Citation: Longhui Zheng, Xiaojuan Yu, Mingce Long, Qilin Li. Humic acid-mediated visible-light degradation of phenol on phosphate-modified and Nafion-modified TiO₂ surfaces[J]. Chinese Journal of Catalysis, ;2017, 38(12): 2076-2084. doi: 10.1016/S1872-2067(17)62951-6 shu

Humic acid-mediated visible-light degradation of phenol on phosphate-modified and Nafion-modified TiO₂ surfaces

a School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;
b Key Laboratory for Thin Film and Microfabrication of the Ministry of Education, Shanghai Jiao Tong University, Shanghai 200240, China;
c Department of Civil and Environmental Engineering, Rice University, Houston, Texas 77005, United States

Received Date: 9 October 2017
Revised Date: 30 October 2017

Fund Project: This work was supported by the National Natural Science Foundation of China (21377084), Special Fund for Agro-Scientific Research in the Public Interest (201503107), and Shanghai Municipal International Cooperation Foundation (15230724600).

Although humic acid (HA) can inhibit TiO₂ photocatalysis, it can sensitize TiO₂ and induce significant visible-light (VL) activity in phenol degradation. This favorable effect of HA was negligible on phosphate-modified TiO₂ (P-TiO₂), but significantly stronger on Nafion-modified TiO₂ (Nf-TiO₂). The reaction rate constants for phenol degradation on Nf-TiO₂ increased from (0.003±0.001) to (0.025±0.003) min^-1 when the reaction was performed in the presence of 20 mg/L HA. The different effects of HA on P-TiO₂ and Nf-TiO₂ photocatalysis cannot be attributed to adsorption changes, because the adsorption capacities of P-TiO₂ and Nf-TiO₂ were only slightly lower than that of TiO₂ at an initial HA concentration of 20 mg/mL. Scavenger tests, electron paramagnetic resonance spectroscopy, and H₂O₂ detection were taken to understand the low VL activity of the P-TiO₂/HA suspension. The main active species for phenol degradation in the TiO₂ and Nf-TiO₂ suspensions were superoxide radicals. There were negligible amounts of superoxide radicals in the P-TiO₂/HA suspension, possibly because a direct four-electron oxygen reduction reaction occurred. The better VL activity of Nf-TiO₂ was rationalized on the basis of Mott-Schottky and electrochemical impedance plots. Nafion modification resulted in cathodic shifts of the energy band positions, increased electron density, and less resistance to electron transfer across the interface between TiO₂ and electrolytes. All these factors facilitated electron transfer and improved the production of active species. Phosphate modification therefore did not improve the VL response of HA sensitized TiO₂, and low concentrations of HA can facilitate VL photocatalytic degradation of organic pollutants on Nafion surface-modified TiO₂.
- Titanium dioxide,
- Humic acid,
- Nafion,
- Phosphate,
- Surface modification
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Humic acid-mediated visible-light degradation of phenol on phosphate-modified and Nafion-modified TiO2 surfaces

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通讯作者: 陈斌, bchen63@163.com

Humic acid-mediated visible-light degradation of phenol on phosphate-modified and Nafion-modified TiO₂ surfaces