Control of monomeric Vo’s versus Vo clusters in ZrO(2−x) for solar-light H(2) production from H(2)O at high-yield (millimoles gr(−1) h(−1))

Pristine zirconia, ZrO(2), possesses high premise as photocatalyst due to its conduction band energy edge. However, its high energy-gap is prohibitive for photoactivation by solar-light. Currently, it is unclear how solar-active zirconia can be designed to meet the requirements for high photocatalytic performance. Moreover, transferring this design to an industrial-scale process is a forward-looking route. Herein, we have developed a novel Flame Spray Pyrolysis process for generating solar-light active nano-ZrO(2−x) via engineering of lattice vacancies, Vo. Using solar photons, our optimal nano-ZrO(2−x) can achieve milestone H(2)-production yield, > 2400 μmolg(−1) h(−1) (closest thus, so far, to high photocatalytic water splitting performance benchmarks). Visible light can be also exploited by nano-ZrO(2−x) at a high yield via a two-photon process. Control of monomeric Vo versus clusters of Vo’s is the key parameter toward Highly-Performing-Photocatalytic ZrO(2−x). Thus, the reusable and sustainable ZrO(2−x) catalyst achieves so far unattainable solar activated photocatalysis, under large scale production.