Kong, D;
Han, X;
Xie, J;
Ruan, Q;
Windle, CD;
Gadipelli, S;
Shen, K;
... Tang, J; + view all
(2019)
Tunable Covalent Triazine-Based Frameworks (CTF-0) for Visible-Light-Driven Hydrogen and Oxygen Generation from Water Splitting.
ACS Catalysis
, 9
pp. 7697-7707.
10.1021/acscatal.9b02195.
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Abstract
Covalent triazine-based frameworks (CTFs), a group of semiconductive polymers, have been identified for photocatalytic water splitting recently. Their adjustable band gap and facile processing offer great potential for discovery and development. Here, we present a series of CTF-0 materials fabricated by two different approaches, a microwave-assisted synthesis and an ionothermal method, for water splitting driven by visible-light irradiation. The material (CTF-0-M2) synthesized by microwave technology shows a high photocatalytic activity for hydrogen evolution (up to 7010 μmol h−1 g−1 ), which is 7 times higher than another (CTF-0-I) prepared by conventional ionothermal trimerization under identical photocatalytic conditions. This leads to a high turnover number (TON) of 726 with respect to the platinum cocatalyst after seven cycles under visible light. We attribute this to the narrowed band gap, the most negative conduction band, and the rapid photogenerated charge separation and transfer. On the other hand, the material prepared by the ionothermal method is the most efficient one for oxygen evolution. CTF-0-I initially produces ca. 6 times greater volumes of oxygen gas than CTF-0-M2 under identical experimental conditions. CTF-0-I presents an apparent quantum efficiency (AQY) of 5.2% at 420 nm for oxygen production without any cocatalyst. The activity for water oxidation exceeds that of most reported CTFs due to a large driving force for oxidation and a large number of active sites. Our findings indicate that the band positions and the interlayer stacking structures of CTF-0 were modulated by varying synthesis conditions. These modulations impact the optical and redox properties, resulting in an enhanced performance for photocatalytic hydrogen and oxygen evolution, confirmed by firstprinciples calculations
| Type: | Article |
|---|---|
| Title: | Tunable Covalent Triazine-Based Frameworks (CTF-0) for Visible-Light-Driven Hydrogen and Oxygen Generation from Water Splitting |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acscatal.9b02195 |
| Publisher version: | https://doi.org/10.1021/acscatal.9b02195 |
| Language: | English |
| Additional information: | This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. https://creativecommons.org/licenses/by/4.0/ |
| Keywords: | covalent triazine-based frameworks, oxygen evolution, hydrogen evolution, visible-light-driven photocatalysis, water splitting |
| 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 UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Electronic and Electrical Eng UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10080372 |
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