中文摘要
芳香族污染物是制浆造纸废水中主要难降解污染物,近年发展起来的PS高级氧化技术避免了Fenton技术存在的只能在pH值3.0-5.0酸性条件下发挥氧化作用、芳香族污染物无法被有效降解等问题,新型金属有机骨架材料MOFs可控的金属活性中心及易功能化组装特性为氧化自由基SO4-•的控制和芳香族污染物的靶向选择提供了可能。但MOFs催化活性位点控制自由基的产生及靶向组装MOFs对芳香族污染物分子识别的机制尚不清楚。本项目拟研究MOFs配位不饱和度和晶型结构的差异对PS体系中SO4-•产生的影响规律、功能化MOFs分子识别位点分布与包覆层孔穴结构的差异对芳香族污染物靶向识别的影响机制,探讨污染物降解链式反应历程,得到功能化MOFs催化活化PS体系靶向降解芳香族污染物的反应机理。研究将为采用功能化MOFs调控PS氧化体系中SO4-•的释放、实现制浆造纸废水中芳香族污染物的有效深度降解提供理论指导。
英文摘要
Aromatic pollutants are the main pollutant in pulping and papermaking wastewater, persulfate (PS) Advanced Oxidation Processes (AOPs) developed in recent years has avoided a lot of problems existed in Fenton processes, thus as only can play the oxidation role in a pH range from 3.0 to 5.0 under acid conditions, cannot effectively degrade the aromatic pollutants, etc. A novel catalyst, Metal Organic Frameworks (MOFs) has provided the opportunity of controlling the free radicals and targeted selecting of the contaminants by MOFs activated persulfate because of its’ controllable metal active sites and easy functional assembling property. But the mechanism of controlling the generation of the free radical by regulating the catalytic active site of MOFs and realizing the molecular recognition of aromatic pollutant through targeted assembly is still not clear. This project intends to research the influencing rule on free radical generation of MOFs with different coordination unsaturability and crystal structure, and research the influencing mechanism on contaminant selectivity of functional MOFs with different distribution of molecular recognition sites and hole structure inside the coating layer, as well as explore the chain reaction mechanism of the targeted degradation of aromatic contaminant by MOFs activated persulfate. The research results can provide the theoretical guidance for controlling the generation and release of sulfate radical in functional MOFs activated persulfate systems and realizing the effective advanced degradation of aromatic pollutants in papermaking wastewater.
