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    Item type:Publication, Access status: without files ,
    Water at charged interfaces
    (2021-07-01)
    Gonella, Grazia
    ;
    Backus, Ellen H.G.
    ;
    Nagata, Yuki
    ;
    Bonthuis, Douwe J.
    ;
    Loche, Philip
    The ubiquity of aqueous solutions in contact with charged surfaces and the realization that the molecular-level details of water–surface interactions often determine interfacial functions and properties relevant in many natural processes have led to intensive research. Even so, many open questions remain regarding the molecular picture of the interfacial organization and preferential alignment of water molecules, as well as the structure of water molecules and ion distributions at different charged interfaces. While water, solutes and charge are present in each of these systems, the substrate can range from living tissues to metals. This diversity in substrates has led to different communities considering each of these types of aqueous interface. In this Review, by considering water in contact with metals, oxides and biomembranes, we show the essential similarity of these disparate systems. While in each case the classical mean-field theories can explain many macroscopic and mesoscopic observations, it soon becomes apparent that such theories fail to explain phenomena for which molecular properties are relevant, such as interfacial chemical conversion. We highlight the current knowledge and limitations in our understanding and end with a view towards future opportunities in the field. [Figure not available: see fulltext.]
    Publicationtype: Review Article
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    Item type:Publication, Access status: with files ,
    Direct and broadband plasmonic charge transfer to enhance water oxidation on a gold electrode
    (American Chemical Society (ACS), 2021-02-23)
    Graf, Matthias
    ;
    Vonbun-Feldbauer, Gregor
    ;
    Koper, Marc T. M.
    Plasmonic photocatalysis via hot charge carriers suffers from their short lifetime compared with the sluggish kinetics of most reactions. To increase lifetime, adsorbates on the surface of a plasmonic metal may create preferential states for electrons to be excited from. We demonstrate this effect with O adsorbates on a nanoporous gold electrode. Nanoporous gold is used to obtain a broadband optical response, to increase the obtained photocurrent, and to provide a SERS-active substrate. Only with adsorbates present, we observe significant photocurrents. Illumination also increases the adsorbate coverage above its dark potential-dependent equilibrium, as derived from a two-laser in situ SERS approach. Density functional theory calculations confirm the appearance of excitable states below the Fermi level. The photocurrent enhancement and broadband characteristics reveal the potential of the plasmonic approach to improve the efficiency of photoelectrochemical water splitting.
    Publicationtype: Journal Article
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