层级纳米花环状Bi2O3/(BiO)2CO3复合材料光催化降解罗丹明B
Hierarchical Nanoflower-Ring Structure Bi2O3/(BiO)2CO3 Composite for Photocatalytic Degradation of Rhodamine B
作者单位E-mail
宋强 齐齐哈尔大学材料科学与工程学院, 齐齐哈尔 161006;齐齐哈尔大学化学与化学工程学院, 齐齐哈尔 161006  
李莉 齐齐哈尔大学材料科学与工程学院, 齐齐哈尔 161006;齐齐哈尔大学化学与化学工程学院, 齐齐哈尔 161006;黑龙江省高校精细化工重点实验室, 齐齐哈尔 161006 qqhrll@163.com 
罗鸿祥 齐齐哈尔大学化学与化学工程学院, 齐齐哈尔 161006  
刘越 齐齐哈尔大学化学与化学工程学院, 齐齐哈尔 161006  
杨长龙 齐齐哈尔大学材料科学与工程学院, 齐齐哈尔 161006  
摘要: 通过程序升温水热法制备了层级纳米花状结构Bi2O3/(BiO)2CO3复合材料(简称BO/BCO)。采用X射线衍射(XRD)、紫外-可见漫反射吸收光谱(UV-Vis/DRS)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和氮气吸附-脱附测定等方法对上述合成材料的晶型结构、组成、光吸收性质、形貌和表面物理化学性质进行了表征。结果表明,该复合材料中(BiO)2CO3的晶型为四方相,Bi2O3的晶型为单斜相,复合后的材料同时具有两者晶型结构。并且,合成时随着OH-的引入与反应时间的增加,复合材料中(BiO)2CO3的特征衍射峰强度逐渐降低,Bi2O3的特征衍射峰强度逐渐增加,证明了Bi2O3在样品中所占比例的增加。从UV-Vis/DRS吸收光谱分析结果显示,与单体(BiO)2CO3和单体Bi2O3相比,合成的BO/BCO复合材料的吸收边带发生偏移,且Bi2O3的引入有效增加其可见光区吸收。同时,样品由片状(BiO)2CO3生长为层级纳米花环状结构的BO/BCO-0.5,而层级结构的形成导致BO/BCO-0.5的带隙能变窄,且对于光电子的反射与散射发生改变,从而有利于光生电荷的转移与光的吸收效率。另外,以罗丹明B为模型分子,通过不同光源照射下的光催化活性实验,循环实验以及捕获实验对复合材料BO/BCO的光催化活性进行了研究。结果表明,与其他体系(单体Bi2O3和P25)相比,BO/BCO-0.5活性有明显提高,并且在多次循环实验后依然保持良好的稳定性。此外,根据捕获实验结果推测了BO/BCO复合材料可能的光催化反应机理。
关键词: 程序升温水热法  氧化铋  碳酸氧铋  层级纳米花环状结构  光催化降解  罗丹明B
基金项目: 国家自然科学基金(21376126),黑龙江省自然科学基金(B201106、B201314),黑龙江省教育厅科学技术研究项目(12511592),黑龙江省政府博士后资助经费(LBH-Z11108),黑龙江省普通高校绿色化工技术重点实验室开放课题资助项目(2013年),黑龙江省政府博士后科研启动金(LBH-Q13172)和齐齐哈尔大学大学生创新创业训练计划项目(201610221112)
Abstract: Hierarchical nanoflower-ring structure Bi2O3/(BiO)2CO3(BO/BCO) composite was successfully synthesized by the temperature-programmed hydrothermal treatment.X-ray diffraction (XRD),UV-Vis diffuse reflectance spectroscopy (UV-Vis/DRS),X-ray photoelectron spectroscopy (XPS),Scanning electron microscopy (SEM),Transmission electron microscopy (TEM) and N2 adsorption-desorption tests were employed to characterize the crystalline phase,chemical composition,optical absorption properties,morphology and surface physicochemical properties of as-synthetized material.The results showed that the crystalline phase of (BiO)2CO3 was tetragonal phase,and the crystalline phase of Bi2O3 was the monoclinic phase in as-composite Bi2O3/(BiO)2CO3 which had both as-crystal structures.Moreover,with the introduction of OH- and reaction time increasing in synthesis process,the intensity of characteristics diffraction peak of (BiO)2CO3 was gradually decreased,meanwhile,that of Bi2O3 was gradually increased,showing that the proportions of Bi2O3 were increased in the sample with reaction time increased.The results of UV-Vis/DRS analysis showed that the absorption edge of as-synthetized composite BO/BCO had shift compared to pure Bi2O3 and pure (BiO)2CO3,and the absorption was effectively increased in the visible light region with the introduction of Bi2O3.At the same time,(BiO)2CO3 nanolayer was changed to the hierarchical nanoflower-ring structure BO/BCO-0.5 composite,and the formation of special morphology leads to narrowed band gap and change the reflection and scattering of photoelectrons,which were conducive to the absorption efficiency of light and transfering of photogenerated charges.In addition,the photocatalytic activities of as-composites BO/BCO were studied by degradation photocatalytic experiments of RhB as the model molecule under different light irradiation,the cycle experiment and the capture experiment.The results of photocatalytic activity experiment showed that the activity of BO/BCO-0.5 was significantly higher than that of other systems (Bi2O3 and P25),and the photocatalytic activity of BO/BCO-0.5 was kept even after three cycles.Meanwhile,according to the capture experimental results,the possible photocatalytic reaction mechanism of BO/BCO composite was speculated.
Keywords: temperature-programmed hydrothermal treatment  bismuth oxide  bismuth subcarbonate  hierarchical nanoflower-ring structure  photocatalytic degradation  rhodamine B
投稿时间:2016-12-20 修订日期:2017-03-16
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宋强,李莉,罗鸿祥,刘越,杨长龙.层级纳米花环状Bi2O3/(BiO)2CO3复合材料光催化降解罗丹明B[J].无机化学学报,2017,33(7):1161-1171.
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