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Visualisation of single atom dynamics in water gas shift reaction for hydrogen generation

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Pratibha L. Gai, Kenta Yoshida, Michael R. Ward, Michael Walsh, Richard Baker, Leon van der Water, Mike J. Watson, Edward D. Boyes

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Abstract

The water gas shift (WGS) reaction, CO+H2O = CO2 + H2, is the basis of heterogeneous catalysis important in the generation of clean hydrogen energy for fuel cells, transportation fuels and in ammonia manufacture. Ceria supported gold and related nanoparticles are potentially viable catalysts for the low temperature WGS reaction. The WGS catalytic reaction is a dynamic process and takes place on the solid catalyst surface at the atomic level. The current understanding of the reaction is inferred from studies of static catalysts and from indirect chemical studies without single atom sensitivity. Therefore the nature of dynamic atomic processes in the WGS reaction has remained inaccessible. Since the catalyst reaction site and atomic processes by which it activates and deactivates, change both in magnitude and mechanism with the reaction environment it is of fundamental importance to visualise the dynamic catalyst at the atomic level in WGS (CO + water mixture) environments, in real time. Novel environmental (scanning) transmission electron microscope with singe atom resolution is used herein to directly visualise and characterise, in real time, evolving atomic structures and processes in practical gold/ceria catalysts in controlled WGS environments. The in-situ observations in WGS have revealed the formation of clusters of only a few gold atoms resulting from single atom dynamics and the catalytic effect of low coordination surface sites. The new insights have important implications for applications of nanoparticles in chemical process technologies including for transportation fuels and emission control.
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Original languageEnglish
JournalCatalysis Science & Technology
Early online date13 Nov 2015
DOIs
StateE-pub ahead of print - 13 Nov 2015

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