Oshima Takayoshi, Ichibha Tom, Oqmhula Kenji, Hibino Keisuke, Mogi Hiroto, Yamashita Shunsuke, Fujii Kotaro, Miseki Yugo, Hongo Kenta, Lu Daling, Maezono Ryo, Sayama Kazuhiro, Yashima Masatomo, Kimoto Koji, Kato Hideki, Kakihana Masato, Kageyama Hiroshi, Maeda Kazuhiko
Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan.
Japan Society for the Promotion of Science, Kojimachi Business Center Building, 5-3-1 Kojimachi, Chiyoda-ku, Tokyo, 102-0083, Japan.
Angew Chem Int Ed Engl. 2020 Jun 8;59(24):9736-9743. doi: 10.1002/anie.202002534. Epub 2020 Apr 2.
Undoped layered oxynitrides have not been considered as promising H -evolution photocatalysts because of the low chemical stability of oxynitrides in aqueous solution. Here, we demonstrate the synthesis of a new layered perovskite oxynitride, K LaTa O N, as an exceptional example of a water-tolerant photocatalyst for H evolution under visible light. The material underwent in-situ H /K exchange in aqueous solution while keeping its visible-light-absorption capability. Protonated K LaTa O N, modified with an Ir cocatalyst, exhibited excellent catalytic activity toward H evolution in the presence of I as an electron donor and under visible light; the activity was six times higher than Pt/ZrO /TaON, one of the best-performing oxynitride photocatalysts for H evolution. Overall water splitting was also achieved using the Ir-loaded, protonated K LaTa O N in combination with Cs-modified Pt/WO as an O evolution photocatalyst in the presence of an I /I shuttle redox couple.
由于氮氧化物在水溶液中的化学稳定性较低，未掺杂的层状氮氧化物未被视为有前景的析氢光催化剂。在此，我们展示了一种新型层状钙钛矿型氮氧化物KLaTaON的合成，它是一种在可见光下用于析氢的耐水光催化剂的杰出范例。该材料在水溶液中进行原位H/K交换，同时保持其可见光吸收能力。用Ir助催化剂改性的质子化KLaTaON在I作为电子供体且在可见光存在的情况下，对析氢表现出优异的催化活性；其活性比Pt/ZrO/TaON（性能最佳的用于析氢的氮氧化物光催化剂之一）高六倍。在I/I穿梭氧化还原对存在的情况下，使用负载Ir的质子化KLaTaON与Cs改性的Pt/WO作为析氧光催化剂相结合，也实现了整体水分解。
