title: Decoupled catalytic hydrogen evolution from a molecular metal oxide redox mediator in water splitting.
abstract: The electrolysis of water using renewable energy inputs is being actively pursued as a route to sustainable hydrogen production. Here we introduce a recyclable redox mediator (silicotungstic acid) that enables the coupling of low-pressure production of oxygen via water oxidation to a separate, catalytic hydrogen production step outside the electrolyzer that requires no post-electrolysis energy input. This approach sidesteps the production of high-pressure gases inside the electrolytic cell (a major cause of membrane degradation) and essentially eliminates the hazardous issue of product gas crossover at the low current densities that characterize renewables-driven water-splitting devices. We demonstrated that a platinum-catalyzed system can produce pure hydrogen over 30 times faster than state-of-the-art proton exchange membrane electrolyzers at equivalent platinum loading.
authors.affiliation: WestCHEM, School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, UK.
authors.forename: Benjamin
authors.initials: B
authors.lastname: Rausch
authors.affiliation: WestCHEM, School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, UK.
authors.forename: Mark D
authors.initials: MD
authors.lastname: Symes
authors.affiliation: WestCHEM, School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, UK.
authors.forename: Greig
authors.initials: G
authors.lastname: Chisholm
authors.affiliation: WestCHEM, School of Chemistry, University of Glasgow, University Avenue, Glasgow G12 8QQ, UK. lee.cronin@glasgow.ac.uk.
authors.forename: Leroy
authors.initials: L
authors.lastname: Cronin