Eine Plattform für die Wissenschaft: Bauingenieurwesen, Architektur und Urbanistik
Eine Plattform für die Wissenschaft: Bauingenieurwesen, Architektur und Urbanistik
Enhancing Photocatalysis: Understanding the Mechanistic Diversity in Photocatalysts Modified with Single‐Atom Catalytic Sites
Surface modification of heterogeneous photocatalysts with single‐atom catalysts (SACs) is an attractive approach for achieving enhanced photocatalytic performance. However, there is limited knowledge of the mechanism of photocatalytic enhancement in SAC‐modified photocatalysts, which makes the rational design of high‐performance SAC‐based photocatalysts challenging. Herein, a series of photocatalysts for the aerobic degradation of pollutants based on anatase TiO2 modified with various low‐cost, non‐noble SACs (vanadate, Cu, and Fe ions) is reported. The most active SAC‐modified photocatalysts outperform TiO2 modified with the corresponding metal oxide nanoparticles and state‐of‐the‐art benchmark photocatalysts such as platinized TiO2 and commercial P25 powders. A combination of in situ electron paramagnetic resonance spectroscopy and theoretical calculations reveal that the best‐performing photocatalysts modified with Cu(II) and vanadate SACs exhibit significant differences in the mechanism of activity enhancement, particularly with respect to the rate of oxygen reduction. The superior performance of vanadate SAC‐modified TiO2 is found to be related to the shallow character of the SAC‐induced intragap states, which allows for both the effective extraction of photogenerated electrons and fast catalytic turnover in the reduction of dioxygen, which translates directly into diminished recombination. These results provide essential guidelines for developing efficient SAC‐based photocatalysts.
Enhancing Photocatalysis: Understanding the Mechanistic Diversity in Photocatalysts Modified with Single‐Atom Catalytic Sites
Surface modification of heterogeneous photocatalysts with single‐atom catalysts (SACs) is an attractive approach for achieving enhanced photocatalytic performance. However, there is limited knowledge of the mechanism of photocatalytic enhancement in SAC‐modified photocatalysts, which makes the rational design of high‐performance SAC‐based photocatalysts challenging. Herein, a series of photocatalysts for the aerobic degradation of pollutants based on anatase TiO2 modified with various low‐cost, non‐noble SACs (vanadate, Cu, and Fe ions) is reported. The most active SAC‐modified photocatalysts outperform TiO2 modified with the corresponding metal oxide nanoparticles and state‐of‐the‐art benchmark photocatalysts such as platinized TiO2 and commercial P25 powders. A combination of in situ electron paramagnetic resonance spectroscopy and theoretical calculations reveal that the best‐performing photocatalysts modified with Cu(II) and vanadate SACs exhibit significant differences in the mechanism of activity enhancement, particularly with respect to the rate of oxygen reduction. The superior performance of vanadate SAC‐modified TiO2 is found to be related to the shallow character of the SAC‐induced intragap states, which allows for both the effective extraction of photogenerated electrons and fast catalytic turnover in the reduction of dioxygen, which translates directly into diminished recombination. These results provide essential guidelines for developing efficient SAC‐based photocatalysts.
Enhancing Photocatalysis: Understanding the Mechanistic Diversity in Photocatalysts Modified with Single‐Atom Catalytic Sites
Kruczała, Krzysztof (Autor:in) / Neubert, Susann (Autor:in) / Dhaka, Kapil (Autor:in) / Mitoraj, Dariusz (Autor:in) / Jánošíková, Petra (Autor:in) / Adler, Christiane (Autor:in) / Krivtsov, Igor (Autor:in) / Patzsch, Julia (Autor:in) / Bloh, Jonathan (Autor:in) / Biskupek, Johannes (Autor:in)
Advanced Science ; 10
01.12.2023
12 pages
Aufsatz (Zeitschrift)
Elektronische Ressource
Englisch
Homogeneity of Supported Single‐Atom Active Sites Boosting the Selective Catalytic Transformations
| Wiley | 2022
| American Chemical Society | 2022
Antenna Mechanism and De-Aggregation Concept: Novel Mechanistic Principles for Photocatalysis
| British Library Online Contents | 2007
Mechanistic understanding of bone
British Library Online Contents | 2003