Citation: ZUO Hui-Wen, LU Chun-Hai, REN Yu-Rong, LI Yi, ZHANG Yong-Fan, CHEN Wen-Kai. Pt₄ Clusters Supported on Monolayer Graphitic Carbon Nitride Sheets for Oxygen Adsorption: A First-Principles Study[J]. Acta Physico-Chimica Sinica, ;2016, 32(5): 1183-1190. doi: 10.3866/PKU.WHXB201603032 shu

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

ZUO Hui-Wen ¹ ,
LU Chun-Hai ² ,
REN Yu-Rong ³ ,
LI Yi ¹ ,
ZHANG Yong-Fan ¹ ,
CHEN Wen-Kai ^1,4,5,,

1.
1 Department of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China;
2.
2 College of Nuclear Technology and Automation Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China;
3.
3 School of Marterials Science and Engineering, Changzhou University, Changzhou 213164, Jiangsu Province, P. R. China;
4.
4 Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, Xiamen 361005, Fujian Province, P. R. China;
5.
5 State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, P. R. China

Corresponding author: CHEN Wen-Kai,
Received Date: 30 November 2015
Available Online: 1 March 2016
Fund Project: 国家自然科学基金(21203227,51574090)资助项目 (21203227,51574090)

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.
- Graphitic carbon nitride,
- Pt cluster,
- Oxygen molecule,
- Adsorption,
- Photocatalyst,
- Density functional theory
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Pt4 Clusters Supported on Monolayer Graphitic Carbon Nitride Sheets for Oxygen Adsorption: A First-Principles Study

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