title: Plasmon enhanced water splitting mediated by hybrid bimetallic Au-Ag core-shell nanostructures.
abstract: In this work, we employed wet chemically synthesized bimetallic Au-Ag core-shell nanostructures (Au-AgNSs) to enhance the photocurrent density of mesoporous TiO2 for water splitting and we compared the results with monometallic Au nanoparticles (AuNPs). While Au-AgNSs incorporated photoanodes give rise to 14× enhancement in incident photon to charge carrier efficiency, AuNPs embedded photoanodes result in 6× enhancement. By varying nanoparticle concentration in the photoanodes, we observed ∼245× less Au-AgNSs are required relative to AuNPs to generate similar photocurrent enhancement for solar fuel conversion. Power-dependent measurements of Au-AgNSs and AuNPs showed a first order dependence to incident light intensity, relative to half-order dependence for TiO2 only photoanodes. This indicated that plasmonic nanostructures enhance charge carriers formed on the surface of the TiO2 which effectively participate in photochemical reactions. Our experiments and simulations suggest the enhanced near-field, far-field, and multipolar resonances of Au-AgNSs facilitating broadband absorption of solar radiation collectively gives rise to their superior performance in water splitting.
authors.affiliation: Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, Tennessee 37235, USA. rizia.bardhan@vanderbilt.edu.
authors.forename: William R
authors.initials: WR
authors.lastname: Erwin
authors.forename: Andrew
authors.initials: A
authors.lastname: Coppola
authors.forename: Holly F
authors.initials: HF
authors.lastname: Zarick
authors.forename: Poorva
authors.initials: P
authors.lastname: Arora
authors.forename: Kevin J
authors.initials: KJ
authors.lastname: Miller
authors.forename: Rizia
authors.initials: R
authors.lastname: Bardhan