Two-Dimensional Perovskite Oxynitride K2 LaTa2 O6 N with an H+ /K+ Exchangeability in Aqueous Solution Forming a Stable Photocatalyst for Visible-Light H2 Evolution.,Angewandte Chemie International Edition

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Two-Dimensional Perovskite Oxynitride K2 LaTa2 O6 N with an H+ /K+ Exchangeability in Aqueous Solution Forming a Stable Photocatalyst for Visible-Light H2 Evolution.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-03-05 , DOI: 10.1002/anie.202002534
Takayoshi Oshima _{1,

2} , Tom Ichibha ₃ , Kenji Oqmhula ₃ , Keisuke Hibino ₁ , Hiroto Mogi ₁ , Shunsuke Yamashita ₄ , Kotaro Fujii ₁ , Yugo Miseki ₅ , Kenta Hongo _{6,

7,

8,

9} , Daling Lu ₁₀ , Ryo Maezono ₃ , Kazuhiro Sayama ₅ , Masatomo Yashima ₁ , Koji Kimoto ₄ , Hideki Kato ₁₁ , Masato Kakihana ₁₁ , Hiroshi Kageyama ₁₂ , Kazuhiko Maeda ₁

Affiliation

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.
School of Information Science, JAIST, Asahidai 1-1, Nomi, Ishikawa, 923-1292, Japan.
Research Center for Advanced Measurement and Characterization, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
Research Center for Photovoltaics (RCPV) and Global Zero Emission Research Center (GZR), National Institute of Advanced Industrial Science and Technology (AIST), Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki, 305-8565, Japan.
Research Center for Advanced Computing Infrastructure, JAIST, Asahidai 1-1, Nomi, Ishikawa, 923-1292, Japan.
Center for Materials Research by Information Integration, Research and Services Division of Materials Data and Integrated System, National Institute for Materials Science, Tsukuba, 305-0047, Japan.
PRESTO, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi-shi, Saitama, 322-0012, Japan.
Computational Engineering Applications Unit, RIKEN, 2-1 Hirosawa, Wako, Saitama, 351-0198, Japan.
Suzukakedai Materials Analysis Division, Technical Department, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan.
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, 980-8577, Japan.
Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto, 615-8510, Japan.

Undoped layered oxynitrides have not been considered as promising H₂‐evolution photocatalysts because of the low chemical stability of oxynitrides in aqueous solution. Here, we demonstrate the synthesis of a new layered perovskite oxynitride, K₂LaTa₂O₆N, as an exceptional example of a water‐tolerant photocatalyst for H₂ evolution under visible light. The material underwent in‐situ H⁺/K⁺ exchange in aqueous solution while keeping its visible‐light‐absorption capability. Protonated K₂LaTa₂O₆N, modified with an Ir cocatalyst, exhibited excellent catalytic activity toward H₂ evolution in the presence of I⁻ as an electron donor and under visible light; the activity was six times higher than Pt/ZrO₂/TaON, one of the best‐performing oxynitride photocatalysts for H₂ evolution. Overall water splitting was also achieved using the Ir‐loaded, protonated K₂LaTa₂O₆N in combination with Cs‐modified Pt/WO₃ as an O₂ evolution photocatalyst in the presence of an I₃⁻/I⁻ shuttle redox couple.

中文翻译：

在水溶液中具有H + / K +交换性的二维钙钛矿型氧氮化物K2 LaTa2 O6 N，形成稳定的可见光H2释放光催化剂。

由于在水溶液中氮氧化物的化学稳定性低，因此未掺杂的层状氮氧化物尚未被视为有前途的H ₂演化光催化剂。在这里，我们展示了一种新的层状钙钛矿型氧氮化物K ₂ LaTa ₂ O ₆ N的合成，作为在可见光下H ₂析出的耐水光催化剂的一个例外实例。该物质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K ₂ LaTa ₂ O ₆ N对H表现出优异的催化活性₂演化的我的存在^-作为电子供体，并在可见光; 该活性是Pt / ZrO ₂ / TaON的六倍，Pt / ZrO ₂ / TaON是表现出H ₂释放性能最好的氧氮化物光催化剂之一。使用也实现整体水分解的Ir-加载，质子化ķ ₂ LATA ₂ ö ₆中的N结合铯改性的Pt / WO ₃为O ₂中的I存在进化光催化剂₃^- / I ^-穿梭氧化还原电。

更新日期：2020-03-05

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