AC02-98CH10886. The theoretical work carried out at Washington State University was supported by the Office of Naval Research (grants N00014-04-1-0688 and N00014-06-1-0315).

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Authors and Affiliations

  1. Department of Materials Science and Engineering, University of Texas at Dallas, Richardson, Texas 75080, USA

    Irinder S. Chopra, Jean François Veyan & Yves J. Chabal

  2. ISP/Applied Sciences Laboratory, Washington State University, Spokane, Washington 99210-1495, USA

    Santanu Chaudhuri

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  1. Irinder S. Chopra
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  2. Santanu Chaudhuri
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Contributions

I.S.C. carried out all the experiments, with technical support from J.F.V. for apparatus design and modification. S.C. carried out all the calculations and Y.J.C. supervised the experimental work. S.C., Y.J.C. and I.S.C. contributed equally to the manuscript.

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Correspondence to Yves J. Chabal.

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Chopra, I., Chaudhuri, S., Veyan, J. et al. Turning aluminium into a noble-metal-like catalyst for low-temperature activation of molecular hydrogen. Nature Mater 10, 884–889 (2011). https://doi.org/10.1038/nmat3123

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