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A Benchmark Quantum Yield for Water Photoreduction on Amorphous Carbon Nitride

机译：非晶态氮化碳在水上光还原的基准量子产率

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摘要

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 approximate to 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 mu mol 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.
机译：非晶态氮化碳（a-CN）是一种较少开发但很有希望的用于制氢的光催化剂。尽管扩展了可见光吸收（​​EVLA），但用于水光还原的低量子效率（QE）是一个长期存在的问题。这意味着EVLA不能按比例转换为大量光生电子的收集。使光吸收和电荷收集之间的失配最小化仍然是科学挑战。此处报道了解决这种明显失配的a-CN的海绵状分层结构。结合的实验和时域有限差分仿真证明了a-CN海绵具有诱导散射的能力，以实现内部光全反射，从而促进了局部电荷载流子的产生。漫反射和瞬态荧光衰减研究表明，与海绵状a-CN相比，海绵状a-CN的光俘获增强了40％，电子寿命比模拟材料长约23倍，因此与模拟结果吻合良好。结果是在10体积％三乙醇胺和1重量％Pt助催化剂的反应体系中，制氢量为203.5μmol h（-1）的新高基准，在420 nm下的QE为6.1％。增强的水光还原是α-CN海绵内存在的光物理和电化学特性的结果。

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