Preparation of g-C3N4/Ag/TiO2 NTs and Photocatalytic Degradation of Ceftazidine

doi:10.11901/1005.3093.2021.139

Chinese Journal of Materials Research

2022, Vol. 36

Issue (5): 392-400 DOI: 10.11901/1005.3093.2021.139

ARTICLES

Current Issue | Archive | Adv Search

Preparation of g-C₃N₄/Ag/TiO₂ NTs and Photocatalytic Degradation of Ceftazidine

TAN Chong¹, LI Yuanyuan¹, WANG Huanhuan¹, LI Junsheng², XIA Zhi², ZUO Jinlong²(

), YAO Lin³

^1.School of Pharmacy (Pharmaceutical Engineering Technology Research Center), Harbin University of Commerce, Harbin 150076, China
^2.School of Food Science and Engineering, Harbin University of Commerce, Harbin 150076, China
^3.College of Life Science and Technology, Harbin Normal University, Harbin 150025, China

Cite this article:

TAN Chong, LI Yuanyuan, WANG Huanhuan, LI Junsheng, XIA Zhi, ZUO Jinlong, YAO Lin. Preparation of g-C₃N₄/Ag/TiO₂ NTs and Photocatalytic Degradation of Ceftazidine. Chinese Journal of Materials Research, 2022, 36(5): 392-400.

Download:

HTML

PDF(5788KB)
Export: BibTeX | EndNote (RIS)

Abstract

Titanium oxide nano-tubes (TiO₂NTs) were firstly prepared by anodic oxidation method, and then Ag and carbonitride g-C₃N₄ were deposited onto TiO₂ NTs under the synergistic action of ultraviolet irradiation and microwave heating to prepare the ternary composite photocatalyst g-C₃N₄/Ag/TiO₂ NTs. Then the prepared composites were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), UV Vis diffuse reflectance spectroscopy (UV-Vis) and photoluminescence spectroscopy (PL).The results show that the composite of g-C₃N₄/Ag/TiO₂ NTs presents a higher degradation rate of 51.8% for the carbaryl under the simulated sunlight, in the contrast, that of the simple TiO₂ NTs is 29.1% only. The improvement of photocatalytic activity is related to the combined effect of the surface plasmon resonance effect of Ag, the excellent charge conductivity of Ag and the formation of heterojunction between g-C₃N₄ and TiO₂ NTs.

Key words: inorganic nonmetallic materials TiO₂ Ag g-C₃N₄ carbaryl photocatalysis

Received: 07 February 2021

ZTFLH:

X703

Fund: Natural Science Foundation of Heilongjiang Province(QC2018021)

About author: ZUO Jinlong, Tel: (0971)6307663, E-mail: zuojinlongnjc@163.com

	Service

	E-mail this article
	Add to citation manager
	E-mail Alert
	RSS
	（）
	Articles by authors
	Chong TAN
	Yuanyuan LI
	Huanhuan WANG
	Junsheng LI
	Zhi XIA
	Jinlong ZUO
	Lin YAO

URL:

https://www.cjmr.org/EN/10.11901/1005.3093.2021.139 OR https://www.cjmr.org/EN/Y2022/V36/I5/392

Fig.1 XRD spectrum of g-C₃N₄ (a),_{TiO₂NTs (b), Ag/TiO₂ NTs (c) and g-C₃N₄/Ag/TiO₂ NTs (d) samples}

Fig.2 SEM image of g-C₃N₄ (a), TiO₂ NTs (b), Ag/TiO₂ NTs (c) and g-C₃N₄/Ag/TiO₂ NTs (d)

Fig.3 TEM image of the g-C₃N₄/Ag/TiO₂ NTs sample

Fig.4 EDS spectrum and element distribution of g-C₃N₄/Ag/TiO₂ (a) C, (b) O, (c) Ti, (d) Ag, (e) N

Fig.5 XPS full spectra of TiO₂ NTs and g-C₃N₄/Ag/TiO₂ NTs (a) and high resolution spectrum of O 1s (b)、Ti 2p (c)、Ag 3d (d)、C 1s (e)、N 1s (f)

Fig.6 UV-Vis DRS spectra (a) and estimated band gap (b) of TiO₂ NTs、Ag/TiO₂ NTs and g-C₃N₄/Ag/TiO₂ NTs

Fig.7 Degradation curves (a) and kinetic analysis (b) of TiO₂ NTs、Ag/TiO₂ NTs and g-C₃N₄/Ag/TiO₂ NTs for carbaryl

Table 1 Photocatalytic degradation kinetic parameters of TiO₂ NTs、Ag/TiO₂ NTs和g-C₃N₄/Ag/TiO₂ NTs

Fig.8 Relationship between the photocatalytic performance of catalysts and reuse numbers

Fig.9 Photoluminescence spectra of TiO₂ NTs、Ag/TiO₂ NTs and g-C₃N₄/Ag/TiO₂ NTs

Fig.10 Free radical scavenging rate

Fig.11 Photoelectrocatalysis mechanism

Fig.12 Chromatogram standard map (a), chromato-gram map (b, c) and product mass spectrum (d) of carbaryl

Fig.13 Degradative pathway (a) and hydrolytic pathway (b) of carbaryl

1	Ruengprapavut S, Sophonnithiprasert T, Pongpoungphet N. The effectiveness of chemical solutions on the removal of carbaryl residues from cucumber and chili presoaked in carbaryl using the HPLC technique [J]. Food Chem., 2019, 30: 125659
2	Şolpan D, Ibrahim K E A, Torun M, et al. The effect of ozonation on the degradation of carbaryl in aqueous solution [J]. J. Environ. Sci. Health, 2020, 55B: 929
3	Wu P, Chen Z B, Zhang Y, et al. RETRACTED: carbaryl waste-water treatment by Rhodopseudomonas sphaeroides [J]. Chemosphere, 2019, 233: 597 doi: 10.1016/j.chemosphere.2019.05.237
4	Wu P, Xie L Y, Mo W T, et al. The biodegradation of carbaryl in soil with Rhodopseudomonas capsulata in wastewater treatment effluent [J]. J. Environ. Manag., 2019, 249: 109226 doi: 10.1016/j.jenvman.2019.06.127
5	Zhang P, Wu J Y, Li L, et al. Sorption and catalytic hydrolysis of carbaryl on pig-manure-derived biochars [J]. J. Agro-Environ. Sci., 2012, 31: 416
	张鹏, 武健羽, 李力等. 猪粪制备的生物炭对西维因的吸附与催化水解作用 [J]. 农业环境科学学报, 2012, 31: 416
6	Su Z, Hu K D, Zhu J W, et al. Environmental conditions of carbaryl degradation by bacillus licheniformis B-1 [J]. Jiangsu J. Agr. Sci., 2018, 34: 585
	苏赵, 胡凯弟, 朱佳雯等. 地衣芽孢杆菌B-1降解西维因的环境条件 [J]. 江苏农业学报, 2018, 34: 585
7	Yurdakal S, Tek B S, Değirmenci Ç, et al. Selective photocatalytic oxidation of aromatic alcohols in solar-irradiated aqueous suspensions of Pt, Au, Pd and Ag loaded TiO₂ catalysts [J]. Catal. Today, 2017, 281: 53 doi: 10.1016/j.cattod.2016.05.054
8	Ali A, Shoeb M, Li Y, et al. Enhanced photocatalytic degradation of antibiotic drug and dye pollutants by graphene-ordered mesoporous silica (SBA 15)/TiO₂ nanocomposite under visible-light irradiation [J]. J. Mol. Liq., 2021, 324: 114696 doi: 10.1016/j.molliq.2020.114696
9	Chen Z S, Liang X P, Fan X W, et al. Fabrication and photocatalytic properties of Ce-La-Ag Co-doped TiO₂/basalt fiber composite photocatalyst [J]. Chin. J. Mater. Res., 2019, 33: 515
	陈子尚, 梁小平, 樊小伟等. Ce-La-Ag共掺杂TiO₂/玄武岩纤维复合光催化剂的制备和性能 [J]. 材料研究学报, 2019, 33: 515 doi: 10.11901/1005.3093.2018.588
10	Yurdakal S, Yanar Ş Ö, Çetinkaya S, et al. Green photocatalytic synthesis of vitamin B₃ by Pt loaded TiO₂ photocatalysts [J]. Appl. Catal., 2017, 202B: 500
11	Liang H J, Jia Z C, Zhang H C, et al. Photocatalysis oxidation activity regulation of Ag/TiO₂ composites evaluated by the selective oxidation of Rhodamine B [J]. Appl. Surf. Sci., 2017, 422: 1 doi: 10.1016/j.apsusc.2017.05.211
12	Zhu Y P, Zhu R L, Yan L X, et al. Visible-light Ag/AgBr/ferrihydrite catalyst with enhanced heterogeneous photo-fenton reactivity via electron transfer from Ag/AgBr to ferrihydrite [J]. Appl. Catal., 2018, 239B: 280
13	Huang B T, Xiao L L, Dong H F, et al. Electrochemical sensing platform based on molecularly imprinted polymer decorated N,S co-doped activated graphene for ultrasensitive and selective determination of cyclophosphamide [J]. Talanta, 2017, 164: 601 doi: 10.1016/j.talanta.2016.11.009
14	Zhu X D, Wang J, Ma Y, et al. Influence of heat treatment on photocatalytic activity of Ag-ZnO heterostructure [J]. Chin. J. Mater. Res., 2020, 34: 770
	朱晓东, 王娟, 马洋等. 热处理对Ag-ZnO异质结构光催化性能的影响 [J]. 材料研究学报, 2020, 34: 770 doi: 10.11901/1005.3093.2020.132
15	Kong J H, Song C X, Zhang W, et al. Enhanced visible-light-active photocatalytic performances on Ag nanoparticles sensitized TiO₂ nanotube arrays [J]. Superlattices Microstruct., 2017, 109: 579 doi: 10.1016/j.spmi.2017.05.050
16	Sun Y, Gao Y, Zeng J Y, et al. Enhancing visible-light photocatalytic activity of Ag-TiO₂ nanowire composites by one-step hydrothermal process [J]. Mater. Lett., 2020, 279: 128506 doi: 10.1016/j.matlet.2020.128506
17	Zhu Z, Lu Z Y, Wang D D, et al. Construction of high-dispersed Ag/Fe₃O₄/g-C₃N₄ photocatalyst by selective photo-deposition and improved photocatalytic activity [J]. Appl. Catal., 2016, 182B: 115
18	Peng Z T, Gao Y R, Yao C, et al. Preparation and photocatalytic activity of Fe/Yb Co-doped titanium dioxide hollow sphere [J]. Chin. J. Mater. Res., 2021, 35: 135
	彭子童, 郜艳荣, 姚楚等. 铁/镱掺杂二氧化钛空心球的制备及其光催化性能 [J]. 材料研究学报, 2021, 35: 135 doi: 10.11901/1005.3093.2020.333
19	Sun X F, Xian T, Di L J, et al. Photocatalytic degradation and reduction properties of AuAg/Bi₂O₃ composite [J]. Chin. J. Mater. Res., 2020, 34: 921
	孙小锋, 县涛, 邸丽景等. AuAg/Bi₂O₃复合材料的光催化降解和还原性能 [J]. 材料研究学报, 2020, 34: 921
20	Peng Z T, Gao Y R, Yao C, et al. Preparation and photocatalytic activity of Fe/Yb Co-doped titanium dioxide hollow sphere [J]. Chin. J. Mater. Res., 2021, 35: 135
	彭子童, 郜艳荣, 姚楚等. 铁/镱掺杂二氧化钛空心球的制备及其光催化性能 [J]. 材料研究学报, 2021, 35: 135 doi: 10.11901/1005.3093.2020.333
21	Cui Z K, Mi L W, Fa W J, et al. Preparation and photocatalytic performance of Pt/BiOCl nanostructures [J]. Chin. J. Mater. Res., 2013, 27: 583
	崔占奎, 米立伟, 法文君等. Pt/BiOCl纳米结构的制备及其光催化性能 [J]. 材料研究学报, 2013, 27: 583
22	Tian T. The research of silver-loading, photoelectric and antibacterial properties of TiO₂ nanotube arrays [D]. Xi'an: Northwestern Polytechnical University, 2016
	田甜. TiO₂纳米管阵列的银负载、光电及抗菌性能研究 [D]. 西安: 西北工业大学, 2016
23	Mou H Y, Song C X, Zhou Y H, et al. Design and synthesis of porous Ag/ZnO nanosheets assemblies as super photocatalysts for enhanced visible-light degradation of 4-nitrophenol and hydrogen evolution [J]. Appl. Catal., 2018, 221B: 565.
24	Zada A, Ali N, Subhan F, et al. Suitable energy platform significantly improves charge separation of g-C₃N₄ for CO₂ reduction and pollutant oxidation under visible-light [J]. Prog. Nat. Sci., 2019, 29: 138 doi: 10.1016/j.pnsc.2019.03.004
25	Sun M Q, Shen S L, Wu Z J, et al. Rice spike-like g-C₃N₄/TiO₂ heterojunctions with tight-binding interface by using sodium titanate ultralong nanotube as precursor and template [J]. Ceram. Int., 2018, 44: 8125 doi: 10.1016/j.ceramint.2018.01.257
26	Troppová I, Šihor M, Reli M, et al. Unconventionally prepared TiO₂/g-C₃N₄ photocatalysts for photocatalytic decomposition of nitrous oxide [J]. Appl. Surf. Sci., 2018, 430: 335 doi: 10.1016/j.apsusc.2017.06.299
27	Qi F, An W J, Wang H, et al. Combing oxygen vacancies on TiO₂ nanorod arrays with g-C₃N₄ nanosheets for enhancing photoelectrochemical degradation of phenol [J]. Mater. Sci. Semicond. Process., 2020, 109: 104954 doi: 10.1016/j.mssp.2020.104954
28	Li Y N, Chen Z Y, Wang M Q, et al. Interface engineered construction of porous g-C₃N₄/TiO₂ heterostructure for enhanced photocatalysis of organic pollutants [J]. Appl. Surf. Sci., 2018, 440: 229 doi: 10.1016/j.apsusc.2018.01.106
29	Tahir M. Well-designed ZnFe₂O₄/Ag/TiO₂ nanorods heterojunction with Ag as electron mediator for photocatalytic CO₂ reduction to fuels under UV/visible light [J]. J. CO₂ Utilizat., 2020, 37: 134
30	Liu C, Dong S S, Chen Y G. Enhancement of visible-light-driven photocatalytic activity of carbon plane/g-C₃N₄/TiO₂ nanocomposite by improving heterojunction contact [J]. Chem. Eng. J., 2019, 371: 706 doi: 10.1016/j.cej.2019.04.089
31	Hu J J, Ma C Y, Wang J L, et al. Preparation and photocatalytic properties of GO/TiO₂-g-C₃N₄ nanocomposites [J]. Chin. J. Inorg. Chem., 2020, 36: 2240
	胡金娟, 马春雨, 王佳琳等. GO/TiO₂-g-C₃N₄纳米复合材料的制备及可见光催化性能 [J]. 无机化学学报, 2020, 36: 2240
32	Liu H. Preparation of Ag@AgBr/ZnO and its photocatalytic oxidation performance [D]. Harbin: Harbin University of Commerce, 2020
	刘昊. Ag@AgBr/ZnO的制备及光催化氧化性能的研究 [D]. 哈尔滨: 哈尔滨商业大学, 2020.
33	Akhundi A, Habibi-Yangjeh A. Novel magnetic g-C₃N₄/Fe₃O₄/AgCl nanocomposites: facile and large-scale preparation and highly efficient photocatalytic activities under visible-light irradiation [J]. Mater. Sci. Semicond. Process., 2015, 39: 162 doi: 10.1016/j.mssp.2015.04.052
34	Miller P L, Chin Y P. Photoinduced degradation of carbaryl in a wetland surface water [J]. J. Agric. Food Chem., 2002, 50: 6758 doi: 10.1021/jf025545m

[1]	LU Yimin, MA Lifang, WANG Hai, XI Lin, XU Manman, YANG Chunlai. Carbon-base Protective Coating Grown by Pulsed Laser Deposition on Copper Substrate[J]. 材料研究学报, 2023, 37(9): 706-712.
[2]	YANG Dongtian, XIONG Liangyin, LIAO Hongbin, LIU Shi. Improved Design of CLF-1 Steel Based on Thermodynamic Simulation[J]. 材料研究学报, 2023, 37(8): 590-602.
[3]	REN Fuyan, OUYANG Erming. Photocatalytic Degradation of Tetracycline Hydrochloride by g-C₃N₄ Modified Bi₂O₃[J]. 材料研究学报, 2023, 37(8): 633-640.
[4]	GUO Fei, ZHENG Chengwu, WANG Pei, LI Dianzhong. Effect of Rare Earth Elements on Austenite-Ferrite Phase Transformation Kinetics of Low Carbon Steels[J]. 材料研究学报, 2023, 37(7): 495-501.
[5]	ZHANG Min, ZHANG Siqian, WANG Dong, CHEN Lijia. Creep Microstructure Damage and Influence on Re-creep Behavior for a Nickel-based Single Crystal Superalloy[J]. 材料研究学报, 2023, 37(6): 417-422.
[6]	YANG Baolei, LIU Tingguang, SU Xianglin, FAN Yu, QIU Liang, LU Yonghao. Effect of Thermal Aging on Mechanical Properties and Intergranular Corrosion Resistance of 316LN[J]. 材料研究学报, 2023, 37(5): 381-390.
[7]	LI Pengyu, LIU Zitong, KANG Shumei, CHEN Shanshan. Effect of Plasma Treatment on Performance of Polybutylene Adipate Coating on Biomedical AZ31 Mg-alloy[J]. 材料研究学报, 2023, 37(4): 271-280.
[8]	LIAO Hongyu, JIA Yongxin, SU Ruiming, LI Guanglong, QU Yingdong, LI Rongde. Effect of Retrogression Times on Microstructure and Corrosion Resistance of 2024 Aluminum Alloy[J]. 材料研究学报, 2023, 37(4): 264-270.
[9]	ZHU Mingxing, DAI Zhonghua. Study on Energy Storage Properties of SrSC_0.5Nb_0.5O₃ Modified BNT-based Lead-free Ceramics[J]. 材料研究学报, 2023, 37(3): 228-234.
[10]	MA Yizhou, ZHAO Qiuying, YANG Lu, QIU Jinhao. Preparation and Dielectric Energy Storage Properties of Thermoplastic Polyimide/Polyvinylidene Fluoride Composite Film[J]. 材料研究学报, 2023, 37(2): 89-94.
[11]	LIU Huan, LI Xingfu, YANG Yi, LI Cong, FU Zhengrong, BAI Yunhua, ZHANG Zhenghong, ZHU Xinkun. Room Temperature Work-Hardenning Behavior of a Novel Sandwich Sheet of Cu-Al Alloy with Gradient Structure Surfaces on Both Sides[J]. 材料研究学报, 2023, 37(2): 95-101.
[12]	CHEN Ruizhi, LIU Lirong, GUO Shengdong, ZHANG Mai, LU Guangxian, LI Yuan, ZHAO Yunsong, ZHANG Jian. Microstructural Stability and Stress Rupture Property of a 6Re/3Ru Containing Nickel-based Single Crystal Superalloy[J]. 材料研究学报, 2023, 37(10): 721-730.
[13]	YAN Chunliang, GUO Peng, ZHOU Jingyuan, WANG Aiying. Electrical Properties and Carrier Transport Behavior of Cu Doped Amorphous Carbon Films[J]. 材料研究学报, 2023, 37(10): 747-758.
[14]	LIU Zhihua, YUE Yuanchao, QIU Yifan, BU Xiang, YANG Tao. Preparation of g-C₃N₄/Ag/BiOBr Composite and Photocatalytic Reduction of Nitrate[J]. 材料研究学报, 2023, 37(10): 781-790.
[15]	ZHOU Yi, TU Qiang, MI Zhonghua. Effect of Preparing Methods on Structure and Properties of Phosphate Glass-ceramics[J]. 材料研究学报, 2023, 37(10): 739-746.

No Suggested Reading articles found!

Viewed

Full text

Abstract

Cited

Shared

Discussed