Nitrogen Photoelectrochemical Reduction on TiB2 Surface Plasmon Coupling Allows Us to Reach Enhanced Efficiency of Ammonia Production

0574348 - ÚACH 2024 RIV US eng J - Journal Article
Zabelina, A. - Miliutina, E. - Dědek, J. - Trelin, A. - Zabelin, D. - Valiev, R. R. - Ramazanov, R. - Burtsev, V. - Popelková, Daniela - Šťastný, Martin - Švorčík, V. - Lyutakov, O.
Nitrogen Photoelectrochemical Reduction on TiB2 Surface Plasmon Coupling Allows Us to Reach Enhanced Efficiency of Ammonia Production.
ACS Catalysis. Roč. 13, č. 16 (2023), s. 10916-10926. ISSN 2155-5435. E-ISSN 2155-5435
R&D Projects: GA MŠMT(CZ) LM2018124
Institutional support: RVO:61388980
Keywords : photoelectrochemical nitrogen reduction * plasmon coupling * TiB2 * NH3 * productionhybrid photocatalyst
OECD category: Inorganic and nuclear chemistry
Impact factor: 12.9, year: 2022
Method of publishing: Open access

Ammonia is one of the most widely produced chemicalsworldwide,which is consumed in the fertilizer industry and is also consideredan interesting alternative in energy storage. However, common ammoniaproduction is energy-demanding and leads to high CO2 emissions.Thus, the development of alternative ammonia production methods basedon available raw materials (air, for example) and renewable energysources is highly demanding. In this work, we demonstrated the utilizationof TiB2 nanostructures sandwiched between coupled plasmonicnanostructures (gold nanoparticles and gold grating) for photoelectrochemical (PEC) nitrogen reduction and selective ammonia production. The utilizationof the coupled plasmon structure allows us to reach efficient sunlightcapture with a subdiffraction concentration of light energy in thespace, where the catalytically active TiB2 flakes wereplaced. As a result, PEC experiments performed at -0.2 V (vs.RHE) and simulated sunlight illumination give the 535.2 and 491.3 & mu,g h(-1) mg(cat) (-1) ammonia yields, respectively, with the utilization of pure nitrogenand air as a nitrogen source. In addition, a number of control experimentsconfirm the key role of plasmon coupling in increasing the ammoniayield, the selectivity of ammonia production, and the durability ofthe proposed system. Finally, we have performed a series of numericaland quantum mechanical calculations to evaluate the plasmonic contributionto the activation of nitrogen on the TiB2 surface, indicatingan increase in the catalytic activity under the plasmon-generatedelectric field.
Permanent Link: https://hdl.handle.net/11104/0344687