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.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Zhang X,Li X,Zhang D,Su NQ,Yang W,Everitt HO,Liu Jdoi
10.1038/ncomms14542subject
Has Abstractpub_date
2017-02-23 00:00:00pages
14542issn
2041-1723pii
ncomms14542journal_volume
8pub_type
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