journal article·2023-06-27Open access

Local Photochemical Nanoscopy of Hot-Carrier-Driven Catalytic Reactions Using Plasmonic Nanosystems

Olivier Henrotte, Eva Yazmin Santiago, Artur Movsesyan, Luca Mascaretti, Morteza Afshar, Alessandro Minguzzi, Alberto Vertova, Zhiming M. Wang, Radek Zbořil, Štěpán Kment, Alexander O. Govorov, Alberto Naldoni

ACS Nano· Volume 17· Issue 12

Abstract

Nanoscale investigation of the reactivity of photocatalytic systems is crucial for their fundamental understanding and improving their design and applicability. Here, we present a photochemical nanoscopy technique that unlocks the local spatial detection of molecular products during plasmonic hot-carrier-driven photocatalytic reactions with nanometric precision. By applying the methodology to Au/TiO 2 plasmonic photocatalysts, we experimentally and theoretically determined that smaller and denser Au nanoparticle arrays present lower optical contribution with quantum efficiency in hot-hole-driven photocatalysis closely related to the population heterogeneity. As expected, the highest quantum yield from a redox probe oxidation is achieved at the plasmon peak. Investigating a single plasmonic nanodiode, we unravel the areas where oxidation and reduction products are evolved with subwavelength resolution (∼200 nm), illustrating the bipolar behavior of such nanosystems. These results open the way to quantitative investigations at the nanoscale to evaluate the photocatalytic reactivity of low-dimensional materials in a variety of chemical reactions.
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Research context

OpenAlex topics: Gold and Silver Nanoparticles Synthesis and Applications · Copper-based nanomaterials and applications · Advanced Photocatalysis Techniques

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

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

Department of Physics and Astronomy, Nanoscale and Quantum Phenomena Institute, Ohio University, Athens, Ohio 45701, United States

Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China

Laboratory of Applied Electrochemistry, Dipartimento di Chimica, Università degli Studi di Milano, via Golgi 19, Milano 20133, Italy

Consorzio Interuniversitario Nazionale per la Scienza e Tecnologia dei Materiali, via Giusti 9, Firenze 50121, Italy

CEET, Nanotechnology Centre, VŠB-Technical University of Ostrava, 17. Listopadu 2172/15, Ostrava-Poruba 708 00, Czech Republic

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

Funding

Universit? degli Studi di Milano · National Key Research and Development Program of China · Ministero dell?Istruzione, dell?Universit? e della Ricerca · European Regional Development Fund · Ministerstvo ?kolstv?, Ml?de?e a Telov?chovy · Grantov? Agentura Cesk? Republiky · Ministero dell'Universit? e della Ricerca · Higher Education Discipline Innovation Project

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