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Metal-Free Single Atom Catalyst for N 2 Fixation Driven by Visible Light
Ist Teil von
Journal of the American Chemical Society, 2018-10, Vol.140 (43), p.14161-14168
Ort / Verlag
United States
Erscheinungsjahr
2018
Link zum Volltext
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
Solar nitrogen (N
) fixation is the most attractive way for the sustainable production of ammonia (NH
), but the development of a highly active, long-term stable and low-cost catalyst remains a great challenge. Current research efforts for N
reduction mainly focus on the metal-based catalysts using the electrochemical approach, while metal-free or solar-driven catalysts have been rarely explored. Herein, on the basis of a concept of electron "acceptance-donation", a metal-free photocatalyst, namely, boron (B) atom, decorated on the optically active graphitic-carbon nitride (B/g-C
N
), for the reduction of N
is proposed by using extensive first-principles calculations. Our results reveal that gas phase N
can be efficiently reduced into NH
on B/g-C
N
through the enzymatic mechanism with a record low onset potential (0.20 V). Moreover, the B-decorated g-C
N
can significantly enhance the visible light absorption, rendering them ideal for solar-driven reduction of N
. Importantly, the as-designed catalyst is further demonstrated to hold great promise for synthesis due to its extremely high stability. Our work is the first report of metal-free single atom photocatalyst for N
reduction, offering cost-effective opportunities for advancing sustainable NH
production.