Please use this identifier to cite or link to this item:
https://hdl.handle.net/2440/109268
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Type: | Journal article |
Title: | A benchmark quantum yield for water photoreduction on amorphous carbon nitride |
Author: | Rahman, M. Tapping, P. Kee, T. Smernik, R. Spooner, N. Moffatt, J. Tang, Y. Davey, K. Qiao, S. |
Citation: | Advanced Functional Materials, 2017; 27(39):1702384-1-1702384-11 |
Publisher: | John Wiley & Sons |
Issue Date: | 2017 |
ISSN: | 1616-301X 1616-3028 |
Statement of Responsibility: | Mohammad Z. Rahman, Patrick C. Tapping, Tak W. Kee, Ronald Smernik, Nigel Spooner, Jillian Moffatt, Youhong Tang, Kenneth Davey, and Shi-Zhang Qiao |
Abstract: | Amorphous carbon nitride (a-CN) is a less-explored but promising photocatalyst for hydrogen production. Despite an extended visible light absorption (EVLA) its low quantum efficiency (QE) for water photoreduction is a long standing problem. This implies that EVLA is not proportionally translated into collection of large amounts of photogenerated electrons. Minimizing the mismatch between light-absorption and charge-collection remains a scientific challenge. Here a sponge-like hierarchical structure of a-CN that addresses this apparent mismatch is reported. Combined experimental and finite difference time domain simulations demonstrate the ability of the a-CN sponge to induce scattering for total internal light reflection that promotes localized charge carrier generation. Diffused reflectance and transient fluorescence decay studies show good agreement with simulations with a 40% enhanced light-trapping and an ≈23 times longer electron lifetime in spongy a-CN compared with that of the bulk material. The result is a new high benchmark for hydrogen production of 203.5 µmol h⁻¹ with a QE of 6.1% at 420 nm in a reaction system of 10 vol% triethanolamine and 1 wt% Pt cocatalyst. The enhanced water photoreduction is a result of amenable photophysical and electrochemical attributes existing within the a-CN sponge. |
Keywords: | a-CN; carbon nitride sponge; hydrogen production; photocatalysis; water photoreduction |
Description: | Published online: August 14, 2017 |
Rights: | © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim |
DOI: | 10.1002/adfm.201702384 |
Grant ID: | http://purl.org/au-research/grants/arc/DP140104062 http://purl.org/au-research/grants/arc/DP160104866 http://purl.org/au-research/grants/arc/DP170104464 |
Published version: | http://dx.doi.org/10.1002/adfm.201702384 |
Appears in Collections: | Aurora harvest 3 Chemistry publications |
Files in This Item:
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hdl_109268.pdf | Submitted version | 1.18 MB | Adobe PDF | View/Open |
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