Shen, R;
Li, N;
Qin, C;
Li, X;
Zhang, P;
Li, X;
Tang, J;
(2023)
Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution.
Advanced Functional Materials
, 33
(34)
, Article 2301463. 10.1002/adfm.202301463.
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Abstract
Covalent triazine frameworks (CTF) offer a tunable platform for photocatalytic H2 generation due to their diverse structures, low costs, and precisely tunable electronic structures. However, high exciton binding energy and short lifetimes of photogenerated carriers restrict their application in photocatalytic hydrogen evolution. Herein, a novel phosphorus-incorporated CTF is introduced to construct a chemically bonded PCTF/WO3 (PCTFW) heterostructure with a precise interface electron transfer channel. The phosphorus incorporation is found to dominantly reduce the exciton binding energy and promote the dissociation of singlet and triplet excitons into free charge carriers due to the regulation of electronic structures. High-quality interfacial W-N bonds improve the interfacial transfer of photogenerated electrons, thus prolonging the lifetime of photogenerated electrons. Femtosecond transient absorption spectroscopy characterizations and DFT calculations further confirm both phosphorus incorporation and Z-scheme heterojunctions can synergistically boost the in-built electric field and accelerate the migration and separation of photogenerated electrons. The optimized photocatalytic H2-evolution rate of resultant PCTFW is 134.84 µmol h−1 (67.42 mmol h−1g−1), with an apparent quantum efficiency of 37.63% at 420 nm, surpassing many reported CTF-based photocatalysts so far. This work highlights the significance of atom-level interfacial exciton dissociation, and charge transfer and separation in improving photocatalysis.
| Type: | Article |
|---|---|
| Title: | Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/adfm.202301463 |
| Publisher version: | https://doi.org/10.1002/adfm.202301463 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | charge separation, exciton dissociation, phosphorus-incorporated covalent triazine frameworks, photocatalytic hydrogen evolution, Z-scheme heterojunctions |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10171156 |
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