Advanced Functional Materials
Advanced Functional Materials
5 years ago

A Benchmark Quantum Yield for Water Photoreduction on Amorphous Carbon Nitride

A Benchmark Quantum Yield for Water Photoreduction on Amorphous Carbon Nitride
Mohammad Z. Rahman, Jillian Moffatt, Tak W. Kee, Ronald Smernik, Patrick C. Tapping, Nigel Spooner, Shi-Zhang Qiao, Kenneth Davey, Youhong Tang
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. Spongy amorphous carbon nitride (a-CN) has been developed and demonstrated for photocatalytic hydrogen production via water-splitting. Hydrogen production with a-CN has an apparent quantum efficiency of 6.1% under visible light irradiation (420 nm). This is a high benchmark for hydrogen production, superseding all previously reported a-CN photocatalysts.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/adfm.201702384

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