Construction of Novel Three Dimensionally Macroporous g-C3N4 for Efficient Adsorption/Photocatalytic Reduction of U(VI)

doi:10.15541/jim20190336

Abstract

Abstract:

Reduction of soluble U(VI) to insoluble U(IV) oxide is an effective approach to control uranium contamination. Three-dimensional (3D) macroporous g-C₃N₄ photocatalyst with interconnected porous was prepared by thermal polymerization and template etching using self-assembly of SiO₂ nanosphere as the template. The material was then applied to adsorption-photocatalytic reduction of U(VI). Characterization results showed that the 3D macroporous g-C₃N₄ photocatalyst presented a well-defined interconnected macroporous architecture and numerous nanopores existed on the well-defined macroporous skeleton. 3D macroporous g-C₃N₄ also had a significant increase in specific surface area which was beneficial to the absorption of visible light. Adsorption results showed that the maximum adsorption capacity of U(VI) on 3D macroporous g-C₃N₄ was ~30.5 mg/g, which was more than ~1.83 times higher than that of bulk g-C₃N₄. The adsorption isotherm matched well with the Langumuir equation. Photocatalytic reduction experiments showed that the 3D macroporous g-C₃N₄ had high photocatalytic activity and good stability with the reduction rate constant of 0.0142 min ^-1, which was ~4.9 times higher than bulk g-C₃N₄ (~0.0024 min ^-1). As the sorption-photocatalytic performance of the sample is excellent, 3D macroporous g-C₃N₄ is a high efficient visible-light-responsive photocatalyst for the removal of U(VI) from radioactive wastewater.

Key words: 3D macroporous g-C₃N₄, U(VI), adsorption, photocatalytic reduction

CLC Number:

TQ174

JIANG Li, GAO Huihui, CAO Ruya, ZHANG Shouwei, LI Jiaxing. Construction of Novel Three Dimensionally Macroporous g-C₃N₄ for Efficient Adsorption/Photocatalytic Reduction of U(VI)[J]. Journal of Inorganic Materials, 2020, 35(3): 359-366.

Figures/Tables 7

Fig. 1 XRD patterns (a) and FT-IR spectra (b) of the bulk g-C3N4 and 3D macroporous g-C3N4

Fig. 2 UV-Vis diffuse reflectance spectra (a) and surface areas (b) of the bulk g-C3N4 and 3D macroporous g-C3N4

Fig. 3 SEM and TEM images of the bulk g-C3N4 (a, b) and 3D macroporous g-C3N4 (c, d)

Fig. 4 (a) Adsorption kinetics and (b) adsorption isotherms for U(VI) on bulk g-C3N4 and 3D macropoous g-C3N4 pH=5.0±0.1, T=293 K, m/V=0.5 g/L The insert in (a) is the pseudo-second-order kinetic plots

Table 1 Fitting parameters of pseudo-first-order and pseudo-second-order kinetic models

Sample	Pseudo-first-ordermodel		Pseudo-second-ordermodel
Sample	k₁/min^-1	R²	k₂/(g∙mg^-1∙min^-1)	R²
Bulk g-C₃N₄	0.0761	0.983	0.0493	0.999
3D macroporous g-C₃N₄	0.1087	0.992	0.0721	0.999

Fig. 5 (a) Dark adsorption and photocatalytic reduction of U(VI) and (b) the rate constant with bulk g-C3N4 and 3D macroporous g-C3N4, (c) cycling runs of 3D macroporous g-C3N4 for the photocatalytic reduction of U(VI) and (d) U4f specta of 3D macroporous g-C3N4 before and after U(VI) photoreduction

Fig. 6 (a) Transient photocurrent responses and (b) electrochemical impedance spectra of bulk g-C3N4 and 3D macroporous g-C3N4

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Construction of Novel Three Dimensionally Macroporous g-C₃N₄ for Efficient Adsorption/Photocatalytic Reduction of U(VI)

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