Selective Preference of Pt Atoms on Covalent Triazine Frameworks in CO2 Photoreduction: Insight into Energy Transfer Mechanisms DOI
Shasha Liu, Chao Zhu, Chao Xu

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5694 - 5705

Published: March 24, 2025

Metal-loaded COF-based photocatalysts facilitate the conversion of CO2 and H2O into storable fuels through a photosynthesis-like mechanism, providing an efficient approach to addressing energy challenges. However, fundamental principles governing internal transfer reaction pathways remain insufficiently understood, posing significant barriers achieving photocatalytic reactions with high selectivity specificity. This study explores heavy-atom effect Pt on exciton-mediated by synthesizing single-atom dispersed PtSA-CTF nanoparticle-aggregated PtNP-CTF defective CTF substrates, thereby revealing selective preferences species their impact pathways. By combining exciton behavior characterization (fs-TA), photoreaction pathway validation (13CO2 isotope labeling) excited-state theoretical calculations (TD-DFT), it was demonstrated that excitons in undergo resonance intermediate during relaxation process from triplet state ground state. The *CO2 then reacts sequentially generated electrons protons, resulting performance CO yield 6.778 mmol·g–1·h–1, 98.2% selectivity, TOF 1102.68 h–1. work provides valuable insights photophysical properties induced excitonic effects, offering guidance for improving efficiency rational design advanced photocatalysts.

Language: Английский

Selective Preference of Pt Atoms on Covalent Triazine Frameworks in CO2 Photoreduction: Insight into Energy Transfer Mechanisms DOI
Shasha Liu, Chao Zhu, Chao Xu

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5694 - 5705

Published: March 24, 2025

Metal-loaded COF-based photocatalysts facilitate the conversion of CO2 and H2O into storable fuels through a photosynthesis-like mechanism, providing an efficient approach to addressing energy challenges. However, fundamental principles governing internal transfer reaction pathways remain insufficiently understood, posing significant barriers achieving photocatalytic reactions with high selectivity specificity. This study explores heavy-atom effect Pt on exciton-mediated by synthesizing single-atom dispersed PtSA-CTF nanoparticle-aggregated PtNP-CTF defective CTF substrates, thereby revealing selective preferences species their impact pathways. By combining exciton behavior characterization (fs-TA), photoreaction pathway validation (13CO2 isotope labeling) excited-state theoretical calculations (TD-DFT), it was demonstrated that excitons in undergo resonance intermediate during relaxation process from triplet state ground state. The *CO2 then reacts sequentially generated electrons protons, resulting performance CO yield 6.778 mmol·g–1·h–1, 98.2% selectivity, TOF 1102.68 h–1. work provides valuable insights photophysical properties induced excitonic effects, offering guidance for improving efficiency rational design advanced photocatalysts.

Language: Английский

Citations

0