Journal
ACS CATALYSIS
Volume 12, Issue 15, Pages 9114-9124Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02447
Keywords
epitaxial heterojunction; single-particle spectroscopy; charge transfer; FLIM; crystal facet
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Funding
- National Natural Science Foundation of China [22072072]
- National Key Research and Development Program of China [2020YFA0710301]
- Natural Science Foundation of Shandong Province [ZR2021JQ06]
- Shandong University Multidisciplinary Research and Innovation Team of Young Scholars [2020QNQT11, 2020QNQT012]
- Qilu Young Scholars and Outstanding Young Scholars Projects of Shandong University
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This study presents a strategy for synthesizing SrTiO3/TiO2 epitaxial heterojunctions and investigates the charge transfer process using single-particle spectroscopy. The results demonstrate that the epitaxial heterointerface promotes charge separation and suppresses photoluminescence lifetime decay. This research provides a new strategy for rational designing heterojunction photocatalysts and in-depth monitoring of the structure-activity relationship at the single-particle level.
Selectively constructing heterojunctions on specific crystal facets enable directional electron-hole migration and favorable charge separation. Meanwhile, in-depth monitoring and investigating charge-transfer process on specific crystal facets of individual single crystal are particularly important. Herein, we report a strategy for synthesizing SrTiO3/TiO2 epitaxial heterojunctions (ST/T), in which highly ordered SrTiO3 mesocrystals are selectively topologically grown on the TiO2 {001} facet. It exhibits good photocatalytic activity for tetracycline (TC) degradation. Notably, single-particle spectroscopy was employed to accurately monitor the transfer and recombination of carriers at the specific nanoregions of individual particle. The weaker photoluminescence (PL) intensity and longer lifetime at the epitaxial central site of ST/T particle indicate that the epitaxial heterointerface promotes the separation of charge carriers. Moreover, in situ monitoring of TC degradation on single ST/T particle confirms that the epitaxial heterojunction suppressed the PL lifetime decay, further demonstrating the pivotal role of site-selective topotactic epitaxy. This study presents a strategy for rational designing heterojunction photocatalysts and is beneficial for in-depth monitoring and understanding the structure-activity relationship at the single-particle level.
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