Journal
ACS CATALYSIS
Volume 13, Issue 15, Pages 10205-10216Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.3c01837
Keywords
thermoplasmonics; oxygen reduction reaction; plasmonics; titanium nitride; nanohybrids; electrocatalysis
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A fabrication approach was developed to create TiN/F-doped carbon hybrids with high catalytic activity for H2O2 production. These hybrids showed a maximum H2O2 selectivity of 90% and achieved a H2O2 productivity of 207 mmol g(TiN) (-1) h(-1) at 0.2 V vs RHE. The formation of nanocomposites played a key role in achieving high currents, with increased TiO x N y surface content promoting higher H(2)O(2) selectivity and fluorinated nanocarbon imparting good stability to the electrodes due to their superhydrophobic properties.
Large-scale development of electrochemical cells is currentlyhinderedby the lack of Earth-abundant electrocatalysts with high catalyticactivity, product selectivity, and interfacial mass transfer. Herein,we developed an electrocatalyst fabrication approach which respondsto these requirements by irradiating plasmonic titanium nitride (TiN)nanocubes self-assembled on a carbon gas diffusion layer in the presenceof polymeric binders. The localized heating produced upon illuminationcreates unique conditions for the formation of TiN/F-doped carbonhybrids that show up to nearly 20 times the activity of the pristineelectrodes. In alkaline conditions, they exhibit enhanced stability,a maximum H2O2 selectivity of 90%, and achievea H2O2 productivity of 207 mmol g(TiN) (-1) h(-1) at 0.2 V vs RHE. A detailedelectrochemical investigation with different electrode arrangementsdemonstrated the key role of nanocomposite formation to achieve highcurrents. In particular, an increased TiO x N y surface content promoted a higherH(2)O(2) selectivity, and fluorinated nanocarbonsimparted good stability to the electrodes due to their superhydrophobicproperties.
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