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利用半导体纳米晶体和镍催化剂在水中生成稳定的氢气。

Robust photogeneration of H2 in water using semiconductor nanocrystals and a nickel catalyst.

机构信息

Department of Chemistry, University of Rochester, Rochester, NY 14627, USA.

出版信息

Science. 2012 Dec 7;338(6112):1321-4. doi: 10.1126/science.1227775. Epub 2012 Nov 8.

Abstract

Homogeneous systems for light-driven reduction of protons to H(2) typically suffer from short lifetimes because of decomposition of the light-absorbing molecule. We report a robust and highly active system for solar hydrogen generation in water that uses CdSe nanocrystals capped with dihydrolipoic acid (DHLA) as the light absorber and a soluble Ni(2+)-DHLA catalyst for proton reduction with ascorbic acid as an electron donor at pH = 4.5, which gives >600,000 turnovers. Under appropriate conditions, the precious-metal-free system has undiminished activity for at least 360 hours under illumination at 520 nanometers and achieves quantum yields in water of over 36%.

摘要

用于光驱动质子还原为 H(2)的均相系统通常由于光吸收分子的分解而寿命较短。我们报告了一种在水中利用 CdSe 纳米晶体作为光吸收体和可溶 Ni(2+)-DHLA 催化剂,以抗坏血酸作为电子供体,在 pH = 4.5 下进行太阳能制氢的稳健且高效的系统,其产氢量超过 600,000 次循环。在适当的条件下,在 520 纳米光照下,该无贵金属系统至少 360 小时保持活性,并在水中实现超过 36%的量子产率。

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