Large-scale development of electrochemical cells is currently hindered by the lack of Earth-abundant electrocatalysts with high catalytic activity, product selectivity, and interfacial mass transfer. Herein, we developed an electrocatalyst fabrication approach which responds to these requirements by irradiating plasmonic titanium nitride (TiN) nanocubes self-assembled on a carbon gas diffusion layer in the presence of polymeric binders. The localized heating produced upon illumination creates unique conditions for the formation of TiN/F-doped carbon hybrids that show up to nearly 20 times the activity of the pristine electrodes. In alkaline conditions, they exhibit enhanced stability, a maximum H2O2 selectivity of 90%, and achieve a H2O2 productivity of 207 mmol gTiN-1 h-1 at 0.2 V vs RHE. A detailed electrochemical investigation with different electrode arrangements demonstrated the key role of nanocomposite formation to achieve high currents. In particular, an increased TiOxNy surface content promoted a higher H2O2 selectivity, and fluorinated nanocarbons imparted good stability to the electrodes due to their superhydrophobic properties.

Czech Advanced Technology and Research Institute Regional Centre of Advanced Technologies and Materials Palacký University Olomouc Šlechtitelů 27 78371 Olomouc Czech Republic

Department of Chemical and Pharmaceutical Sciences ICCOM CNR Trieste Research Unit INSTM Trieste Center for Energy Environment and Transport Giacomo Ciamician University of Trieste Via L Giorgieri 1 34127 Trieste Italy

Department of Chemistry and NIS Centre University of Turin 10125 Turin Italy

Nanotechnology Centre Centre of Energy and Environmental Technologies VŠB Technical University of Ostrava 17 listopadu 2172 15 Poruba 708 00 Ostrava Czech Republic

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Single Atom Cocatalysts in Photocatalysis

Facet-Control versus Co-Catalyst-Control in Photocatalytic H2 Evolution from Anatase TiO2 Nanocrystals