Acta Phys. -Chim. Sin. ›› 2016, Vol. 32 ›› Issue (5): 1183-1190.doi: 10.3866/PKU.WHXB201603032

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Pt4 Clusters Supported on Monolayer Graphitic Carbon Nitride Sheets for Oxygen Adsorption: A First-Principles Study

Hui-Wen ZUO1,Chun-Hai LU2,Yu-Rong REN3,Yi LI1,Yong-Fan ZHANG1,Wen-Kai CHEN1,4,5,*()   

  1. 1 Department of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China
    2 College of Nuclear Technology and Automation Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China
    3 School of Marterials Science and Engineering, Changzhou University, Changzhou 213164, Jiangsu Province, P. R. China
    4 Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, Xiamen 361005, Fujian Province, P. R. China
    5 State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, P. R. China
  • Received:2015-11-30 Published:2016-05-07
  • Contact: Wen-Kai CHEN
  • Supported by:
    the National Natural Science Foundation of China(21203227);the National Natural Science Foundation of China(51574090)


The structural and electronic properties of Pt4 nanoparticles adsorbed on monolayer graphitic carbon nitride (Pt4/g-C3N4), as well as the adsorption behavior of oxygen molecules on the Pt4/g-C3N4 surface have been investigated through first-principles density-functional theory (DFT) calculations with the generalized gradient approximation (GGA). The interaction of the oxygen molecules with the bare g-C3N4 and the Pt4 clusters was also calculated for comparison. Our calculations show that Pt nanoparticles prefer to bond with four edge N atoms on heptazine phase g-C3N4 (HGCN) surfaces, forming two hexagonal rings. For s-triazine phase g-C3N4 (TGCN) surfaces, Pt nanoparticles prefer to sit atop the single vacancy site, forming three bonds with the nearest nitrogen atoms. Stronger hybridization of the Pt nanoparticles with the sp2 dangling bonds of neighboring nitrogen atoms leads to the Pt4 clusters strongly binding on both types of g-C3N4 surface. In addition, the results from Mulliken charge population analyses suggest that there are electrons flowing from the Pt clusters to g-C3N4. According to the comparative analyses of the O2 adsorbed on the Pt4/HGCN, Pt4/TGCN, and pure g-C3N4 systems, the presence of metal clusters promotes greater electron transfer to oxygen molecules and elongates the O―O bond. Meanwhile, its greater adsorbate-substrate distortion and large adsorption energy render the Pt4/HGCN system slightly superior to the Pt4/TGCN system in catalytic performance. The results validate that being supported on g-C3N4 may be a good way to modify the electronic structure of materials and their surface properties improve their catalytic performance.

Key words: Graphitic carbon nitride, Pt cluster, Oxygen molecule, Adsorption, Photocatalyst, Density functional theory


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