Fe物种改性海胆状Nb2O5光催化降解类吩噻嗪染料
Photocatalytic Degradation of Quasi-phenothiazine Dyes by Fe Species Modified Urchin-like Nb2O5 Nanospheres
作者单位E-mail
畅通 运城学院应用化学系, 运城 044000  
牛浩通 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 太原 030001
太原理工大学材料科学与工程学院, 太原 030024 
 
马瑞婧 运城学院物理与电子工程系, 运城 044000  
王会香 中国科学院山西煤炭化学研究所煤转化国家重点实验室, 太原 030001 wanghx@sxicc.ac.cn 
吕宝亮 运城学院应用化学系, 运城 044000
中国科学院山西煤炭化学研究所煤转化国家重点实验室, 太原 030001 
lbl604@sxicc.ac.cn 
摘要: 我们在合成海胆状Nb2O5纳米球光催化剂的基础上,向体系中直接引入Fe3+离子,制备了Fe物种修饰的Nb2O5纳米球。对产物进行了X射线粉末衍射(XRD)、傅里叶变换红外光谱(FT-IR)、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)、N2吸附-脱附测试、紫外可见吸收谱(UV-Vis)和光致发光谱(PL)表征。结果表明,引入Fe3+后,Nb2O5纳米球的微观形貌和晶型结构没有发生显著变化,但其比表面积有所增加,原位复合的Fe物种以低结晶度的Fe2O3和Fe(Ⅱ)NbxOy物种分布在Nb2O5纳米球表面。相比于单一海胆状Nb2O5,Fe物种修饰的Nb2O5催化剂表现出了良好的光催化活性,能高效且选择性地降解类吩噻嗪染料亚甲基蓝(MB)和甲苯胺蓝(TB),原因为:(1) Fe物种可以对类吩噻嗪染料分子中的N和S形成配位吸附;(2) Fe物种与Nb2O5导带匹配,可以有效分离其光生电子,提高空穴的氧化能力;(3) Fenton反应在快速消耗光生电子的同时产生大量·OH用于染料的氧化。
关键词: 五氧化二铌  表面化学  光催化  吩噻嗪染料  Fenton反应
基金项目: 国家自然科学基金(No.21972158)、山西省青年基金(No.201901D211583)、山西省优秀博士启动基金(No.SQ2019006)和运城学院(No.YQ-2018013)资助。
Abstract: Herein, Fe species modified urchin-like Nb2O5 nanospheres were prepared by directly introducing Fe3+ cations into the system on the basis of synthesizing urchin-like Nb2O5 nanospheres via hydrothermal method. The synthesized samples were characterized in detail by power X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N2 adsorption-desorption test, X-ray photoelectron spectroscopy (XPS), UV-Vis absorption spectroscopy (UV-Vis) and photoluminescence emission spectroscopy (PL). The results indicated that Fe3+ cations had no obvious effect on the morphology and hexagonal structure of Nb2O5, but could increase the specific surface area of samples. The Fe species of Fe2O3 and Fe(Ⅱ)NbxOy with low crystallinity were most likely to be form in situ on the Nb2O5 surface during the experiment and uniformly dispersed. Compared with pure urchin-like Nb2O5 nanospheres, the Fe species modified Nb2O5 samples exhibited high photocatalytic activity under full light irradiation, and they could selectively degrade quasiphenothiazine dyes of methylene blue (MB) and toluidine blue (TB) with a high efficiency. One of the reasons is that Fe species can form coordination adsorption with N and S in quasi-phenothiazine dye molecules. Moreover, Fe species can separate photoexcited electrons of Nb2O5 and then decrease the recombination of photoexcited electron/hole by their matched conduction band (CB) with Nb2O5, and leading to the improvement of hole oxidation activity. Furthermore, Fenton reaction under the presence of trace H2O2 quickly consumes photoelectrons and generates a number of·OH radicals to oxidize dye molecules.
Keywords: Nb2O5  surface chemistry  photocatalysis  phenothiazine dyes  Fenton reaction
投稿时间:2020-12-01 修订日期:2021-01-06
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畅通,牛浩通,马瑞婧,王会香,吕宝亮.Fe物种改性海胆状Nb2O5光催化降解类吩噻嗪染料[J].无机化学学报,2021,37(4):717-727.
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