摘要
以铝-分子筛(Al-MCM-41)为载体,采用加热回流法制备一种非均相芬顿催化剂还原氧化石墨烯-羟基铁/Al-MCM-41(r GO-Fe OOH/Al-MCM-41).以喹啉模拟有机废水,考察该催化剂在不同氧化体系、不同H_2O_2投加量、不同催化剂投加量和不同水质因素(喹啉初始浓度和p H值)条件下对喹啉降解效能的影响,同时考察了催化剂的重复使用性.结果表明,喹啉的光芬顿降解过程符合准一级反应动力学,降解过程中溶液中的NO-3浓度先升高后下降,表明喹啉的吡啶环被打开.对比芬顿反应,模拟日光芬顿反应中光的引入促进羟基自由基的产生,使得喹啉去除率由45%提高到了99%;喹啉降解速率随着催化剂和H_2O_2投加量的增加而升高,但投加量过多会消耗·OH自由基从而抑制喹啉降解,在光芬顿体系中,该催化剂在p H=3.6—9.6的范围内都表现出了很高的活性;当喹啉初始浓度为20 mg·L^(-1),催化剂投加量为0.5 g·L^(-1),H_2O_2投加量为20 mmol·L^(-1),p H=6.3时,该催化剂对喹啉有很好的矿化效果(TOC去除率为3%).催化剂重复使用性能稳定,重复使用5次喹啉去除率仍高达99%,但TOC去除率略有降低,铁溶出率为0.48%以下.
The heterogeneous Fenton catalyst reduced graphene oxide-goethite supported on Al-MCM-41（r GO-Fe OOH/Al-MCM-41） was prepared by the heating reflux method.The effects of oxidation system,catalyst dosage,H2O2 amount and water quality conditions（initial concentration of quinoline and p H） were investigated for quinoline degradation.The reuse of r GO-Fe OOH/Al-MCM-41 was also evaluated.The results showed that quinoline degradation using heterogeneous photo-Fenton method was well-fitted to a pseudo-first-order kinetic model.The concentration of NO-3in the solution increased firstly and then decreased,which indicated the opening of pyridine ring.In comparison with Fenton reaction,the generation of hydroxyl radicals was promoted by simulated sunlight in the photo-Fenton reaction.The quinolone removal efficiency increased from 45% to 99%.The quinoloneremoval efficiency increased with the catalyst and H2O2 dosage.However,excessive dosage consumed too much ·OH radicals and inhibited quinoline degradation.In photo-Fenton system,the catalyst exhibited higher activity than that in the Fenton reaction system in a wide p H range（3.6—9.6）.Under the optimal condition（20 mg·L-1of initial quinoline concentration,0.5 g·L-1of catalyst dosage,20 mmol·L-1of H2O2 dosage,p H = 6.3）,quinolone and TOC removals were 99%and 3%,respectively.Moreover,the catalyst naintained high activity for quinoline removal（99%）after five times use,but TOC removal decreased slightly.The dissolution rate of Fe was below0.48%.
出处
《环境化学》
CAS
CSCD
北大核心
2017年第5期1072-1082,共11页
Environmental Chemistry
基金
国家自然科学基金(51578070)
国家国际科技合作专项项目(2013DFR90290)
国家地理空气与水保护基金(GEFC-08-16)资助~~
