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Hydrogen Generation from Water by Catalysts of Platinum-Based Clusters Pt3X (X = Al, Si, Cu) and CO Oxidation by Their Products
Zhen-Dong Sun1,2
1.Department of Physics, Shandong University, Jinan 250100, China;2.Department of Physics and Electrical Engineering, Kashi University, Kashgar 844006, China
Abstract:
Reducing sizes of precious metals and utilization of the mixed small clusters of them as catalysts in reactions are important methods due to more active sites for higher catalytic efficiency. Based on first-principles calculations in this work, we found that the platinum-based clusters of Pt3X (X = Al, Si, Cu) which have occurrence of the magic numbers can effectively catalyze the water decomposition and hydrogen production in just one-step reaction process. The adsorbate of the H2O@Pt3X clusters have strong absorption in the UV and visible regions with wavelength from 300 to 760 nm, indicating the sunlight can be used to drive catalytic hydrolysis for producing clean hydrogen. In addition, the O atom remains on the clusters after hydrolysis and can react with CO to form CO2 in activation barrier of 0.34 ~ 0.58 eV, showing the recycling ability of the products after hydrolysis for elimination the “poisoning” CO by oxidation. Moreover, the formed CO2 molecule can be detached from the Pt3X clusters at 323 K. Our results provide interesting guidance for practical designing the useful photocatalysts.
Key words:  H2O decomposition, H2 generation  elimination of CO  Pt-based clusters  photocatalyst
FundProject:
铂基团簇Pt3X (X = Al, Si, Cu) 催化水制氢及其水解产物氧化CO
Zhen-Dong Sun1,2
1.Department of Physics, Shandong University, Jinan 250100, China;2.Department of Physics and Electrical Engineering, Kashi University, Kashgar 844006, China
摘要:
降低贵金属的尺寸和利用掺杂的小团簇作为催化反应中的催化剂是提高催化效率的重要方法,因为其有更多的活性位点。本文基于第一性原理,我们研究了利用具有幻数结构特点的Pt3X (X = Al, Si, Cu) 团簇仅通过一步反应就能催化分解水制氢的反应过程。吸附物H2O@Pt3X 团簇在波长从300 -- 760 nm的紫外和可见光范围内有强吸收,表明太阳光可以方便地用于Pt3X的催化水解制氢的反应。此外,水解后滞留在团簇上的O原子可在反应活化能为0.34~0.58 eV内与CO氧化反应生成CO2。这个通过氧化消除“毒性” CO的结果表明了反应产物有能作催化剂的循环再利用能力。此外,我们发现生成的CO2分子还可以在323 K的温度下脱离Pt3X 小团簇。 我们的研究结果为实际中设计有用的光催化剂提供了有趣的指导。
关键词:  H2O decomposition, H2 generation  elimination of CO  Pt-based clusters  photocatalyst
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