TiO2锐钛矿上作为助催化剂的单铂原子的受控负载优化了光催化氢气的产生。,Advanced Materials

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TiO2锐钛矿上作为助催化剂的单铂原子的受控负载优化了光催化氢气的产生。
Advanced Materials ( IF 27.4 ) Pub Date : 2020-03-03 , DOI: 10.1002/adma.201908505
Seyedsina Hejazi ₁ , Shiva Mohajernia ₁ , Benedict Osuagwu ₁ , Giorgio Zoppellaro ₂ , Pavlina Andryskova ₂ , Ondrej Tomanec ₂ , Stepan Kment ₂ , Radek Zbořil ₂ , Patrik Schmuki _{1,

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Affiliation

由于许多催化反应的比活和选择性通常大大提高，因此单原子（SA）催化是催化领域的一个新领域。在这里，描述了一种原子尺度的缺陷工程方法，以形成和控制作为化学光催化氢气产生的助催化剂的铂SA位点的陷阱。溅射的TiO2薄层用作模型光催化剂，并与更常用的（001）锐钛矿片进行了比较。为了形成稳定的SA铂，在不同条件下（导致不同但确定的Ti3 + -Ov表面缺陷），在Ar / H2中还原TiO2层，然后将其浸入稀六氯铂酸溶液中。HAADF-STEM结果表明，只有在薄膜基板上，SA位点的密度才能通过退火的还原程度得到成功控制。与传统的铂纳米粒子修饰的TiO2表面相比，优化的SA-Pt装饰可以将TiO2溅射样品的归一化光催化活性提高150倍。HAADF-STEM，XPS和EPR研究共同证实了TiO2上装饰的Pt的原子性质。重要的是，可以精确地优化相关表面暴露缺陷中心的密度，从而在光催化活性中起关键作用的Pt-SA位点的密度。

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On the Controlled Loading of Single Platinum Atoms as a Co-Catalyst on TiO2 Anatase for Optimized Photocatalytic H2 Generation.

Single-atom (SA) catalysis is a novel frontline in the catalysis field due to the often drastically enhanced specific activity and selectivity of many catalytic reactions. Here, an atomic-scale defect engineering approach to form and control traps for platinum SA sites as co-catalyst for photocatalytic H2 generation is described. Thin sputtered TiO2 layers are used as a model photocatalyst, and compared to the more frequently used (001) anatase sheets. To form stable SA platinum, the TiO2 layers are reduced in Ar/H2 under different conditions (leading to different but defined Ti3+ -Ov surface defects), followed by immersion in a dilute hexachloroplatinic acid solution. HAADF-STEM results show that only on the thin-film substrate can the density of SA sites be successfully controlled by the degree of reduction by annealing. An optimized SA-Pt decoration can enhance the normalized photocatalytic activity of a TiO2 sputtered sample by 150 times in comparison to a conventional platinum-nanoparticle-decorated TiO2 surface. HAADF-STEM, XPS, and EPR investigation jointly confirm the atomic nature of the decorated Pt on TiO2 . Importantly, the density of the relevant surface exposed defect centers-thus the density of Pt-SA sites, which play the key role in photocatalytic activity-can be precisely optimized.

更新日期：2020-04-21

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