核黄素及AQS介导P25光电子还原铀(Ⅵ)研究  

Research on riboflavin and AQS mediated P25 photocatalytic reduction of uranium(Ⅵ)

作　　者：王萍萍[1,2] 董发勤 何辉超[2] 刘明学[2] 罗昭培[1] 王旭辉[2] 周磊[1,2] 霍婷婷 WANG Pingping;DONG Faqin;HE Huichao(School of Environment and Resources, Southwest University of Science and Technology, Mianyang Sichuan 621010,China;Key Laboratory of Solid Waste Treatment and Resources Recycle, Mianyang Sichuan 621010,China)

机构地区：[1]西南科技大学环境与资源学院,四川绵阳621010 [2]固体废物处理与资源化教育部重点实验室,四川绵阳621010

出　　处：《化工矿物与加工》2019年第4期59-64,共6页Industrial Minerals & Processing

基　　金：国家自然科学基金项目(2014CB846003)

摘　　要：光催化还原铀(Ⅵ)因其具有清洁无二次污染、耗能少、处理迅速等优点而备受关注。本文以典型电子穿梭体核黄素(RF)与蒽醌-2-磺酸钠(AQS)作为研究对象,利用电化学、扫描电镜(SEM)、红外光谱(FTIR)与X射线光电子能谱(XPS)等方法考察RF与AQS在水溶液中的氧化还原行为,以及在RF与AQS介导下P25光电子对U(Ⅵ)还原率及还原产物的影响。结果表明:循环伏安(CV)分析证实RF与AQS具有氧化还原活性,其峰电流j_(op)和-j_(rp)vs.v^(1/2)线性关系较好,符合Randles Sevcik的控制扩散反应公式。RF与AQS能够促进P25光电子对U(Ⅵ)的还原,反应24h,光电子对U(Ⅵ)的还原率均大于90%,与对照相比还原率分别提高了9.79%与7.79%。SEM分析表明,P25光电子还原U(Ⅵ)在对电极上生成了薄片状、针柱状结晶矿物;EDS分析表明其为含U矿物;XRD分析还原产物为(UO_2)_8O_2(OH)_(12)·12H_2O与UO_2;FTIR分析表明,还原作用后472.4cm^(-1)处吸收峰为U^(4+)—O键的特征振动峰,913.9cm^(-1)处吸收峰为UO_2^(2+)中U=O的红外伸缩振动峰,光电子还原铀产物主要以U(IV)与U(Ⅵ)矿物形式存在;XPS分析也证明光电子还原铀产物以U(IV)与U(Ⅵ)矿物形式存在。Photocatalytic reduction U(VI) has attracted much attention due to its advantages such as no secondary pollution, less energy consumption and rapid ireaiment. Based on the typical electron shuttle body riboflavin (RF) and anthraquinone-2- sulfonic acid sodium (AQS) as the research object, electrochemical and scanning electron microscopy (SEM). infrared spectra (FTIR) and X-ray photoelectron spectroscopy ( XPS) and other methods were used to investigate the REDOX behaviors of RF and AQS in aqueous solution and the influence of P25 optoelectronics mediated by RF and AQS on U(VI) reduction rate and ihe reduction products. The results show that cyclic voltammetry (CV) analysis confirms that RF and AQS have REDOX activity,and the linear relationship between peak current jop and -jrp vs.v1/2 is good. which conforms to Randles Sevcik controlled diffusion reaction formula. RF and AQS can promote the reduction of U( VI) by P25 photoelectron. After the reaction for 24 h, the reduction rate of U(VI) of photoelectron is greater than 90%. The reduction rate of photoelectron pair U(VI) is more than 90%, which is 9. 79% and 7. 79% higher than that of the control group. The SEMT analysis indicates that crystalline minerals in the form of thin sheet or needle column are formed on the electrode by the reduction of U( VI) by P25 photoelectron. The EDS analysis shows that it is a uranium containing mineral and the XRD analysis indicates that the reduction products are (UO2)8O2(OH)12·12H2O and UO2 The FTIR analysis shows that after the action, the absorption peak at 472.4cm^-1 is the characteristic vibration peak of U4^+-O bond. The absorption peak at 913.9cm^-1 is U =Oinfrared stretching vibration peak in UO2^2+. The photoelectron reduction uranium products mainly exist as U(IV) and U (VI) minerals. The XPS analysis also demonstrates that the photoelectron reduction uranium products exist as U(IV) and U(VI) minerals.

关 键 词：U(VI) 光电化学还原 RF AQS 

分 类 号：X753[环境科学与工程—环境工程]