酸性红37在UV/K2S2O8体系中的降解动力学和转化机制
Degradation kinetic and transformation mechanism of acid red 37 in UV/K2S2O8 system
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摘要:
为了探索单偶氮染料Acid red 37（AR37）降解的可行性及在活性氧物种作用下可能的反应位点和迁移转化机制，采用光活化过硫酸盐技术并根据单因素试验和响应曲面法优化试验考察了底物浓度，K2S2O8用量和温度3个因素对AR37降解率的影响，得出AR37光催化降解的最优条件为：底物浓度90 μmol·L-1，K2S2O8用量8.47 mmol·L-1和温度36℃.最后，利用GCMS对AR37在UV/K2S2O8体系下降解中间产物进行初步的分离与分析，并结合AR37前线电子云密度（FEDs）的理论计算结果对其降解途径进行推导.研究发现AR37在·SO4-等活性氧物种作用下，C2、N8、N16、C17和C18等活性位点容易被自由基直接攻击或者发生电子转移反应，从而引起AR37分子中N=N和C-N键断裂后的进一步羟基化反应，是其主要的降解途径.
Abstract:In order to explore the feasibility of monoazo acid red (AR37) deyradation and its transformation mechanism under the attack of reactive oxygen species, a semi-empirical expression was obtained with the help of photo-activated persulfate technology and central composite design based on response surface methodology. Three variables, i.e. K2S2O8 concentration, reaction temperature and substrate concentration were investigated for performance optimization. The optimal conditions are as follow:substrate concentration=90 μmol·L-1, K2S2O8 concentration=8.47 mmol·L-1 and reaction temperature=36℃. Finally, the degradation intermediates of AR37 were identified by GC/MS. Combined with the Frontier Electron Densities (FEDs) of AR37, the positions of C2, N8, N16, C17 and C18 are likely to be attacked or initiate the single electron transfer reaction under the attack of·SO4-, which resulted in the cleavage of N=N and C-N bonds and further hydroxylation and mineralization of the degradation intermediates under the attack of the reactive oxygen species.
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