Photo-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction

TitlePhoto-illuminated diamond as a solid-state source of solvated electrons in water for nitrogen reduction
Publication TypeJournal Article
Year of Publication2013
AuthorsZhu, D, Zhang, L, Ruther, RE, Hamers, RJ
JournalNature Materials
Volumeadvance online publication
Date Published06/2013
Keywordsammonia, catalysis, diamond, nitrogen, nitrogen fixation
Abstract

The photocatalytic reduction of N2 to NH3 is typically hampered by poor binding of N2 to catalytic materials and by the very high energy of the intermediates involved in this reaction. Solvated electrons directly introduced into the reactant solution can provide an alternative pathway to overcome such limitations. Here we demonstrate that illuminated hydrogen-terminated diamond yields facile electron emission into water, thus inducing reduction of N2 to NH3 at ambient temperature and pressure. Transient absorption measurements at 632 nm reveal the presence of solvated electrons adjacent to the diamond after photoexcitation. Experiments using inexpensive synthetic diamond samples and diamond powder show that photocatalytic activity is strongly dependent on the surface termination and correlates with the production of solvated electrons. The use of diamond to eject electrons into a reactant liquid represents a new paradigm for photocatalytic reduction, bringing electrons directly to reactants without requiring molecular adsorption to the surface.

DOI10.1038/nmat3696
Refereed DesignationRefereed