School of Engineering, the University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.
Japan Technological Research Association of Artificial Photosynthetic Chemical Process, 2-11-9 Iwamotocho, Chiyoda-ku, Tokyo, 101-0032, Japan.
Angew Chem Int Ed Engl. 2017 Apr 18;56(17):4739-4743. doi: 10.1002/anie.201700117. Epub 2017 Mar 21.
Ta N is a very promising photocatalyst for solar water splitting because of its wide spectrum solar energy utilization up to 600 nm and suitable energy band position straddling the water splitting redox reactions. However, its development has long been impeded by poor compatibility with electrolytes. Herein, we demonstrate a simple sputtering-nitridation process to fabricate high-performance Ta N film photoanodes owing to successful synthesis of the vital TaO precursors. An effective GaN coating strategy is developed to remarkably stabilize Ta N by forming a crystalline nitride-on-nitride structure with an improved nitride/electrolyte interface. A stable, high photocurrent density of 8 mA cm was obtained with a CoPi/GaN/Ta N photoanode at 1.2 V under simulated sunlight, with O and H generated at a Faraday efficiency of unity over 12 h. Our vapor-phase deposition method can be used to fabricate high-performance (oxy)nitrides for practical photoelectrochemical applications.
TaN 是一种很有前途的光解水催化剂，因为它能利用宽光谱太阳能（600nm 以内），且其能带位置横跨水分解氧化还原反应，非常适合。然而，其发展长期以来一直受到与电解质兼容性差的阻碍。在此，我们通过简单的溅射氮化工艺制备了高性能 TaN 薄膜光阳极，因为成功合成了重要的 TaO 前驱体。开发了一种有效的 GaN 涂层策略，通过形成具有改进的氮化物/电解质界面的晶态氮化物-氮化物结构，显著稳定 TaN。在模拟太阳光下，CoPi/GaN/TaN 光阳极在 1.2V 时获得了稳定的、高达 8mA·cm 的高光电流密度，O 和 H 的法拉第效率超过 12 小时达到 100%。我们的气相沉积方法可用于制造用于实际光电化学应用的高性能（氧）氮化物。
