首页|SnO2QDs-g-C3N4/C的合成及其光催化降解四环素研究

SnO2QDs-g-C3N4/C的合成及其光催化降解四环素研究

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以二水合氯化锡(SnCl2·2H2O)为Sn源,芦蒿(artemisia selengensis)为生物模板诱导合成的g-C3N4/C(ACN)材料为载体,通过简单的水热法引入氧化锡量子点(SnO2QDs),制备了SnO2QDs/ACN复合材料。通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、光致发光光谱(PL)、氮气吸附-脱附测试(BET)和紫外-可见光漫反射光谱(UV-Vis DRS)等方法对材料的晶体结构、微观形貌和孔结构进行了表征。结果表明:SnO2QDs-g-C3N4/C材料已成功合成,生物碳骨架具有丰富且完整的介孔结构,SnO2QDs结晶度高且均匀锚定在生物碳表面,负载SnO2QDs后复合材料的比表面积增大、活性位点增加、载流子分离效率提升。通过对光催化降解效率及其反应动力学分析可知,7%SnO2QDs/ACN-2具有最高的四环素(TC)降解效率,达到56。5%。对比g-C3N4和ACN的光催化降解效率,分别达到其2。87倍和1。78倍。通过自由基捕获实验确定了复合材料降解四环素的主要活性物种为·O2-,而h+和·OH不参与反应。
Synthesis of SnO2QDs-g-C3N4/C and Its Photocatalytic Degradation of Tetracycline
Antibiotics have been widely used in clinical medicine,animal husbandry,and aquaculture since antibiotics were discov-ered.However,the abuse of antibiotics and the incomplete absorption of organisms have brought great harm and potential threat to or-ganisms in the environment.Therefore,the technology of removing residual antibiotics has drawn interesting attention.Among them,Photocatalytic degradation technology based on solar energy was designed to remove residual antibiotics from the environment.Catalyst materials play an important role in photocatalytic degradation technology,such as graphene,nano-diamond,carbon nano tube.Among them,graphite phase carbon nitride(g-C3N4)has attracted extensive attention due to its unique crystal structure,band structure,easy preparation,environmental protection,and low cost.However,the pure phase g-C3N4 has some disadvantages,such as low absorption of visible light,high recombination rate of photo-generated carriers,and low specific surface area reactive active sites,which serious-ly limited its application.In order to solve the problems,biological stems can be used as templates to adjust the morphology and size of g-C3N4 because biological stems have the advantages of uneven surface structure,high morphology similarity,low cost,and easy ac-cess.Meanwhile,metal oxide quantum could be adopted to g-C3N4 to adjust the energy band structure of semiconductors and reduce photo-carrier recombination through the quantum size effect,high surface activity,and special energy band structure.In this work,SnO2QDs/ACN was designed to be synthesized with SnCl2·2H2O as Sn source and g-C3N4/C(ACN)material as a carrier by simple hy-drothermal method.X-ray diffraction(XRD)was used to detect the crystal structure and chemical composition of SnO2QDs/ACN com-posites,and the microscopic morphology of SnO2QDs/ACN composites was observed by scanning electron microscopy(SEM)and transmission electron microscopy(TEM).The results of XRD,SEM,and TEM showed that SnO2QDs/ACN composites had been suc-cessfully synthesized and the biocarbon skeleton structure remained completely,while the lattice of SnO2QDs was anchored evenly on the carbon surface.Fluorescence spectrum test(PL)results showed that the emission peak intensity of 7%SnO2QDs/ACN-2 significant-ly decreased with the introduction of SnO2QDs,which proved that the carrier separation efficiency of SnO2QDs/ACN-2 further im-proved.The results of nitrogen adsorption-desorption test(BET)showed that 7%SnO2QDs/ACN-2 had high specific surface area,rich mesoporous structure and large specific surface area,resulting in increasing the contact area between the composites and the de-gradants to provide more active sites,and improve the photocatalytic activity of the materials.Based on the optical absorption theory,the band gap values of ACN-2(1.27 eV)and 7%SnO2QDs/ACN-2(1.50 eV)could be estimated by using Kubelka-Munk formula,which indicated the band gap of the composites was affected by with the quantum size effect of SnO2QDs.However,the band gap val-ues of 7%SnO2QDs/ACN-2 were still smaller than that of g-C3N4.The results showed that the electron transition of 7%SnO2QDs/ACN-2 required low energy.Therefore,it was easy to produce photogenerated charge carriers under visible light irradiation under the action.,the photogenerated electron-hole pair was not easy to recombine and obtained a longer life to improve efficient photocatalytic ability.To further reveal the mechanism of the photocatalytic reaction,the role of each free radical in the catalytic reaction was studied by adding quenching agent.The results showed that h+and·OH did not participate in the reaction and·O2-played a decisive role in the reaction.When the semiconductor exposed to visible light irradiation,the electrons were excited from valance band to the conduction band of g-C3N4 and then the electrons of the conduction band of g-C3N4 transferred to the conduction band of SnO2QDs.The conduction potential of SnO2QDs(-0.38 eV)and g-C3N4(-1.37 eV)was higher than that of E(O2/O2-),the resulting electrons could easily move to the sur-face of the material through highly conductive biological carbon.Where they could react with O2 to form·O2-.Through the analysis of photocatalytic degradation efficiency and reaction kinetics of SnO2QDs/ACN-2 for tetracycline within 30 min,7%SnO2QDs/ACN-2 showed the highest degradation efficiency and could degrade 56.5%tetracycline,which was 2.87 times that of g-C3N4 and 1.78 times that of ACN-2.The results showed that SnO2QDs/ACN-2 with good photocatalytic degradation effect and stability had been successfully constructed,which was a potential candidate material for tetracycline purification.

g-C3N4biological template methodtin oxide quantum dotsphotocatalytic degradationtetracycline

于巧玲、刘成宝、曹一达、郑磊之、陈丰、钱君超、邱永斌、孟宪荣、陈志刚

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苏州科技大学材料科学与工程学院,江苏省环境功能材料重点实验室,江苏苏州 215009

苏州科技大学江苏水处理技术与材料协同创新中心,江苏苏州 215009

江苏省陶瓷研究所有限公司,江苏宜兴 214221

苏州市环境科学研究所,江苏苏州 215007

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石墨相氮化碳 生物模板法 SnO2量子点 光催化降解 四环素

江苏省自然科学基金项目江苏省自然科学基金项目苏州市科技发展计划项目(民生科技—关键技术应用研究)

BK20180103BK20180971SS202036

2024

稀有金属
北京有色金属研究总院

稀有金属

CSTPCD北大核心
影响因子:1.483
ISSN:0258-7076
年,卷(期):2024.48(8)