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, Naomi J. Halas

Research output: Contribution to journalArticlepeer-review

40 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)61-70
Number of pages10
JournalNature Energy
Volume5
Issue number1
DOIs
StatePublished - Jan 1 2020

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology

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