title: Aluminum Nanocrystals as a Plasmonic Photocatalyst for Hydrogen Dissociation.
abstract: Hydrogen dissociation is a critical step in many hydrogenation reactions central to industrial chemical production and pollutant removal. This step typically utilizes the favorable band structure of precious metal catalysts like platinum and palladium to achieve high efficiency under mild conditions. Here we demonstrate that aluminum nanocrystals (Al NCs), when illuminated, can be used as a photocatalyst for hydrogen dissociation at room temperature and atmospheric pressure, despite the high activation barrier toward hydrogen adsorption and dissociation. We show that hot electron transfer from Al NCs to the antibonding orbitals of hydrogen molecules facilitates their dissociation. Hot electrons generated from surface plasmon decay and from direct photoexcitation of the interband transitions of Al both contribute to this process. Our results pave the way for the use of aluminum, an earth-abundant, nonprecious metal, for photocatalysis.
authors.forename: Linan
authors.initials: L
authors.lastname: Zhou
authors.forename: Chao
authors.initials: C
authors.lastname: Zhang
authors.forename: Michael J
authors.initials: MJ
authors.lastname: McClain
authors.affiliation: Department of Physics and Astronomy, University of New Mexico , Albuquerque, New Mexico 87131, United States.
authors.forename: Alejandro
authors.initials: A
authors.lastname: Manjavacas
authors.forename: Caroline M
authors.initials: CM
authors.lastname: Krauter
authors.forename: Shu
authors.initials: S
authors.lastname: Tian
authors.affiliation: Johannes Gutenberg University Mainz , D 55099 Mainz, Germany.
authors.forename: Felix
authors.initials: F
authors.lastname: Berg
authors.affiliation: Army Aviation and Missile RD&E Center, Redstone Arsenal , Alabama 35898, United States.
authors.forename: Henry O
authors.initials: HO
authors.lastname: Everitt
authors.forename: Emily A
authors.initials: EA
authors.lastname: Carter
authors.forename: Peter
authors.initials: P
authors.lastname: Nordlander
authors.forename: Naomi J
authors.initials: NJ
authors.lastname: Halas
keywords: Plasmonic photocatalysis; aluminum nanocrystals; hot electron; hydrogen dissociation; interband transition