- Title
- Improved carrier dynamics in nickel/urea-functionalized carbon nitride for ethanol photoreforming
- Creator
- Gunawan, Denny; Toe, Cui Ying; Sun, Kaiwen; Scott, Jason; Amal, Rose
- Relation
- Photochemical & Photobiological Sciences Vol. 21, p. 2115-2126
- Publisher Link
- http://dx.doi.org/10.1007/s43630-022-00282-4
- Publisher
- Springer
- Resource Type
- journal article
- Date
- 2022
- Description
- Photoreforming has been shown to accelerate the H2 evolution rate compared to water splitting due to thermodynamically favorable organic oxidation. In addition, the potential to simultaneously produce solar fuel and value-added chemicals is a significant benefit of photoreforming. To achieve an efficient and economically viable photoreforming process, the selection and design of an appropriate photocatalyst is essential. Carbon nitride is promising as a metal-free photocatalyst with visible light activity, high stability, and low fabrication cost. However, it typically exhibits poor photogenerated charge carrier dynamics, thereby resulting in low photocatalytic performance. Herein, we demonstrate improved carrier dynamics in urea-functionalized carbon nitride with in situ photodeposited Ni cocatalyst (Ni/Urea-CN) for ethanol photoreforming. In the presence of 1 mM Ni2+ precursor, an H2 evolution rate of 760.5 µmol h−1 g−1 and an acetaldehyde production rate of 888.2 µmol h−1 g−1 were obtained for Ni/Urea-CN. The enhanced activity is ascribed to the significantly improved carrier dynamics in Urea-CN. The ability of oxygen moieties in the urea group to attract electrons and to increase the hole mobility via a positive shift in the valence band promotes an improvement in the overall carrier dynamics. In addition, high crystallinity and specific surface area of the Urea-CN contributed to accelerating charge separation and transfer. As a result, the electrons were efficiently transferred from Urea-CN to the Ni cocatalyst for H2 evolution while the holes were consumed during ethanol oxidation. The work demonstrates a means by which carrier dynamics can be tuned by engineering carbon nitride via edge functionalization.
- Subject
- carbon nitride; nickel cocatalyst; urea; photoreforming; ethanol; SDG 7; Sustainable Development Goals
- Identifier
- http://hdl.handle.net/1959.13/1480854
- Identifier
- uon:50576
- Identifier
- ISSN:1474-905X
- Rights
- © The Author(s) 2022. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
- Language
- eng
- Full Text
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