Preparation and Properties of Ag@C3N4 Photocatalyst Supported by Hydrogel

doi:10.15541/jim20210535

Abstract

Abstract:

Graphitic carbon nitride (g-C₃N₄) is widely used in the field of photocatalysis due to its unique two-dimensional planar structure and suitable energy band structure. However, it has some disadvantages such as fast recombination of the electron-hole, low visible-light utilization efficiency and poor dispersion in water, which hinder its application. In this study, the hydrogel prepared by sodium alginate was used as matrix to improve the dispersion of Ag@C₃N₄ composite in water, and at the same time enhanced the separation efficiency of photoelectron-holes pairs, thus improving its photocatalytic performance. Firstly, g-C₃N₄ was synthesized by thermal polymerization and then exfoliated into nanosheets by ultrasound. Then, Ag nanoparticles were deposited in situ on the surface of g-C₃N₄ by solution method to prepare Ag@C₃N₄. Finally, hydrogel loaded with Ag@C₃N₄ (SA/Ag@C₃N₄) was obtained by using calcium ion as crosslinker and sodium alginate (SA) as precursor. The morphology, microstructure and phase composition of the as-prepared photocatalyst were characterized. The as-prepared SA/Ag@C₃N₄ exhibited a 1.5 times higher photocatalytic degradation rate of methyl orange than that of Ag@C₃N₄. The catalytic mechanism was investigated by photoluminescence spectrum, time resolved photoluminescence spectrum and electron paramagnetic resonance spectrum. The results showed that the surface plasmon resonance effect of silver nanoparticles together with the porous structure and mass transfer channel of sodium alginate hydrogel plays a synergistic role in the enhancement of photocatalytic performance.

Key words: carbon nitride, silver nanoparticles, sodium alginate, hydrogel, photocatalysis

CLC Number:

TQ426

WANG Xiaojun, XU Wen, LIU Runlu, PAN Hui, ZHU Shenmin. Preparation and Properties of Ag@C₃N₄ Photocatalyst Supported by Hydrogel[J]. Journal of Inorganic Materials, 2022, 37(7): 731-740.

Figures/Tables 13

Fig. 1 Macro morphologies of g-C3N4 (a), Ag@C3N4 (b), SA (c), and SA/Ag@C3N4 (d)

Fig. 2 SEM images of C3N4 (a), Ag@C3N4 (b) and SA/Ag@C3N4 (c, d), TEM (e) and HRTEM (f) images of Ag@C3N4

Fig. 3 FT-IR spectra of C3N4, Ag@C3N4, SA, and SA/Ag@C3N4 Colorful figures are available on the website

Fig. 4 XRD patterns of C3N4, Ag@C3N4, SA and SA/Ag@C3N4 (a), and magnified XRD patterns of SA/Ag@C3N4(b) Colorful figures are available on the website

Fig. 5 N2 adsorption-desorption isotherms (a) and pore size distribution curves (b) of C3N4, Ag@C3N4 and SA/Ag@C3N4 Colorful figures are available on the website

Fig. 6 SEM image (a) and EDX element mappings of Ag@C3N4 sample ((b) C, (c) N, (d) Ag)

Fig. 7 XPS spectra of C3N4 (a, b), Ag@C3N4 (c, d) and SA/Ag@C3N4 (e-g) (a, c, e) C1s; (b, d, f) N1s; (g) Ag3d

Fig. 8 Methyl orange degradation curves (a), degradation rates (b) of C3N4, Ag@C3N4, SA, and SA/Ag@C3N4, and cyclic stability(c) of SA/Ag@C3N4 Colorful figures are available on the website

Fig. 9 PL (a) and TRPL (b) spectra of C3N4, Ag@C3N4 and SA/Ag@C3N4 Colorful figures are available on the website

Fig. 10 (a) UV-Vis diffuse reflection spectra and (b) (αhν)0.5 vs hν curves of C3N4, Ag@C3N4, SA and SA/Ag@C3N4 Colorful figures are available on the website

Fig. 11 EPR spectra of C3N4 (a, b), Ag@C3N4 (c, d) and SA/Ag@C3N4 (e, f) during detecting ·OH (a, c, e) and ·O2- (b, d, f) Colorful figures are available on the website

Fig. 12 Transient photocurrent curves (a) and EIS curves (b) of C3N4 and Ag@C3N4 Colorful figures are available on the website

Fig. 13 Schematic diagram and catalytic mechanism of SA/Ag@C3N4

References 41

[1]	陈思, 李侃, 徐云兰, 等. N、F掺杂的TiO₂膜电极在可见光条件下光电催化氧化诱惑红脱色效果的研究. 净水技术, 2009, 28(4): 55-59.
[2]	任南琪, 周显娇, 郭婉茜, 等. 染料废水处理技术研究进展. 化工学报, 2013, 64(1): 84-94.
[3]	CHEN Q H, XIN Y J, ZHU X W. Au-Pd nanoparticles-decorated TiO₂ nanobelts for photocatalytic degradation of antibiotic levofloxacin in aqueous solution. Electrochimica Acta, 2015, 186: 34-42. DOI URL
[4]	MARDAREV D, TEODORESCU V, IANCULESCU A, et al. Thermal behavior study of some Sol-Gel TiO₂ based materials. Journal of Thermal Analysis and Calorimetry, 2008, 92(1): 7-13. DOI URL
[5]	XIN G, MENG Y. Pyrolysis synthesized g-C₃N₄ for photocatalytic degradation of methylene blue. Journal of Chemistry, 2013, 2013: 1-5.
[6]	JI H, CHANG F, HU X, et al. Photocatalytic degradation of 2, 4, 6-trichlorophenol over g-C₃N₄ under visible light irradiation. Chemical Engineering Journal, 2013, 218: 183-190. DOI URL
[7]	LI X H, ZHANG J, CHEN X, et al. Condensed graphitic carbon nitride nanorods by nanoconfinement: promotion of crystallinity on photocatalytic conversion. Chemistry of Materials, 2011, 23(19): 4344-4348. DOI URL
[8]	JORGE A B, MARTIN D J, DHANOA M T S, et al. H₂ and O₂ evolution from water half-splitting reactions by graphitic carbon nitride materials. Physical Chemistry C, 2013, 117(14): 7178-7185. DOI URL
[9]	CHEN Q, LI S, XU H, et al. Co-MOF as an electron donor for promoting visible-light photoactivities of g-C₃N₄ nanosheets for CO₂ reduction. Chinese Journal of Catalysis, 2020, 41(3): 514-523. DOI URL
[10]	HAN C Q, LI J, MA Z Y, et al. Black phosphorus quantum dot/g-C₃N₄composites for enhanced CO₂ photoreduction to CO. Science China Materials, 2018, 61(9): 1159-1166. DOI URL
[11]	张家晶, 郑永杰, 金春雪, 等. g-C₃N₄基光催化剂改性的研究进展. 现代化工, 2021, 3: 42-47.
[12]	ZHANG J S, CHEN X F, TAKANABE K, et al. Synthesis of a carbon nitride structure for visible-light catalysis by copolymerization. Angewandte Chemie International Edition, 2010, 49(2): 441-444. DOI URL
[13]	MENG J C, WANG X Y, LIU Y Q, et al. Acid-induced molecule self-assembly synthesis of Z-scheme WO₃/g-C₃N₄ heterojunctions for robust photocatalysis against phenolic pollutants. Chemical Engineering Journal, 2021, 403: 126354.
[14]	KREIBIG U. Electronic properties of small silver particles: the optical constants and their temperature dependence. Journal of Physics F: Metal Physics, 1974, 4: 999-1014. DOI URL
[15]	刘兵, 周益民, 吴清珍, 等. 纤维素水凝胶包覆Fe₃O₄类Fenton纳米催化剂的制备及其催化降解性能. 材料科学与工程学报, 2017, 35(1): 119-124.
[16]	冯华伟, 薛长国, 林秀玲. 海藻酸钠-碳材料复合凝胶吸附水中污染物的研究进展. 化工新型材料, 2021, 49(3): 241-244.
[17]	李莉, 郭伊荇, 周萍, 等. 孔道结构H₃PW₁₂O₄₀/TiO₂的制备及其可见光光催化降解水溶性染料的性能. 催化学报, 2005, 3: 209-215.
[18]	张晨宇, 王利强. 添加LDH-ZnO的海藻酸钠基抗菌复合材料研究综述. 包装工程, 2020, 41(23): 76-82.
[19]	KHAN S B, AHMAD S, KAMAL T, et al. Metal nanoparticles decorated sodium alginatecarbon nitride composite beads as effective catalyst for the reduction of organic pollutants. International Journal of Biological Macromolecules, 2020, 164: 1087-1098. DOI URL
[20]	BARRETT E P, JOYNER L G, HALENDA P P. The determination of pore volume and area distributions in porous substances. I. Computations from nitrogen isotherms. Journal of the American Chemical Society, 1951, 73(1): 373-380. DOI URL
[21]	BRUNAUER S, EMMETT P H, TELLER E. Adsorption of gases in multimolecular layers. Journal of the American Chemical Society, 1938, 60(2): 309-319. DOI URL
[22]	ZHENG Y, LIN L, YE X, et al. Helical graphitic carbon nitrides with photocatalytic and optical activities. Angewandte Chemie International Edition, 2014, 53: 11926-11930. DOI URL
[23]	WATERHOUSE G, BOWMAKER G A, METSON J B. The thermal decomposition of silver (I, Ⅲ) oxide: A combined XRD, FT-IR and Raman spectroscopic study. Physical Chemistry Chemical Physics, 2001, 3(17): 3838-3845. DOI URL
[24]	FAN J C, SHI Z X, LIAN M, et al. Mechanically strong graphene oxide/sodium alginate/polyacrylamide nanocomposite hydrogel with improved dye adsorption capacity. Journal of Materials Chemistry A, 2013, 1(25): 7433-7443. DOI URL
[25]	ITHIARA D, BIANCA C S, ALVARO L M, et al. Formulation and optimization of a novel TiO₂/calcium alginate floating photocatalyst. International Journal of Biological Macromolecules, 2019, 137: 992-1001. DOI URL
[26]	MOHSIN N, ALAMGIR A K, ABID H, et al. Reduced graphene oxide-TiO₂/sodium alginate 3-dimensional structure aerogel for enhanced photocatalytic degradation of ibuprofen and sulfamethoxazole. Chemosphere, 2020, 261: 127702.
[27]	MOHSIN N, MOKREMA M, JIHO K, et al. Photodegradation of microcystin-LR using graphene-TiO₂/sodium alginate aerogels. Carbohydrate Polymers, 2018, 199: 109-118. DOI URL
[28]	樊新, 黄可龙, 刘素琴, 等. 化学还原法制备纳米银粒子及其表征. 功能材料, 2007, 38(6): 996-999.
[29]	WANG X, MAEDA K, THOMAS A, et al. A metal- free polymeric photocatalyst for hydrogen production from water under visible light. Nature Materials, 2009, 8: 76-80. DOI URL
[30]	金瑞瑞, 游继光, 张倩, 等. Fe掺杂g-C₃N₄的制备及其可见光催化性能. 物理化学学报, 2014, 30(9): 1706-1712.
[31]	YU X, HU C W, HAO D N, et al. Tubular carbon nitride with hierarchical network: localized charge carrier generation and reduced charge recombination for high-performance photocatalysis of H₂ and H₂O₂ production. Solar RRL, 2020, 5(5): 566-571.
[32]	查莉, 王璐瑶, 郑雅慧, 等. 纤维素/海藻酸钠复合气凝胶的表面功能化与仿生矿化. 功能高分子学报, 2020, 33(4): 382-389.
[33]	TONG Q, DONG Y M, YAN L, et al. High-efficient synthesis and photo catalytic properties of Ag/AgBr/TiO₂monolithic photocatalysts using sodium alginate as substrate. Journal of Inorganic Materials, 2017, 32(6): 637-642. DOI URL
[34]	JING H, LI W, ZHOU H M, et al. Metallic MoO₂-modified graphitic carbon nitride boosting photocatalytic CO₂ reduction via Schottky junction. Solar RRL, 2020, 4(8): 841-848.
[35]	ZHANG Y Z, HUANG Z X, SHI J W, et al. Maleic hydrazide- based molecule doping in three-dimensional lettuce-like graphite carbon nitride towards highly effiffifficient photocatalytic hydrogen evolution. Applied Catalysis B: Environmental, 2020, 272: 119009.
[36]	CHENG L, YIN H, CAI C, et al. Single Ni atoms anchored on porous few-layer g-C₃N₄ for photocatalytic CO₂ reduction: the role of edge confinement. Small, 2020, 16: 986-996.
[37]	SUBHAJYOTI S, RAJKUMAR Y, ABHINAV K, et al. Surface modifified C, O co-doped polymeric g-C₃N₄ as an efficient photocatalyst for visible light assisted CO₂ reduction and H₂O₂ production. Applied Catalysis B: Environmental, 2019, 259: 118054.
[38]	ZENG Z X, YU H T, QUAN X, et al. Structuring phase junction between tri-s-triazine and triazine crystalline C₃N₄ for efficient photocatalytic hydrogen evolution. Applied Catalysis B: Environmental, 2018, 227: 153-160. DOI URL
[39]	FRANZ URBACH. The long-wavelength edge of photographic sensitivity and of the electronic absorption of solids. Physical Review, 1953, 92(5): 1324.
[40]	CUSHING S K, LI J, MENG F, et al. Photocatalytic activity enhanced by plasmonic resonant energy transfer from metal to semiconductor. Journal of the American Chemical Society, 2012, 134(36): 15033-15041. DOI URL
[41]	ALBERTO A, DI W. Photoelectrochemical properties of graphene and its derivatives. Nanomaterials, 2013, 3: 325-356. DOI URL

Preparation and Properties of Ag@C₃N₄ Photocatalyst Supported by Hydrogel

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