title: Efficient hydrogen evolution catalysis using ternary pyrite-type cobalt phosphosulphide.
abstract: The scalable and sustainable production of hydrogen fuel through water splitting demands efficient and robust Earth-abundant catalysts for the hydrogen evolution reaction (HER). Building on promising metal compounds with high HER catalytic activity, such as pyrite structure cobalt disulphide (CoS2), and substituting non-metal elements to tune the hydrogen adsorption free energy could lead to further improvements in catalytic activity. Here we present a combined theoretical and experimental study to establish ternary pyrite-type cobalt phosphosulphide (CoPS) as a high-performance Earth-abundant catalyst for electrochemical and photoelectrochemical hydrogen production. Nanostructured CoPS electrodes achieved a geometrical catalytic current density of 10 mA cm(-2) at overpotentials as low as 48 mV, with outstanding long-term operational stability. Integrated photocathodes of CoPS on n(+)-p-p(+) silicon micropyramids achieved photocurrents up to 35 mA cm(-2) at 0 V versus the reversible hydrogen electrode (RHE), onset photovoltages as high as 450 mV versus RHE, and the most efficient solar-driven hydrogen generation from Earth-abundant systems.
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: Miguel
authors.initials: M
authors.lastname: Cabán-Acevedo
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: Michael L
authors.initials: ML
authors.lastname: Stone
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: J R
authors.initials: JR
authors.lastname: Schmidt
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: Joseph G
authors.initials: JG
authors.lastname: Thomas
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: Qi
authors.initials: Q
authors.lastname: Ding
authors.affiliation: Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia.
authors.forename: Hung-Chih
authors.initials: HC
authors.lastname: Chang
authors.affiliation: Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia.
authors.forename: Meng-Lin
authors.initials: ML
authors.lastname: Tsai
authors.affiliation: Division of Computer, Electrical and Mathematical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia.
authors.forename: Jr-Hau
authors.initials: JH
authors.lastname: He
authors.affiliation: Department of Chemistry, University of Wisconsin-Madison, 1101 University Avenue Madison, Wisconsin 53706, USA.
authors.forename: Song
authors.initials: S
authors.lastname: Jin