Journal
NATURE MATERIALS
Volume 12, Issue 9, Pages 836-841Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NMAT3696
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Funding
- National Science Foundation [DMR-1207281, DMR-1121288]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1207281] Funding Source: National Science Foundation
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The photocatalytic reduction of N-2 to NH3 is typically hampered by poor binding of N-2 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 N-2 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.
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