Photoelectrocatalysis has emerged as a promising route for conversion of atmospheric nitrogen to ammonia or nitrates under mild conditions. The electrochemical driving force, provided by photoexcitation or applied bias, enables an alternative to high temperatures and pressures that are required to overcome kinetic and thermodynamic limitations in thermal catalysis. The most well-known catalyst for photocatalytic nitrogen fixation is titanium dioxide, but the fundamental mechanism of the reaction remains controversial. We provide computational and experimental evidence for a carbon-based active site and inherently photochemical reaction mechanism for photocatalytic ammonia, and examine the possibility of improving the kinetics of electrochemical nitrogen reduction by doping the titania catalyst with transition metals. The implications and limitations of the approach are discussed, along with an outlook for promising future strategies to computationally design new catalysts for photoelectrochemical nitrogen reduction.

Computational insight into photoelectrocatalaytic nitrogen fixation by titania-based catalysts

ACS Fall 2021

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