Sun Rulin, Wang Ruimin, Liu Xinlu, Chen Xiao, Che Li, Fan Hongjun, Yang Xueming, Guo Qing
College of Environmental Sciences and Engineering, Dalian Maritime University, Dalian, Liaoning 116026, P.R. China.
State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, P.R. China.
J Phys Chem Lett. 2022 Apr 14;13(14):3182-3187. doi: 10.1021/acs.jpclett.2c00234. Epub 2022 Apr 1.
Understanding the mechanism of hydrogen (H) formation from the conversion of water (HO) and renewables on TiO surfaces with cocatalysts via either photocatalysis or other catalytic processes is of significant importance to the successful design of efficient catalysts. Herein, we have investigated H production from HO, CHOH, and CHOH on a Pt cluster covered rutile (R)-TiO(110) surface (Pt/R-TiO(110)) to address the mechanism of H production. Experimental results demonstrate that surface adsorbates not only help H atom diffusion on Pt/R-TiO(110) but also take part in H production directly. Further density functional theory (DFT) calculations suggest that H production on Pt/R-TiO(110) occurs via a synergistic catalysis process between Pt clusters and interfacial adsorbates rather than a recombination reaction of H atoms on Pt clusters. This work provides new insight into H production from HO and renewables with Pt/TiO catalysts, which may be applicable to H production on other Pt cluster deposited metal oxide catalysts.
了解通过光催化或其他催化过程在含助催化剂的TiO表面上由水（H₂O）和可再生能源转化形成氢气（H₂）的机制，对于成功设计高效催化剂具有重要意义。在此，我们研究了在Pt团簇覆盖的金红石（R）-TiO(110)表面（Pt/R-TiO(110)）上由H₂O、CH₃OH和C₂H₅OH产生H₂的过程，以阐明H₂产生的机制。实验结果表明，表面吸附物不仅有助于H原子在Pt/R-TiO(110)上扩散，还直接参与H₂的产生。进一步的密度泛函理论（DFT）计算表明，Pt/R-TiO(110)上的H₂产生是通过Pt团簇与界面吸附物之间的协同催化过程，而不是Pt团簇上H原子的复合反应。这项工作为使用Pt/TiO催化剂从H₂O和可再生能源中产生H₂提供了新的见解，这可能适用于其他沉积有Pt团簇的金属氧化物催化剂上的H₂产生。
