Light-driven methane dry reforming with single atomic site antenna-reactor plasmonic photocatalysts

Linan Zhou, John Mark P. Martirez, Jordan Finzel, Chao Zhang, Dayne F. Swearer, Shu Tian, Hossein Robatjazi, Minhan Lou, Liangliang Dong, Luke Henderson, Phillip Christopher, Emily A. Carter (), Peter Nordlander () and Naomi J. Halas ()
Additional contact information
Linan Zhou: Rice University
John Mark P. Martirez: Princeton University
Jordan Finzel: University of California, Santa Barbara
Chao Zhang: Rice University
Dayne F. Swearer: Rice University
Shu Tian: Rice University
Hossein Robatjazi: Rice University
Minhan Lou: Rice University
Liangliang Dong: Rice University
Luke Henderson: Rice University
Phillip Christopher: University of California, Santa Barbara
Emily A. Carter: Princeton University
Peter Nordlander: Rice University
Naomi J. Halas: Rice University

Nature Energy, 2020, vol. 5, issue 1, 61-70

Abstract: Abstract Syngas, an extremely important chemical feedstock composed of carbon monoxide and hydrogen, can be generated through methane (CH4) dry reforming with CO2. However, traditional thermocatalytic processes require high temperatures and suffer from coke-induced instability. Here, we report a plasmonic photocatalyst consisting of a Cu nanoparticle ‘antenna’ with single-Ru atomic ‘reactor’ sites on the nanoparticle surface, ideal for low-temperature, light-driven methane dry reforming. This catalyst provides high light energy efficiency when illuminated at room temperature. In contrast to thermocatalysis, long-term stability (50 h) and high selectivity (>99%) were achieved in photocatalysis. We propose that light-excited hot carriers, together with single-atom active sites, cause the observed performance. Quantum mechanical modelling suggests that single-atom doping of Ru on the Cu(111) surface, coupled with excited-state activation, results in a substantial reduction in the barrier for CH4 activation. This photocatalyst design could be relevant for future energy-efficient industrial processes.

Date: 2020
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DOI: 10.1038/s41560-019-0517-9

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