Preparation of SiO2@Ag@SiO2@TiO2 Core-shell Structure and Its Photocatalytic Degradation Property

doi:10.15541/jim20210685

Abstract

Abstract:

Photocatalytic degradation is an eco-friendly and high-efficiency way to degrade dye pollutants which has broad application prospects in water pollution control. In this study, the multi-layer core-shell structure of SiO₂@Ag@SiO₂@TiO₂ was synthesized by different methods as a photocatalyst for pollutant degradation, with oxidation-reduction method, modified Stöber method and hydrothermal method in turn. Effect of silver nitrate (AgNO₃), tetraethyl orthosilicate (TEOS) and tetrabutyl titanate (TBOT) on the coating effect were discussed. Microstructure, phase structure, pore structure parameters and photoelectrical properties of SiO₂-based multi-layer core-shell structure were systematically analyzed by various characterization methods while its degradation performance of methylene blue (MB) was also studied and discussed. The results show that when the mass ratio of AgNO₃, TEOS and TBOT to SiO₂ is 5 : 2.4 : 6 : 1, each layer of the multi-layer cored shell structure achieves the optimal coating effect. Compared with SiO₂@TiO₂ and SiO₂@Ag@TiO₂, the core-shell structure of SiO₂@Ag@SiO₂@TiO₂ photocatalyst has the best photocatalytic activity. Its photocatalytic degradation efficiency is close to 93% after simulated visible light irradiation for 45 min, and degradation efficiency keeps at 90% after 4 cycles of recycling tests.

Key words: core-shell structure, photocatalysis, titanium dioxide, methylene blue

CLC Number:

TB333

CHI Congcong, QU Panpan, REN Chaonan, XU Xin, BAI Feifei, ZHANG Danjie. Preparation of SiO₂@Ag@SiO₂@TiO₂ Core-shell Structure and Its Photocatalytic Degradation Property[J]. Journal of Inorganic Materials, 2022, 37(7): 750-756.

Figures/Tables 12

Fig.1 Schematic diagram for synthesizing SiO2@Ag@SiO2@TiO2 microspheres

Fig. 2 SEM images of SiO2@Ag microspheres prepared with different AgNO3/SiO2 mass ratios (a) 2 : 1; (b) 3 : 1; (c) 4 : 1; (d) 5 : 1

Fig. 3 STEM image (a), EDS pattern of selected region (b), TEM image (c), and HRTEM image (d) of SiO2@Ag microspheres

Fig. 4 SEM images of SiO2@Ag microspheres before (a) and after (b) thermal-treated at 500 ℃

Fig. 5 SEM images of SiO2@Ag@SiO2 microspheres prepared with different TEOS/SiO2 mass ratios (a) 0.9 : 1; (b) 1.4 : 1; (c) 1.9 : 1; (d) 2.4 : 1

Fig. 6 SEM images of SiO2@Ag@TiO2 microspheres with different TBOT/SiO2 mass ratios (a) 3 : 1; (b) 4 : 1; (c) 5 : 1; (d) 6 : 1; (e) 7 : 1; (f) 8 : 1

Fig. 7 (a) TEM image, (b) EDS pattern, (c) HRTEM image and corresponding elemental mapping of O, Si, Ag and Ti of SiO2@Ag@SiO2@TiO2 microspheres

Fig. 8 XRD patterns of different SiO2-based microspheres

Table 1 Pore structure parameters of different microspheres

Sample	S_BET/ (m²·g^-1)	Pore volume/ (cm³·g^-1)	Average pore size/nm
SiO₂	18.95	0.23	56.20
SiO₂@Ag	23.87	0.38	62.78
SiO₂@Ag@TiO₂	48.36	0.23	15.85
SiO₂@Ag@SiO₂@TiO₂	81.36	0.25	10.37

Fig. 9 Nitrogen adsorption-desorption isotherms of different SiO2-based microspheres

Fig. 10 ln(At/A0)-t curves of different samples and cyclic tests of MB degradation by SiO2@Ag@SiO2@TiO2 (insert)

Fig. 11 Transient photocurrent responses (a) and electrochemical impedance spectra (b) of different samples

References 21

[1]	DAWOOD S, SEN T K, PHAN C. Synthesis and characterization of novel-activated carbon from waste biomass pine cone and its application in the removal of Congo Red dye from aqueous solution by adsorption. Water, Air & Soil Pollution, 2014, 225(1): 1-16.
[2]	MOZIA S, SZYMAŃSKI K, MICHALKIEWICZ B, et al. Effect of process parameters on fouling and stability of MF/UF TiO₂ membranes in a photocatalytic membrane reactor. Separation and Purification Technology, 2015, 142: 137-148. DOI URL
[3]	TIAN Y S, HE W H, ZHU X P, et al. Improved electrocoagulation reactor for rapid removal of phosphate from wastewater. ACS Sustainable Chemistry&Engineering, 2017, 5(1): 67-71.
[4]	FU L Y, WU C Y, ZHOU Y X, et al. Ozonation reactivity characteristics of dissolved organic matter in secondary petrochemical wastewater by single ozone, ozone/H₂O₂, and ozone/catalyst. Chemosphere, 2019, 233: 34-43. DOI URL
[5]	CHEN W M, GU Z P, RAN G L, et al. Application of membrane separation technology in the treatment of leachate in China: a review. Waste Management, 2021, 121: 127-140. DOI URL
[6]	OLVERA-VARGAS H, OTURAN N, OTURAN M A, et al. Electro-Fenton and solar photoelectron-fenton treatments of the pharmaceutical ranitidine in pre-pilot flow plant scale. Separation & Purification Technology, 2015, 146: 127-135.
[7]	RASHID R, SHAFIQ I, AKHTER P. A state-of-the-art review on wastewater treatment techniques: the effectiveness of adsorption method. Environmental Science and Pollution Research International, 2021, 28(8): 9050-9066. DOI URL
[8]	BUZZETTI L, CRISENZA G E M, MELCHIORRE P. Mechanistic studies in photocatalysis. Angewandte Chemie International Edition, 2019, 58(12): 3730-3747. DOI URL
[9]	LI X B, KANG B B, DONG F, et al. Enhanced photocatalytic degradation and H₂/H₂O₂ production performance of S-pCN/WO_2.72 S-scheme heterojunction with appropriate surface oxygen vacancies. Nano Energy, 2021, 81: 105671.
[10]	XIONG J, LI X B, HUANG J T, et al. CN/rGO@BPQDs high-low junctions with stretching spatial charge separation ability for photocatalytic degradation and H₂O₂ production. Applied Catalysis B: Environmental, 2020, 266: 118602.
[11]	WANG R, CAI X, SHEN F L. Preparation of TiO₂ hollow microspheres by a novel vesicle template method and their enhanced photocatalytic properties. Ceramics International, 2013, 39(8): 9465-9470. DOI URL
[12]	NATARAJAN S, BAJAJ H C, TAYADE R J. Recent advances based on the synergetic effect of adsorption for removal of dyes from waste water using photocatalytic process. Journal of Environmental Sciences, 2018, 65(03): 201-222. DOI URL
[13]	CUI Z H, WU F, JIANG H. First-principles study of relative stability of rutile and anatase TiO₂ using the random phase approximation. Physical Chemistry Chemical Physics, 2016, 18(43): 29914-29922. DOI URL
[14]	LI X B, WANG W W, DONG F, et al. Recent advances in noncontact external-field-assisted photocatalysis: from fundamentals to applications. ACS Catalysis, 2021, 11(8): 4739-4769. DOI URL
[15]	YU J, LEI J, WANG L, et al. TiO₂ inverse opal photonic crystals: synthesis, modification, and applications-a review. Journal of Alloys and Compounds, 2018, 769: 740-757. DOI URL
[16]	GUITOUME D, ACHOUR S, SOBTI N, et al. Structural optical and photoelectrochemical properties of TiO₂ films decorated with plasmonic silver nanoparticles. Optik, 2018, 154: 182-191. DOI URL
[17]	FU X, PAN L, LI S, et al. Controlled preparation of Ag nanoparticle films by a modified photocatalytic method on TiO₂ films with Ag seeds for surface-enhanced Raman scattering. Applied Surface Science, 2016, 363(15): 412-420. DOI URL
[18]	YU X X, LIU S W, YU J G. Superparamagnetic γ-Fe₂O₃@SiO₂@TiO₂ composite microspheres with superior photocatalytic properties. Applied Catalysis B: Environmental, 2011, 104(1/2): 12-20. DOI URL
[19]	ULLAH S, FERREIRA-NETO E P, PASA A A, et al. Enhanced photocatalytic properties of core@shell SiO₂@TiO₂ nanoparticles. Applied Catalysis B: Environmental, 2015, 179: 333-343. DOI URL
[20]	PAN D L, HAN Z Y, MIAO Y C, et al. Thermally stable TiO₂ quantum dots embedded in SiO₂ foams: characterization and photocatalytic H₂ evolution activity. Applied Catalysis B: Environmental, 2018, 229: 130-138. DOI URL
[21]	CHI C C, REN C N, QU P P, et al. Controllable synthesis of nano- silica and self-assembly of photonic crystals. Journal of Shaanxi University of Science & Technology, 2021, 39(01): 117-125.

Preparation of SiO₂@Ag@SiO₂@TiO₂ Core-shell Structure and Its Photocatalytic Degradation Property

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 12

References 21

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	WU Rui, ZHANG Minhui, JIN Chenyun, LIN Jian, WANG Deping. Photothermal Core-Shell TiN@Borosilicate Bioglass Nanoparticles: Degradation and Mineralization [J]. Journal of Inorganic Materials, 2023, 38(6): 708-716.
[2]	WU Lin, HU Minglei, WANG Liping, HUANG Shaomeng, ZHOU Xiangyuan. Preparation of TiHAP@g-C₃N₄ Heterojunction and Photocatalytic Degradation of Methyl Orange [J]. Journal of Inorganic Materials, 2023, 38(5): 503-510.
[3]	MA Xiaosen, ZHANG Lichen, LIU Yanchao, WANG Quanhua, ZHENG Jiajun, LI Ruifeng. 13X@SiO₂: Synthesis and Toluene Adsorption [J]. Journal of Inorganic Materials, 2023, 38(5): 537-543.
[4]	MA Xinquan, LI Xibao, CHEN Zhi, FENG Zhijun, HUANG Juntong. BiOBr/ZnMoO₄ Step-scheme Heterojunction: Construction and Photocatalytic Degradation Properties [J]. Journal of Inorganic Materials, 2023, 38(1): 62-70.
[5]	CHEN Hanxiang, ZHOU Min, MO Zhao, YI Jianjian, LI Huaming, XU Hui. 0D/2D CoN/g-C₃N₄ Composites: Structure and Photocatalytic Performance for Hydrogen Production [J]. Journal of Inorganic Materials, 2022, 37(9): 1001-1008.
[6]	XUE Hongyun, WANG Congyu, MAHMOOD Asad, YU Jiajun, WANG Yan, XIE Xiaofeng, SUN Jing. Two-dimensional g-C₃N₄ Compositing with Ag-TiO₂ as Deactivation Resistant Photocatalyst for Degradation of Gaseous Acetaldehyde [J]. Journal of Inorganic Materials, 2022, 37(8): 865-872.
[7]	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.
[8]	LIU Xuechen, ZENG Di, ZHOU Yuanyi, WANG Haipeng, ZHANG Ling, WANG Wenzhong. Selective Oxidation of Biomass over Modified Carbon Nitride Photocatalysts [J]. Journal of Inorganic Materials, 2022, 37(1): 38-44.
[9]	ZHANG Xian, ZHANG Ce, JIANG Wenjun, FENG Deqiang, YAO Wei. Synthesis, Electronic Structure and Visible Light Photocatalytic Performance of Quaternary BiMnVO₅ [J]. Journal of Inorganic Materials, 2022, 37(1): 58-64.
[10]	LIU Peng, WU Shimiao, WU Yunfeng, ZHANG Ning. Synthesis of Zn_0.4(CuGa)_0.3Ga₂S₄/CdS Photocatalyst for CO₂ Reduction [J]. Journal of Inorganic Materials, 2022, 37(1): 15-21.
[11]	CHEN Xiaomei, CHEN Ying, YUAN Xia. Decomposition of Cyclohexyl Hydroperoxide Catalyzed by Core-shell Material Co₃O₄@SiO₂ [J]. Journal of Inorganic Materials, 2022, 37(1): 65-71.
[12]	ZHOU Fan, BI Hui, HUANG Fuqiang. Ultra-large Specific Surface Area Activated Carbon Synthesized from Rice Husk with High Adsorption Capacity for Methylene Blue [J]. Journal of Inorganic Materials, 2021, 36(8): 893-903.
[13]	WANG Luping, LU Zhanhui, WEI Xin, FANG Ming, WANG Xiangke. Application of Improved Grey Model in Photocatalytic Data Prediction [J]. Journal of Inorganic Materials, 2021, 36(8): 871-876.
[14]	AN Weijia, LI Jing, WANG Shuyao, HU Jinshan, LIN Zaiyuan, CUI Wenquan, LIU Li, XIE Jun, LIANG Yinghua. Fe(III)/rGO/Bi₂MoO₆ Composite Photocatalyst Preparation and Phenol Degradation by Photocatalytic Fenton Synergy [J]. Journal of Inorganic Materials, 2021, 36(6): 615-622.
[15]	XIAO Xiang, GUO Shaoke, DING Cheng, ZHANG Zhijie, HUANG Hairui, XU Jiayue. CsPbBr₃@TiO₂ Core-shell Structure Nanocomposite as Water Stable and Efficient Visible-light-driven Photocatalyst [J]. Journal of Inorganic Materials, 2021, 36(5): 507-512.