Preparation of Potassium Doped g-C3N4 Thin Film Photoanode and Its Application in Photoelectrocatalytic Oxidation of Diclofenac Sodium in Water

doi:10.7503/cjcu20220005

Abstract

Abstract:

The difficulty in preparing thin film photoelectrodes with high optical quality and excellent electro- chemical property limited the application of photoelectrocatalytic oxidation process in water treatment. In this paper， g-C₃N₄ thin film electrodes loaded on indium tin oxide（ITO） glass was prepared by in situ calcination method and used potassium doping to improve their photoelectrocatalytic activity. The electrodes were characterized， the photoelectrocatalytic degradation of diclofenac sodium（DCF） in water with them was studied， and the DCF degradation pathways were investigated. The results showed that the in situ calcination method could prepare high-quality K⁺/g-C₃N₄ thin film photoelectrodes， and the doping of K⁺ insignificantly changed the crystalline shape， valence state， and porous morphology of g-C₃N₄ on the electrode. However， it could increase the loading of g-C₃N₄ on ITO glass and enhance the photocurrent response of the electrode to visible light. The optimal doping concentration of K⁺ was 0.002 mol/L. The rate constant of DCF degradation in photoelectrocatalytic oxidation process with the K⁺/g-C₃N₄ thin film electrode was 1.86 times higher than that with the pure g-C₃N₄ film electrode. The DCF removal rate from water in 2 h reaction time reached 70% with the initial pH of 4， applied potential of 1 V， and light intensity of 0.96 W/cm². For the photoelectrocatalytic oxidation of DCF with the K⁺/g-C₃N₄ film electrode， there was a synergy between photocatalytic oxidation and electrochemical oxidation. They could optimize each other and enhance the concentration of the photogenerated holes（h⁺） and hydroxyl radicals（·OH） produced in the reaction process. Under the action of these two active substances， DCF in water was oxidized by h⁺ into carbazole derivatives， reacted with ·OH to form polyhydroxy aromatic compounds， and finally occurred reaction of ring opening to form small molecules.

Key words: Potassium doped g-C₃N₄ thin film photoanode, Photoelectrocatalytic oxidation, Diclofenac sodium, Photocatalytic oxidation, Electrochemical oxidation

CLC Number:

O643

TrendMD:

GONG Yanxi, WANG Jianbing, CHAI Buyu, HAN Yuanchun, MA Yunfei, JIA Chaomin. Preparation of Potassium Doped g-C₃N₄ Thin Film Photoanode and Its Application in Photoelectrocatalytic Oxidation of Diclofenac Sodium in Water[J]. Chem. J. Chinese Universities, 2022, 43(6): 20220005.

Figures/Tables 11

References 30

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Degradation condition	Degradation of equation	Rate constant/min^-1	Half?life/min
PC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0012t-0.0259	0.0012	577.62
EC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0008t-0.0190	0.0008	866.43
PEC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0041t-0.0238	0.0041	169.06
PEC oxidation（I/g?C₃N₄）	ln（c_t /c₀）=-0.0022t-0.0367	0.0022	315.07
PEC oxidation（D/g?C₃N₄）	ln（c_t /c₀）=-0.0015t-0.0350	0.0015	462.10

Degradation condition	Degradation of equation	Rate constant/min^-1	Half?life/min
PC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0012t-0.0259	0.0012	577.62
EC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0008t-0.0190	0.0008	866.43
PEC oxidation（K⁺/g?C₃N₄）	ln（c_t /c₀）=-0.0041t-0.0238	0.0041	169.06
PEC oxidation（I/g?C₃N₄）	ln（c_t /c₀）=-0.0022t-0.0367	0.0022	315.07
PEC oxidation（D/g?C₃N₄）	ln（c_t /c₀）=-0.0015t-0.0350	0.0015	462.10

Voltage/V	Degradation of equation	Rate constant/min^-1	Half?life/min
0.5	ln（c_t /c₀）=-0.0020t-0.0475	0.0020	346.57
1.0	ln（c_t /c₀）=-0.0035t-0.0868	0.0035	198.04
1.5	ln（c_t /c₀）=-0.0020t-0.0718	0.0020	346.57
2.0	ln（c_t /c₀）=-0.0015t-0.0676	0.0015	462.10

Voltage/V	Degradation of equation	Rate constant/min^-1	Half?life/min
0.5	ln（c_t /c₀）=-0.0020t-0.0475	0.0020	346.57
1.0	ln（c_t /c₀）=-0.0035t-0.0868	0.0035	198.04
1.5	ln（c_t /c₀）=-0.0020t-0.0718	0.0020	346.57
2.0	ln（c_t /c₀）=-0.0015t-0.0676	0.0015	462.10

Initial pH	Degradation of equation	Rate constant/min^-1	Half?life/min
4	ln（c_t /c₀）=-0.0088t-0.0809	0.0088	78.77
6	ln（c_t /c₀）=-0.0032t-0.1536	0.0032	625.00
8	ln（c_t /c₀）=-0.0030t-0.0982	0.0030	231.05
10	ln（c_t /c₀）=-0.0011t-0.0305	0.0011	630.13

Preparation of Potassium Doped g-C₃N₄ Thin Film Photoanode and Its Application in Photoelectrocatalytic Oxidation of Diclofenac Sodium in Water

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