氟喹诺酮与ONOOH化学发光行为多样性的机理研究

项目名称： 氟喹诺酮与ONOOH化学发光行为多样性的机理研究

项目编号： No.21265013

项目类型： 地区科学基金项目

立项/批准年度： 2013

项目学科： 数理科学和化学

项目作者： 程祥磊

作者单位： 南昌大学

项目金额： 50万元

中文摘要： 氟喹诺酮的残留和污染问题已威胁到全球安全，化学发光分析因独特的优点备受青睐，但机理研究的滞后已成为制约其发展的瓶颈。本项目拟以七种氟喹诺酮与过氧亚硝酸ONOOH的化学发光反应为研究对象，在前期研究发现氟喹诺酮的化学发光发射波长与荧光发射波长差异多样性的基础上，采用电子顺磁共振研究化学发光启动步骤中ONOOH衍生自由基的种类和变化，利用停流瞬态吸收光谱技术系统研究七种氟喹诺酮反应过程中所产生的激发态中间体，结合LC-MS和NMR技术解析稳态产物结构，揭示氟喹诺酮化学发光反应中激发态中间体转化历程和ONOOH氧化还原反应类型，阐明氟喹诺酮的化学发光反应机理，突破目前同系物的化学发光机理均为同一模式的思维定势，是对化学发光机理的有力发展，同时也为化学发光反应机理研究提供新的思路。相关研究成果极有望为污水中抗生素的绿色、环境友好型高级氧化处理提供新方案。

中文关键词： 化学发光；多样性；氟喹诺酮类；过氧亚硝酸；脱氟

英文摘要： The residue and pollution of fluoroquinolones (FQs) are now a global safety issue. With significant advantages, chemiluminescence (CL) has attracted the attention of many users and scientists, but the studies on CL mechanisms have lagged behind and hindered the development of the CL techniques. In the present proposal, CL reaction between peroxynitrous acid (ONOOH) and seven selected FQs would be investigated in detail. Based on the phenomena of the diversity of maximum emission wavelength between CL and fluorescence spectra in this CL system, the species and transformation process of ONOOH-deriving free radicals would be measured by using electronic spin resonance spectroscopy (ESR) in the trigger step of CL reaction. On the other hand, different transient, intermediate products in the reaction of seven FQs and ONOOH would be studied intensively. By the aid of LC-MS and NMR, the information about the final stable products of the proposed CL reaction could be resolved. Then, the formation procedure of the involving transient, excited species and the redox type of ONOOH would be uncovered step by step. On the basis of these experimental results, the CL mechanisms between ONOOH and FQs will be clarified. The results of the present proposal would be helpful for the studies on underlying CL mechanisms and break thro

英文关键词： chemiliminescence；diveristy；fluoroquinolones；peroxynitrous acid；defluorination