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Single Atoms in Photocatalysis: Low Loading Is Good Enough! AITranslate

Friedrich-Alexander-University of Erlangen-Nuremberg; University of Erlangen-Nuremberg; Friedrich-Alexander-University of Erlangen-Nuremberg; Friedrich-Alexander-University of Erlangen-Nuremberg; University of Erlangen-Nuremberg; University of Erlangen-Nuremberg; King Abdulaziz University
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Publisher: ACS
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Abstract AITranslate

We disperse Pt single atoms (SAs) with different loading densities on anatase TiO2 thin films and evaluate the photocatalytic H2 generation as a function of the incident light intensity. We show that under common illumination intensities (such as terrestrial solar illumination), a minuscule Pt SA loading of ∼105 atoms μm–2 (surface Pt content ∼0.1 at.%) is sufficient to achieve a maximized H2 production rate. This results in a maximum turnover frequency at a single Pt atom site of ∼300 H2 molecules s–1. For a vast majority of illumination conditions and a suitable surface configuration, it is not the density of co-catalytic sites that is rate-determining (a high loading is not needed!), but the charge carrier generation (and flux of photoelectrons to the co-catalytic centers) determines the overall reaction rate. This is in stark contrast to SA catalysis of classic chemical reactions where generally a maximum loading of reactive SA delivers a maximum activity.

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DOI:https://doi.org/10.1021/acsenergylett.2c02801

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Citation Information:

We disperse Pt single atoms (SAs) with different loading densities on anatase TiO2 thin films and evaluate the photocatalytic H2 generation as a function of the incident light intensity. We show that under common illumination intensities (such as terrestrial solar illumination), a minuscule Pt SA loading of ∼105 atoms μm–2 (surface Pt content ∼0.1 at.%) is sufficient to achieve a maximized H2 production rate. This results in a maximum turnover frequency at a single Pt atom site of ∼300 H2 molecules s–1. For a vast majority of illumination conditions and a suitable surface configuration, it is not the density of co-catalytic sites that is rate-determining (a high loading is not needed!), but the charge carrier generation (and flux of photoelectrons to the co-catalytic centers) determines the overall reaction rate. This is in stark contrast to SA catalysis of classic chemical reactions where generally a maximum loading of reactive SA delivers a maximum activity.

quote

GB/T 7714-2015 [1] Shanshan Qin, Johannes Will, Hyesung Kim, et al. ACS Energy Letters, 2023(8). DOI:10.1021/acsenergylett.2c02801.
MLA [1] Shanshan Qin, et al., ACS Energy Letters, no. 8, 2023, https://doi.org/10.1021/acsenergylett.2c02801.
APA [1] Shanshan Qin, Johannes Will, Hyesung Kim, Nikita Denisov, Simon Carl, Erdmann Spiecker, & Patrik Schmuki. (2023). ACS Energy Letters(8). https://doi.org/10.1021/acsenergylett.2c02801
IEEE [1] Shanshan Qin, Johannes Will, Hyesung Kim, Nikita Denisov, Simon Carl, Erdmann Spiecker, and Patrik Schmuki, ACS Energy Letters, no. 8, 2023, doi: 10.1021/acsenergylett.2c02801.