Non Thermal‐Driven Photocatalytic Ammonia Decomposition at Near‐Room Temperature on a Plasmonic Nanocone Array

Abstract The efficient and sustainable production of hydrogen is crucial for the transition to a clean energy future. Ammonia (NH 3 ) is an attractive hydrogen carrier due to its high energy density and safe storage properties. However, conventional ammonia decomposition requires high temperatures, making the process energy‐intensive and costly. Here, a plasmon‐driven photocatalytic approach is presented for ammonia cracking at near‐room temperature, utilizing a plasmonic antenna‐reactor system made by a sharp tip anodic alumina oxide (AAO) array coated with a plasmonic Au film (antenna), decorated with Cu nanoparticles (reactors). This nanostructured catalyst harnesses surface plasmon resonances (SPRs) and generates hot carriers under visible light illumination, significantly enhancing the reaction efficiency. The best AAO@Au@Cu configuration exhibited a hydrogen evolution rate of 227 µmol h −1 g Cu −1 under 1 Sun irradiation at 35 °C. The enhanced activity is due to plasmonic non thermal effects, with the highest catalytic activity observed at 565 nm, corresponding to the SPR mode of the nanostructure. Mechanistic insights, supported by XPS, TOF‐SIMS, and spin‐polarized density functional theory calculations, suggested a multi‐step NH 3 decomposition pathway involving NH 2 NH 2 (hydrazine) and NH‐NH intermediates. This study highlights the potential of plasmonic nanomaterials in revolutionizing low‐temperature NH 3 decomposition, paving the way for sustainable hydrogen production at solar intensities.

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Publication Details

Journal
Advanced Functional Materials
Published
2025-10-16
DOI
https://doi.org/10.1002/adfm.202505216
Citations
1
Primary Topic
Advanced Photocatalysis Techniques
Type
article
Field-Weighted Citation Impact
0.36

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article

Non Thermal‐Driven Photocatalytic Ammonia Decomposition at Near‐Room Temperature on a Plasmonic Nanocone Array

Olivier Henrotte, Luca Mascaretti, Tiziano Montini, T. P. Bui et al.
1 citations
Advanced Functional Materials
Advanced Photocatalysis Techniques
0.36
article

Non Thermal‐Driven Photocatalytic Ammonia Decomposition at Near‐Room Temperature on a Plasmonic Nanocone Array

Olivier Henrotte, Luca Mascaretti, Tiziano Montini, T. P. Bui, Piotr Błoński, Matteo Bisetto, Michal Otyepka, Radek Zbořil, Paolo Fornasiero, Stephen Sanders, Andrea Schirato, Seyedsina Hejazi, Alessandro Alabastri, Hana Kmentová, Štěpán Kment, Jan Navrátil, Petr Bábor, Alberto Naldoni
article en
1 citations

Abstract

Abstract The efficient and sustainable production of hydrogen is crucial for the transition to a clean energy future. Ammonia (NH 3 ) is an attractive hydrogen carrier due to its high energy density and safe storage properties. However, conventional ammonia decomposition requires high temperatures, making the process energy‐intensive and costly. Here, a plasmon‐driven photocatalytic approach is presented for ammonia cracking at near‐room temperature, utilizing a plasmonic antenna‐reactor system made by a sharp tip anodic alumina oxide (AAO) array coated with a plasmonic Au film (antenna), decorated with Cu nanoparticles (reactors). This nanostructured catalyst harnesses surface plasmon resonances (SPRs) and generates hot carriers under visible light illumination, significantly enhancing the reaction efficiency. The best AAO@Au@Cu configuration exhibited a hydrogen evolution rate of 227 µmol h −1 g Cu −1 under 1 Sun irradiation at 35 °C. The enhanced activity is due to plasmonic non thermal effects, with the highest catalytic activity observed at 565 nm, corresponding to the SPR mode of the nanostructure. Mechanistic insights, supported by XPS, TOF‐SIMS, and spin‐polarized density functional theory calculations, suggested a multi‐step NH 3 decomposition pathway involving NH 2 NH 2 (hydrazine) and NH‐NH intermediates. This study highlights the potential of plasmonic nanomaterials in revolutionizing low‐temperature NH 3 decomposition, paving the way for sustainable hydrogen production at solar intensities.

Advanced Functional MaterialsVol. 36(21)
United States Department of the Army (US), Central European Institute of Technology (CZ), VSB - Technical University of Ostrava (CZ), University of Trieste (IT), NeoPhotonics (United States) (US), United States Army (US), Regional Centre of Advanced Technologies and Materials (CZ), Czech Technical University in Prague (CZ), University of Turin (IT), Brno University of Technology (CZ), Palacký University Olomouc (CZ), Rice University (US), Politecnico di Milano (IT)
National Science Foundation, Dipartimenti di Eccellenza, European Commission, Ministerstvo Školství, Mládeže a Tělovýchovy, Ministero dell’Istruzione, dell’Università e della Ricerca, Central European Institute of Technology, Univerzita Palackého v Olomouci, Ministero dell'Università e della Ricerca, HORIZON EUROPE Framework Programme
Openalex Percentile: Top 37%
Advanced Photocatalysis Techniques
0.36
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