微球状Br掺杂BiOCl复合光催化剂去除单质汞研究
X511; 光催化氧化法是治理大气环境汞污染问题的有效手段.目的 为开发低成本的可见光脱汞催化剂,方法 采用一步共沉淀法合成不同溴(Br)含量的BiOBrxCl1-x微球复合材料,在湿法光催化脱汞装置上考察它们在荧光灯辐照下的光催化活性,利用N2 吸附-脱附、XRD、UV-Vis DRS、SEM、HRTEM、XPS和ESR等技术对其结构进行分析,并采用密度泛函理论研究BiOCl和BiOBr之间的电荷转移规律.结果 结果表明,相较于BiOCl和BiOBr,BiOBrxCl1-x复合材料的光催化性能均得到提升,其中BiOBr0.2Cl0.8光催化剂的脱汞效率高达90.3%,较BiOCl提高了50%...
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| Published in | 河南理工大学学报（自然科学版） Vol. 43; no. 6; pp. 90 - 99 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | Chinese |
| Published |
河南理工大学 机械与动力工程学院,河南 焦作 454000
01.11.2024
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| Subjects | |
| Online Access | Get full text |
| ISSN | 1673-9787 |
| DOI | 10.16186/j.cnki.1673-9787.2022020067 |
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| Abstract | X511; 光催化氧化法是治理大气环境汞污染问题的有效手段.目的 为开发低成本的可见光脱汞催化剂,方法 采用一步共沉淀法合成不同溴(Br)含量的BiOBrxCl1-x微球复合材料,在湿法光催化脱汞装置上考察它们在荧光灯辐照下的光催化活性,利用N2 吸附-脱附、XRD、UV-Vis DRS、SEM、HRTEM、XPS和ESR等技术对其结构进行分析,并采用密度泛函理论研究BiOCl和BiOBr之间的电荷转移规律.结果 结果表明,相较于BiOCl和BiOBr,BiOBrxCl1-x复合材料的光催化性能均得到提升,其中BiOBr0.2Cl0.8光催化剂的脱汞效率高达90.3%,较BiOCl提高了50%;与 NO-3 和 SO2-4 相比,Cl-和 CO2-3 对 BiOBr0.2Cl0.8 光催化剂脱汞性能的抑制作用更显著;BiOBr0.2Cl0.8复合材料的比表面积均略高于BiOBr的和BiOCl的,较高的比表面积有利于光催化剂提供较多的活性位;随着Br含量逐渐增加,BiOCl的XRD特征峰强度逐渐减弱,复合材料的光吸收能力有规律地红移,表明BiOBr与BiOCl之间存在较强的相互作用,并非简单的机械混合;与BiOCl相比,BiOBr0.2Cl0.8复合材料的Bi 4f和O 1s均向高结合能方向偏移,表明引入Br影响了BiOCl中Bi和O的存在形态;3种活性物参与了Hg0的氧化脱除过程,其作用由大到小依次为·O-2,h+,·OH.结论 光催化活性的提高主要原因为BiOCl与BiOBr形成了Z型异质结,从而增强了光生电荷的分离.研究结果可为低成本、高效卤氧化铋基脱汞光催化剂的开发提供新思路. |
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| AbstractList | X511; 光催化氧化法是治理大气环境汞污染问题的有效手段.目的 为开发低成本的可见光脱汞催化剂,方法 采用一步共沉淀法合成不同溴(Br)含量的BiOBrxCl1-x微球复合材料,在湿法光催化脱汞装置上考察它们在荧光灯辐照下的光催化活性,利用N2 吸附-脱附、XRD、UV-Vis DRS、SEM、HRTEM、XPS和ESR等技术对其结构进行分析,并采用密度泛函理论研究BiOCl和BiOBr之间的电荷转移规律.结果 结果表明,相较于BiOCl和BiOBr,BiOBrxCl1-x复合材料的光催化性能均得到提升,其中BiOBr0.2Cl0.8光催化剂的脱汞效率高达90.3%,较BiOCl提高了50%;与 NO-3 和 SO2-4 相比,Cl-和 CO2-3 对 BiOBr0.2Cl0.8 光催化剂脱汞性能的抑制作用更显著;BiOBr0.2Cl0.8复合材料的比表面积均略高于BiOBr的和BiOCl的,较高的比表面积有利于光催化剂提供较多的活性位;随着Br含量逐渐增加,BiOCl的XRD特征峰强度逐渐减弱,复合材料的光吸收能力有规律地红移,表明BiOBr与BiOCl之间存在较强的相互作用,并非简单的机械混合;与BiOCl相比,BiOBr0.2Cl0.8复合材料的Bi 4f和O 1s均向高结合能方向偏移,表明引入Br影响了BiOCl中Bi和O的存在形态;3种活性物参与了Hg0的氧化脱除过程,其作用由大到小依次为·O-2,h+,·OH.结论 光催化活性的提高主要原因为BiOCl与BiOBr形成了Z型异质结,从而增强了光生电荷的分离.研究结果可为低成本、高效卤氧化铋基脱汞光催化剂的开发提供新思路. |
| Abstract_FL | Photocatalytic oxidation is an effective technology to control atmospheric mercury pollution.Objec-tives To develop a low-cost visible-light-driven mercury removal catalyst,Methods microspherical BiO-BrxCl1-x composite photocatalysts with different molar contents of bromine(Br)were synthesized by an one-step coprecipitation method,and their photocatalytic performances of Hg0 removal under fluorescent lamp(FSL)were implemented in a wet photocatalytic mercury removal device.The physical and chemical struc-tures of the samples were analyzed by N2 adsorption-desorption,XRD,UV-Vis DRS,SEM,HRTEM,XPS and ESR.Moreover,the charge transfer between BiOCl and BiOBr was studied using density functional theory.Results The results showed that compared with BiOCl and BiOBr,the photocatalytic performances of BiOBrxCl1-x composites were all improved,and the Hg0 removal efficiency of BiOBr0.2Cl0.8 photocatalyst reached as high as 90.3%,which was about 50%than that of pure BiOCl.Compared with NO3-and SO42-,Cl-and CO32-exhibited significant inhibitions on Hg0 removal.The specific surface area of BiOBr0.2Cl0.8 com-posites was slightly higher than that of BiOBr and BiOCl,which would be beneficial for providing more reac-tive sites.With the gradual increase of Br content,the XRD characteristic peak intensity of BiOCl gradually decreased,and the photocatalytic absorption capacity appeared redshift regularly,indicating a strong interac-tion between BiOBr and BiOCl,not a simple mechanical mixing.Both Bi 4f and O 1s of the BiOBr0.2Cl0.8 composite material were shifted towards higher binding energies,indicating that the introduction of Br af-fected the species of Bi and O in BiOCl.The mechanism analysis displayed that the three active species were involved in the oxidative process of Hg0 removal with the high-to-low order of·O-2,h+,·OH.Conclu-sions The improvement of photocatalytic activity was mainly due to the formation of Z-type heterojunction between BiOCl and BiOBr,which effectively enhanced the separation of photo-generated charges.The study provided a new idea for the development of low-cost and efficient bismuth oxyhalide-based photocatalysts for mercury removal. |
| Author | 刘艳雯 张丹 张景繁 郑海坤 张旭 张安超 孙志君 |
| AuthorAffiliation | 河南理工大学 机械与动力工程学院,河南 焦作 454000 |
| AuthorAffiliation_xml | – name: 河南理工大学 机械与动力工程学院,河南 焦作 454000 |
| Author_FL | ZHANG Xu LIU Yanwen ZHANG Jingfan SUN Zhijun ZHANG Dan ZHANG Anchao ZHENG Haikun |
| Author_FL_xml | – sequence: 1 fullname: ZHANG Anchao – sequence: 2 fullname: ZHANG Jingfan – sequence: 3 fullname: ZHANG Dan – sequence: 4 fullname: SUN Zhijun – sequence: 5 fullname: ZHANG Xu – sequence: 6 fullname: LIU Yanwen – sequence: 7 fullname: ZHENG Haikun |
| Author_xml | – sequence: 1 fullname: 张安超 – sequence: 2 fullname: 张景繁 – sequence: 3 fullname: 张丹 – sequence: 4 fullname: 孙志君 – sequence: 5 fullname: 张旭 – sequence: 6 fullname: 刘艳雯 – sequence: 7 fullname: 郑海坤 |
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| DOI | 10.16186/j.cnki.1673-9787.2022020067 |
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| DocumentTitle_FL | Study on the removal of elemental mercury by microspherical Br-doped BiOCl comosite photocatalyst |
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| Keywords | 单质汞脱除 光催化剂 氯氧化铋 BiOCl the removal of elemental mercury BiOBr 溴氧化铋 photocatalyst |
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| Title | 微球状Br掺杂BiOCl复合光催化剂去除单质汞研究 |
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