Synthesis of Diatomite/g-C3N4 Composite with Enhanced Visible-light-responsive Photocatalytic Activity

doi:10.15541/jim20160015

Abstract

Abstract:

Novel visible-light-responsive diatomite/g-C₃N₄ composite was successfully synthesized via a facile impregnation-calcination method. The sample was characterized by TG, XRD, FE-SEM, HR-TEM, FT-IR, XPS, UV-Vis-DRS, and PL spectra. The photocatalytic activities of samples were evaluated by degradation of RhB under visible light irradiation. Experimental results indicated that 2.32wt% diatomite/g-C₃N₄ composite exhibits high efficiency for the degradation of RhB. The photoreaction kinetics constant value is about 1.9 times as high as that of g-C₃N₄ under visible light irradiation. The radical trap experiments indicate that ·O₂^- serves as the main active species for the photodegradation of RhB over 2.32wt% diatomite/g-C₃N₄ under visible light irradiation. The enhanced photoactivity is mainly attributed to the electrostatic interaction between g-C₃N₄ and negatively charged diatomite, synergistic effect lead to the efficient migration of the photogenerated electrons and holes of g-C₃N₄.

Key words: diatomite/g-C3N4 composite, impregnation-calcination method, visible-light-irradiation, electrostatic interaction

CLC Number:

TB321

WANG Dan-Jun, SHEN Hui-Dong, GUO Li, HE Xiao-Mei, ZHANG Jie, FU Feng. Synthesis of Diatomite/g-C₃N₄ Composite with Enhanced Visible-light-responsive Photocatalytic Activity[J]. Journal of Inorganic Materials, 2016, 31(8): 881-889.

Figures/Tables 10

Fig. 1 XRD patterns of samples(a) XRD patterns of diatomite, g-C3N4 and diatomite/g-C3N4 composite; (b) Enlarged XRD pattern of diatomite g-C3N4 and diatomite/g-C3N4 composites from 25° to 30° The peaks marked by (●) in (a) are the characteristic of the Quartz impurity in the diatomite sample

Fig. 2 XPS spectra of g-C3N4 and diatomite/g-C3N4(2.32wt%)(a) Survey spectra; (b) C1s; (c) N1s

Table 1 Content in diatomite/g-C3N4 by TG curves analysis

Samples	Diatomite theoretical content /wt%	Diatomite experimental/wt%
Diatomite/g-C₃N₄ (1.22wt%)	1.79	1.22
Diatomite/g-C₃N₄(2.32wt%)	3.56	2.32
Diatomite/g-C₃N₄(5.46wt%)	6.78	5.46
Diatomite/g-C₃N₄(13.88wt%)	15.38	13.88
Diatomite/g-C₃N₄(25.21wt%)	26.67	25.21

Fig. 3 TG curves for heating diatomite, g-C3N4 and diatomite/g-C3N4 composites

Fig. 4 FE-SEM and TEM images of samples(a) FE-SEM image of diatomite; (b) FE-SEM image of alkali washed diatomite; (c) FE-SEM image of diatomite/g-C3N4 composite; (d) TEM of diatomite/g-C3N4 composite; (e) SEAD pattern of g-C3N4; (f) Conjunction edge between flake-like g-C3N4 and diatomite particles

Fig. 5 FT-IR spectra of diatomite, g-C3N4 and diatomite/g- C3N4 composites

Fig. 6 (a) UV-Vis spectra and (b) plot of (αhν)1/2 vs energy (hν) for the band gap energy of g-C3N4 and diatomite/g-C3N4 composites

Fig. 7 Photocatalytic activity of the samples(A) Photocatalytic degradation efficiency of RhB by g-C3N4 and diatomite/g-C3N4 composites; (B) Comparison of mixted, treated and untreated diatomite/g-C3N4(2.32wt%); (C) Kinetic fit for the degradation of RhB with g-C3N4 and diatomite/g-C3N4 composites (a, blank; b, g-C3N4; c, diatomite/g-C3N4 (1.22wt%); d, diatomite/g-C3N4 (2.32wt%); e, diatomite/g-C3N4 (5.46wt%); f, diatomite/g-C3N4 (13.88wt%); g, diatomite/g-C3N4 (25.21wt%); h, diatomite/g- C3N4 mixture (2.32wt%); i, diatomite); (D) Adsorption percentage and rate constants; (E) Absorption spectral changes of RhB under visible light irradiation using diatomite/g-C3N4 (2.32wt%) as photocatalyst; (F) XRD patterns of diatomite/g-C3N4 before and after being used

Fig. 8 PL spectra of g-C3N4 and diatomite/ g-C3N4 composites

Fig. 9 Trapping experiment of active species during photocatalytic degradation of RhB over diatomite/g-C3N4 (2.32wt%) under visible light irradiation

References 46

[1]	KONSTANINOU I K, ALBANIS T A.TiO2-assistd photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations.Appl. Catal. B, 2004, 49(1): 1-14.
[2]	ARSLAN A I, TURELII G, OLMEZ H T.Treatment of zao dye production wastewaters using Photo-fenton-like advanced oxidation process: optimization by response surface methodology.J. Photochem. Photobiol. A, 2009, 202(2/3): 142-153.
[3]	WALTER M G, WARREN E L, MCKONE J R, et al.Solar water splitting cells.Chem. Rev., 2010, 110(11): 6446-6473.
[4]	WANG X C, MAEDA K, THOMAS A, et al.A metal-free polymeric photocatalyst for hydrogen production from water under visible light.Nat. Mater., 2009, 8(1): 76-80.
[5]	YAN S C, LI Z S, ZOU Z G.Photodegradation performance of g-C3N4 fabricated by directly heating melamine.Langmuir, 2009, 25(17): 10397-10401.
[6]	ZHANG X D, XIE X, WANG H, et al.Enhanced photoresponsive ultrathin graphitic-phase C3N4 nanosheets for bioimaging.J. Am. Chem. Soc., 2013, 135(1): 18-21.
[7]	ZHANG Y, MORI T, YE J, et al.Phosphorus-doped carbon nitride solid: enhanced electrical conductivity and photocurrent generation.J. Am. Chem. Soc., 2010, 132(18): 6294-6295.
[8]	MA X G, LV Y H, XU J, et al.A strategy of enhancing the photoactivity of g-C3N4 via doping of nonmetal elements: a first- principles study.J. Phys. Chem. C, 2012, 116(44): 23485-23493.
[9]	YAN S C, LI Z S, ZOU Z G.Photodegradation of rhodamine B and methyl orange over boron-doped g-C3N4 under visible light irradiation.Langmuir, 2010, 26(6): 3894-3901.
[10]	WANG Y, ZHANG J, WANG X, et al.Boron-and fluorine-containing mesoporous carbon nitride polymers: metal-free catalysts for cyclohexane oxidation.Angew. Chem. Int. Ed., 2010, 49(19): 3356-3359.
[11]	CHEN X F, ZHANG J S, FU X Z, et al.Fe-g-C3N4-catalyzed oxidation of benzene to phenol using hydrogen peroxide and visible light.J. Am. Chem. Soc., 2009, 131(33): 11658-11659.
[12]	GE L, ZUO F, LIU J K, et al.Synthesis and efficient visible light photocatalytic hydrogen rvolution of polymeric g-C3N4 coupled with CdS quantum dots.J. Phys. Chem. C, 2012, 116(25): 13708-13714.
[13]	LI T T, ZHAO L H, HE Y M, et al.Synthesis of g-C3N4/SmVO4 composite photocatalyst with improved visible light photocatalytic activities in RhB degradation.Appl. Catal. B, 2013, 129: 255-263.
[14]	WANG X J, YANG W Y, LI F T, et al.In situ microwave-assisted synthesis of porous N-TiO2/g-C3N4 heterojunctions with enhanced visible-light photocatalytic properties.Ind. Eng. Chem. Res., 2013, 52(48): 17140-17150.
[15]	KATSUMATA H, SAKAI T, SUZUKI T, et al.Highly efficient photocatalytic activity of g-C3N4/Ag3PO4 hybrid photocatalysts through Z-scheme photocatalytic mechanism under visible light.Ind. Eng. Chem. Res., 2014, 53(19): 8013-8025.
[16]	HE Y M, CAI J, LI T T, et al.Synthesis, characterization, and activity evaluation of DyVO4/g-C3N4 composites under visible-light irradiation.Ind. Eng. Chem. Res., 2012, 51(45): 14729-14737.
[17]	DONG F, NI Z L, LI P D, et al.A general method for type I and type II g-C3N4/g-C3N4 metal-free isotype heterostructures with enhanced visible light photocatalysis.New J. Chem., 2015, 39(6): 4737-4744.
[18]	GE L, HAN C, LIU J, et al. Enhanced visible light photocatalytic activity of novel polymeric g-C3N4 loaded with Ag nanoparticles. Appl. Catal. A, 2011, 409-410: 215-222.
[19]	JUNG K W, JANG D, AHN K H.A novel approach for improvement of purity and porosity in diatomite (diatomaceous earth) by applying an electric field.Int. J. Miner. Process, 2014, 131: 7-11.
[20]	WANG B, ZHANG G X, LENG X.Characterization and improved solar light activity of vanadium doped TiO2/diatomite hybrid catalysts.J. Hazard. Mater., 2015, 285: 212-220.
[21]	SUN Z M, YANG X P, ZHANG G X, et al.A novel method for purification of low grade diatomite powders in centrifugal fields.Int. J. Miner. Process, 2013, 125: 18-26.
[22]	LOSIC D, MITCHELL J G, VOELCKER N H.Diatomaceous lessons in nanotechnology and advanced materials.Adv. Mater., 2009, 21(29): 2947-2958.
[23]	SPRYNSKYY M, KOVALCHUK I, BUSZEWSKI B.The separation of uranium ions by natural and modified diatomite from aqueous solution.J. Hazard. Mater., 2010, 181(1/2/3): 700-707.
[24]	YU W B, YUAN P, LIU D, et al.Facile preparation of hierarchically porous diatomite/MFI-type zeolite composites and their performance of benzene adsorption: The effects of NaOH etching pretreatment.J. Hazard. Mater., 2015, 285: 173-181.
[25]	DU Y C, FAN H G, WANG L P, et al.α-Fe2O3 nanowires deposited diatomite: highly efficient absorbents for the removal of arsenic.J. Mater. Chem. A, 2013, 1(26): 7729-7737.
[26]	PADMANABHAN S K, PAL S, HAQ E U, et al.Nanocrystalline TiO2-diatomite composite catalysts: effect of crystallization on the photocatalytic degradation of rhodamine B.Appl. Catal. A: Gen., 2014, 485: 157-162.
[27]	XIA Y, LI F F, JIANG Y S, et al.Interface actions between TiO2 and porous diatomite on the structure and photocatalytic activity of TiO2-diatomite.Appl. Surf. Sci., 2014, 303: 290-296.
[28]	KARAMAN S, KARAIPEKLI A, ALPER B A.Polyethylene glycol (PEG)/diatomite composite as a novel form-stable phase change material for thermal energy storage.Solar Energy Mater. Solar Cells, 2011, 95: 1647-1653.
[29]	LIANG X H, FU X Y.Effect of the Ce-TiO2/diatomite on the photo-catalysis degradation of MB.Mater. Sci. Forum., 2014, 789: 44-47.
[30]	JEONG S G, JEON J, LEE J H, et al.Optimal preparation of PCM/diatomite composites for enhancing thermal properties.Int. J. Heat Mass Trans., 2013, 62: 711-717.
[31]	GUO S F, SHI L.Synthesis of succinic anhydride from maleic anhydride on Ni/diatomite catalysts.Catal. Today, 2013, 212: 137-141.
[32]	HOU Y, LAURSEN A B, ZHANG J, et al.Layered nanojunctions for hydrogen-evolution catalysis.Angew. Chem. Int. Ed., 2013, 52(13): 3621-3625.
[33]	WANG J L, YU Y, ZHANG L Z. Highly efficient photocatalytic removal of sodium pentachlorophenate with Bi3O4Br under visible light. Appl. Catal. B: Environ., 2013, 136-137: 112-121.
[34]	NIU P, LIU G, CHENG H M.Nitrogen vacancy-promoted photocatalytic activity of graphitic carbon nitride.J. Phys. Chem. C, 2012, 116(20): 11013-11018.
[35]	KHRAISHEH M A M, AL-DEGS Y S, MCMINN W A M. Remediation of wastewater containing heavy metals using raw and modified diatomite.Chem. Eng. J., 2004, 99(2): 177-184.
[36]	ELZEA J M, RICE S B.TEM and X-ray diffraction evidence for cristobalite and tridymite stacking sequences in opal.Clays & Clay Miner, 1996, 44: 492-500.
[37]	DONG L, WU Y, SUN M, et al.Efficient synthesis of polymeric g-C3N4 layered materials as novel efficient visible light driven photocatalysts.J. Mater. Chem., 2011, 21: 15171-15174.
[38]	WANG Y J, BAI X J, PAN C S, et al.Enhancement of photocatalytic activity of Bi2WO6 hybridized with graphite-like C3N4.J. Mater. Chem., 2012, 22(23): 11568-11573.
[39]	ZIMMERMAN J L, WILLIAMS R, KHABASHESKU V N, et al.Synthesis of spherical carbon nitride nanostructures.Nano Lett., 2001, 1: 731-734.
[40]	JIANG L, CHEN L L, ZHU J J, et al.Novel p-n heterojunction photocatalyst constructed by porous graphite-like C3N4 and nanostructured BiOI: facile synthesis and enhanced photocatalytic activity.Dalton Trans., 2013, 42(44): 15726-15734.
[41]	ZHANG Y, THOMAS A, ANTONIETTI M, et al.Activation of carbon nitride solids by protonation: morphology changes, enhanced ionic conductivity, and photoconduction experiments.J. Am. Chem. Soc., 2009, 131(1): 50-51.
[42]	XIAGN Q, YU J, JARONIEC M.Preparation and enhanced visible-light photocatalytic H2-production activity of graphene/C3N4 composites.J. Phys. Chem. C, 2011, 115(15): 7355-7363.
[43]	ZHANG P F, ZHANG J L, CHEN F, et al.Study of adsorption and degradation of acid orange 7 on the surface of CeO2 under visible light irradiation.Appl. Catal. B, 2009, 85(3/4): 148-154.
[44]	YIN M C, LI Z S, KOU J H, et al.Mechanism investigation of visible light-induced degradation in a heterogeneous TiO2/eosin Y/rhodamine B system.Environ. Sci. Technol., 2009, 43(21): 8361-8366.
[45]	YIN M C, LI Z S, KOU J H, et al.Diatomite-immobilized BiOI hybrid photocatalyst: facile deposition synthesis and enhanced photocatalytic activity.Appl. Surf. Sci., 2015, 353: 1179-1185.
[46]	LI Y P, ZHAN J, HUANG L Y, et al.Synthesis and photocatalytic activity of a bentonite/g-C3N4 composite.RSC Adv., 2014, 4(23): 11831-11839.

Synthesis of Diatomite/g-C₃N₄ Composite with Enhanced Visible-light-responsive Photocatalytic Activity

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