A Cocatalyst that Stabilizes a Hydride Intermediate during Photocatalytic Hydrogen Evolution over a Rhodium‐Doped TiO2 Nanosheet,Angewandte Chemie International Edition

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A Cocatalyst that Stabilizes a Hydride Intermediate during Photocatalytic Hydrogen Evolution over a Rhodium‐Doped TiO2 Nanosheet
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-06-19 , DOI: 10.1002/anie.201803214
Shintaro Ida _{1,

2} , Kenta Sato ₂ , Tetsuya Nagata ₁ , Hidehisa Hagiwara _{2,

3} , Motonori Watanabe ₃ , Namhoon Kim ₄ , Yoshihito Shiota ₅ , Michio Koinuma ₁ , Sakae Takenaka ₆ , Takaaki Sakai ₂ , Elif Ertekin _{3,

4} , Tatsumi Ishihara _{2,

3}

Affiliation

The hydrogen evolution reaction using semiconductor photocatalysts has been significantly improved by cocatalyst loading. However, there are still many speculations regarding the actual role of the cocatalyst. Now a photocatalytic hydrogen evolution reaction pathway is reported on a cocatalyst site using TiO₂ nanosheets doped with Rh at Ti sites as one‐atom cocatalysts. A hydride species adsorbed on the one‐atom Rh dopant cocatalyst site was confirmed experimentally as the intermediate state for hydrogen evolution, which was consistent with the results of density functional theory (DFT) calculations. In this system, the role of the cocatalyst in photocatalytic hydrogen evolution is related to the withdrawal of photo‐excited electrons and stabilization of the hydride intermediate species; the presence of oxygen vacancies induced by Rh facilitate the withdrawal of electrons and stabilization of the hydride.

中文翻译：

铑掺杂的TiO2纳米片在光催化氢释放过程中稳定氢化物中间体的助催化剂

通过负载助催化剂，使用半导体光催化剂的制氢反应已得到显着改善。然而，关于助催化剂的实际作用仍然有许多推测。现在报道了使用TiO ₂在助催化剂位点上的光催化氢释放反应途径在Ti部位掺杂Rh的纳米片作为单原子助催化剂。实验证明，吸附在单原子Rh掺杂剂助催化剂位点上的氢化物是氢释放的中间状态，这与密度泛函理论（DFT）计算的结果一致。在该系统中，助催化剂在光催化氢逸出中的作用与光激发电子的撤出和氢化物中间体的稳定有关。Rh引起的氧空位的存在有助于电子的撤出和氢化物的稳定。

更新日期：2018-06-19

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