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Atomically Engineered Active Sites for Photocatalytic Hydrogen Evolution Reaction

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 SEMINARThe State Key Lab ofHigh Performance Ceramics and Superfine MicrostructureShanghai Institute of Ceramics, Chinese Academy of Sciences

  中 国 科 学 院 上 海 硅 酸 盐 研 究 所 高 性 能 陶 瓷 和 超 微 结 构 国 家 重 点 实 验 室 

  Atomically Engineered Active Sites for Photocatalytic Hydrogen Evolution Reaction 

  Speaker 

  杨化桂 教授 

  华东理工大学 

  时间:2015年11月24日(星期二)下午 14: 00 

  地点: 2号楼607会议室 (国家重点实验室) 

  欢迎广大科研人员和研究生参与讨论! 

  联系人:施剑林(2712),步文博(2610) 

   

  Abstract: 

  The growing energy crisis and environmental issues are driving the development of clean and sustainable energy sources. In particular, solar energy as one of the best sources of renewable energy has attracted significant attention as a promising way to solve these problems. Herein, we studied various atomically engineered catalytic materials to enhance the solar-driven water splitting. First of all, using polymer ligands to control the size and valence state of platinum monoxide clusters, we found that Pt in a higher oxidation has remarkable hydrogen oxidation reaction suppression ability, while its H2 evolution capacity is still comparable to that of the benchmark of conventional Pt cocatalyst.[1] Moreover, we explored the active sites of Pt/TiO2 photocatalyst on atomic level by a collaborative analysis from both experimental and theoretical work; metallic Pt0 nanoparticles have little contribution to the activity of solar water splitting and by contrast, oxidized species Ptδ+ truly take the role of the catalytic active sites.[2] In addition, we designed and synthesized a surface H-bonding network decorated g-C3N4 photocatalyst with high efficiency of visible-light-driven H2 production. According to NMR and theoretical modeling, the H-bonding bridge can effectively shorten the distance between water molecules and g-C3N4, provide multiple channels for the transition between protons and the excited electrons on g-C3N4, stabilize the anionic intermediate and transition states, and restrain charge recombination.[3] Furthermore, we anchored isolated Pt atoms on TiO2 and this photocatalyst exhibits a high solar-driven hydrogen evolution performance compared with Pt nanoparticles or clusters. The configurations of the isolated Pt atoms and their catalytic hydrogen evolution activity were calculated by large-scale periodic DFT analysis.[4] Additionally, we found that the photoreactivity of hydrogen generation can be correlated with the cluster size of the oxidized platinum cocatalyst as function, and the maximum turnover frequency is found on the smallest-sized cocatalyst.[5] These results would open a door for rethinking of the detailed principles of photocatalysis, and may also stimulate novel ideas for the design and optimization of heterogeneous photocatalysts. 

  References: 

  1. Y. H. Li, J. X., Z. J. Chen, Z. Li, F. Tian, H. G. Yang*,  Nature Commun., 2013, 4, 2500. 
  2. J. Xing, H. B. Jiang, J. F. Chen, Y. H. Li, H. G. Yang*,  J. Mater. Chem. A, 2013, 1, 15258. (Cover story) 
  3. X. L. Wang, W. Q. Fang, H. F. Wang, H. G. Yang*,  J. Mater. Chem. A, 2013, 1, 14089. (Cover story) 
  4. J. Xing, J. F. Chen, Y. H. Li, W. T. Yuan, H. G. Yang*, Chem. Eur. J., 2014, 20, 2138. (Cover story) 
  5. Y. H. Li, J. X., X. H. Yang, H. G. Yang*,  Chem. Eur. J., 2014, 20, 12377. 
 
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