Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation

Xiao Zhang, Xueqian Li, Du Zhang, Neil Qiang Su, Weitao Yang, Henry O. Everitt () and Jie Liu ()
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Xiao Zhang: Duke University
Xueqian Li: Duke University
Du Zhang: Duke University
Neil Qiang Su: Duke University
Weitao Yang: Duke University
Henry O. Everitt: Duke University
Jie Liu: Duke University

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: Abstract Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. The reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350 °C.

Date: 2017
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DOI: 10.1038/ncomms14542

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