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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2016,Vol.32>> Issue(8)>> 2059-2068     doi: 10.3866/PKU.WHXB201604225         中文摘要
FT-IR, XPS and DFT Study of the Adsorption Mechanism of Sodium Salicylate onto Goethite or Hematite
HU Hui-Ping1, WANG Meng1, DING Zhi-Ying1, JI Guang-Fu2
1 College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, P. R. China;
2 Institute of Fluid Physics, Chinese Academy of Engineering Physics, Mianyang 621900, Sichuan Province, P. R. China
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The adsorption of sodium salicylate on goethite or hematite surfaces was investigated by Fourier transform infrared (FT-IR) spectroscopy, X-ray photoemission spectroscopy (XPS), and periodic plane-wave density functional theory (DFT) calculations. The core level shift (CLS) and charge transfer of the adsorbed surface iron sites calculated by DFT with periodic interfacial structures were compared with the X-ray photoemission experiments. The FT-IR results reveal that the interfacial structure of sodium salicylate adsorbed on goethite or hematite surfaces can be classified as bidentate binuclear (V) or bidentate mononuclear (IV), respectively. The DFT calculated results indicate that the bidentate binuclear (V) structure of sodium salicylate is favorable on the goethite (101) surface, with an adsorption energy of -5.46 eV, while the adsorption of sodium salicylate on the goethite (101) surface as a bidentate mononuclear (IV) structure is not predicted, as it has a positive adsorption energy of 3.80 eV. Conversely, on the hematite (001) surface, the bidentate mononuclear (IV) structure of the adsorbed sodium salicylate has anadsorption energy of -4.07 eV, confirming its favorability. Moreover, the calculated CLS of Fe 2p (-0.68 eV) for the adsorbed iron site on the goethite (101) surface is consistent with the experimentally observed CLS of Fe 2p (-0.5 eV) for SSa-treated goethite (goethite after the treatment of sodium salicylate). Our calculated CLS of Fe 2p (-0.80 eV) for the adsorbed iron site on the hematite (001) surface is likewise in good agreement with the experimentally observed CLS of Fe 2p (-0.8 eV) for SSa-treated hematite (hematite after the treatment of sodium salicylate). Thus, goethite is predicted to adsorb sodium salicylate as a bidentate binuclear (V) structure via the bonding of one carboxylate oxygen atom and the phenolic oxygen atom of sodium salicylate to two surface iron atoms of goethite (101). Meanwhile, on the hematite surface, the bidentate mononuclear (IV) complex formed via the bonding of one carboxylate oxygen atom and the phenolic oxygen atom of sodium salicylate to one surface iron atom of hematite (001) can be regarded as plausible.



Keywords: Goethite   Hematite   Sodium salicylate adsorption   FT-IR   XPS   DFT calculation  
Received: 2016-01-28 Accepted: 2016-04-22 Publication Date (Web): 2016-04-22
Corresponding Authors: WANG Meng, DING Zhi-Ying Email: mengwchem@163.com;huierding@126.com

Fund: The project was supported by the National Natural Science Foundation of China (51134007, 51174231).

Cite this article: HU Hui-Ping, WANG Meng, DING Zhi-Ying, JI Guang-Fu. FT-IR, XPS and DFT Study of the Adsorption Mechanism of Sodium Salicylate onto Goethite or Hematite[J]. Acta Phys. -Chim. Sin., 2016,32 (8): 2059-2068.    doi: 10.3866/PKU.WHXB201604225

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