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

References 38

[1]	WANG X X, YU S J, WANG X K . Removal of radionuclides by metal-organic framework-based materials. Journal of Inorganic Materials, 2019,34(1):17-26.
[2]	TAN X, FANG M, TAN L , et al. Core-shell hierarchical C@Na₂Ti₃O₇·9H₂O nanostructures for the efficient removal of radionuclides. Environmental Science: Nano, 2018,5(5):1140-1149.
[3]	BAI Z Q, YUAN L Y, ZHU L , et al. Introduction of amino groups into acid-resistant MOFs for enhanced U(VI) sorption. Journal of Materials Chemistry A, 2015,3(2):525-534.
[4]	CAI Y, CHEN L, YANG S , et al. Rational synthesis of novel phosphorylated chitosan-carboxymethyl cellulose composite for highly effective decontamination of U(VI). ACS Sustainable Chemistry & Engineering, 2019,7(5):5393-5403.
[5]	WU X, JIANG S, SONG S , et al. Constructing effective photocatalytic purification system with P-introduced g-C₃N₄ for elimination of UO₂ ²⁺. Applied Surface Science, 2018,430:371-379.
[6]	WANG L, SONG H, YUAN L , et al. Efficient U(VI) reduction and sequestration by Ti₂CT_x MXene. Environmental Science＆Technology, 2018,52(18):10748-10756.
[7]	LIU H, LI M, CHEN T , et al. New synthesis of nZVI/C composites as an efficient adsorbent for the uptake of U(VI) from aqueous solutions. Environmental Science＆Technology, 2017,51(16):9227-9234.
[8]	ZHU K, CHEN C, XU M , et al. In situ carbothermal reduction synthesis of Fe nanocrystals embedded into N-doped carbon nanospheres for highly efficient U(VI) adsorption and reduction. Chemical Engineering Journal, 2018,331:395-405.
[9]	ZOU Y, WANG X, KHAN A , et al. Environmental remediation and application of nanoscale zero-valent iron and its composites for the removal of heavy metal ions: a review. Environmental Science＆Technology, 2016,50(14):7290-7304.
[10]	LI Z, WANG L, MENG J , et al. Zeolite-supported nanoscale zero- valent iron: new findings on simultaneous adsorption of Cd(II), Pb(II), and As(III) in aqueous solution and soil. Journal of Hazardous Materials, 2018,344:1-11.
[11]	CHEN L, FENG S, ZHAO D , et al. Efficient sorption and reduction of U(VI) on zero-valent iron-polyaniline-graphene aerogel ternary composite. Journal of Colloid and Interface Science, 2017,490:197-206.
[12]	SHENG G, YANG P, TANG Y , et al. New insights into the primary roles of diatomite in the enhanced sequestration of UO₂ ²⁺ by zerovalent iron nanoparticles: an advanced approach utilizing XPS and EXAFS. Applied Catalysis B: Environmental, 2016,193:189-197.
[13]	SUN Y, LI J, HUANG T , et al. The influences of iron characteristics, operating conditions and solution chemistry on contaminants removal by zero-valent iron: a review. Water Research, 2016,100:277-295.
[14]	DENG H, LI Z, WANG L , et al. Nanolayered Ti₃C₂ and SrTiO₃ composites for photocatalytic reduction and removal of uranium (VI). ACS Applied Nano Materials, 2019,2(4):2283-2294.
[15]	HU L, YAN X W, ZHANG X J , et al. Integration of adsorption and reduction for uranium uptake based on SrTiO₃/TiO₂ electrospun nanofibers. Applied Surface Science, 2018,428:819-824.
[16]	CHEN K, CHEN C L, REN X M , et al. Interaction mechanism between different facet TiO₂ and U(VI): experimental and density- functional theory investigation. Chemical Engineering Journal, 2019,359:944-954.
[17]	LI P, WANG J, WANG Y , et al. Photoconversion of U(VI) by TiO₂: an efficient strategy for seawater uranium extraction. Chemical Engineering Journal, 2019,365:231-241.
[18]	LIU X N, DU P H, PAN W Y , et al. Immobilization of uranium(VI) by niobate/titanate nanoflakes heterojunction through combined adsorption and solar-light-driven photocatalytic reduction. Applied Catalysis B: Environmental, 2018,231:11-22.
[19]	LI Z J, HUANG Z W, GUO W L , et al. Enhanced photocatalytic removal of uranium(VI) from aqueous solution by magnetic TiO₂/ Fe₃O₄ and its graphene composite. Environmental Science & Technology, 2017,51(10):5666-5674.
[20]	FENG J N, YANG Z Q, HE S , et al. Photocatalytic reduction of Uranium(VI) under visible light with Sn-doped In₂S₃ microspheres. Chemosphere, 2018,212:114-123.
[21]	ZHANG S, LIU Y, GU P , et al. Enhanced photodegradation of toxic organic pollutants using dual-oxygen-doped porous g-C₃N₄: mechanism exploration from both experimental and DFT studies. Applied Catalysis B: Environmental, 2019,248:1-10.
[22]	ZHANG S, SONG S, GU P , et al. Visible-light-driven activation of persulfate over cyano and hydroxyl group co-modified mesoporous g-C₃N₄ for boosting bisphenol A degradation. Journal of Materials Chemistry A, 2019,7(10):5552-5560.
[23]	ZHANG S, GU P, MA R , et al. Recent developments in fabrication and structure regulation of visible-light-driven g-C₃N₄-based photocatalysts towards water purification: a critical review. Catalysis Today, 2019,335:65-77.
[24]	ZHANG S, HU C, JI H , et al. Facile synthesis of nitrogen-deficient mesoporous graphitic carbon nitride for highly efficient photocatalytic performance. Applied Surface Science, 2019,478:304-312.
[25]	GAO H, CAO R, XU X , et al. Construction of dual defect mediated Z-scheme photocatalysts for enhanced photocatalytic hydrogen evolution. Applied Catalysis B: Environmental, 2019,245:399-409.
[26]	GAO H, CAO R, ZHANG S , et al. Three-dimensional hierarchical g-C₃N₄ architectures assembled by ultrathin self-doped nanosheets: extremely facile hexamethylenetetramine activation and superior photocatalytic hydrogen evolution. ACS Applied Materials & Interfaces, 2019,11(2):2050-2059.
[27]	ZHANG S, GAO H, HUANG Y , et al. Ultrathin g-C₃N₄ nanosheets coupled with amorphous Cu-doped FeOOH nanoclusters as 2D/0D heterogeneous catalysts for water remediation. Environmental Science: Nano, 2018,5(5):1179-1190.
[28]	GAO H, YANG H, XU J , et al. Strongly coupled g-C₃N₄ nanosheets-Co₃O₄ quantum dots as 2D/0D heterostructure composite for peroxymonosulfate activation. Small, 2018,14(31):1801353.
[29]	JIANG X H, XING Q J, LUO X B , et al. Simultaneous photoreduction of uranium(VI) and photooxidation of arsenic(III) in aqueous solution over g-C₃N₄/TiO₂ heterostructured catalysts under simulated sunlight irradiation. Applied Catalysis B: Environmental, 2018,228:29-38.
[30]	KE L, LI P F, WU X , et al. Graphene-like sulfur-doped g-C₃N₄ for photocatalytic reduction elimination of UO₂ ²⁺ under visible light. Applied Catalysis B: Environmental, 2017,205:319-326.
[31]	LU C H, ZHANG P, JIANG S J , et al. Photocatalytic reduction elimination of UO₂ ²⁺ pollutant under visible light with metal-free sulfur doped g-C₃N₄ photocatalyst. Applied Catalysis B: Environmental, 2017,200:378-385.
[32]	LU C H, CHEN R Y, WU X , et al. Boron doped g-C₃N₄ with enhanced photocatalytic UO₂ ²⁺ reduction performance. Applied Surface Science, 2016,360:1016-1022.
[33]	DUAN S, WU L, LI J , et al. Two-dimensional copper-based metal- organic frameworks nano-sheets composites: one-step synthesis and highly efficient U(VI) immobilization. Journal of Hazardous Materials, 2019,373:580-590.
[34]	QIAN L, HU P, JIANG Z , et al. Effect of pH, fulvic acid and temperature on the sorption of uranyl on ZrP₂O₇. Science China Chemistry, 2010,53(6):1429-1437.
[35]	WANG D, XU Y, XIAO D , et al. Ultra-thin iron phosphate nanosheets for high efficient U(VI) adsorption. Journal of Hazardous Materials, 2019,371:83-93.
[36]	LI S, WANG L, PENG J , et al. Efficient thorium(IV) removal by two-dimensional Ti₂CT_x MXene from aqueous solution. Chemical Engineering Journal, 2019,366:192-199.
[37]	GAO H, CAO R, XU X , et al. Surface area- and structure-dependent effects of LDH for highly efficient dye removal. ACS Sustainable Chemistry & Engineering, 2019,7(1):905-915.
[38]	ZHU J, LIU Q, LIU J , et al. Ni-Mn LDH-decorated 3D Fe-inserted and N-doped carbon framework composites for efficient uranium (VI) removal. Environmental Science: Nano, 2018,5(2):467-475.

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

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