超声辐射下糖蜜酒精废水的均相催化降解的研究
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摘要
糖蜜酒精废水是一种难降解的废水,是广西糖业综合利用中的难题。本研究系统地分析了糖蜜酒精废水的来源和特性,研究了单频声化学、US/H_2O_2(声化学即超声波与双氧水氧化)和US/H_2O_2和过渡金属离子系统催化氧化等处理糖蜜酒精废水的技术,深化了认识,揭示了一些特征和本质问题。为糖蜜酒精废水的治理提供了新思路和新途径。
在单频超声化学实验中,研究了单频超声波催化氧化降解糖蜜酒精废水的效果和降解机理,详细探讨了影响糖蜜酒精废水降解的各种因素。实验结果表明:单独超声降解糖蜜酒精废水时,溶液pH值对降解速率影响显著,低pH值有利于降解;降低糖蜜酒精废水溶液的初始浓度,提高声强都能提高糖蜜酒精废水的降解速率;超声降解糖蜜酒精废水的机理以·OH自由基氧化为主;不同气体饱和时,降解速率的大小顺序为Ar＞O_2＞空气＞N_2;低温有利于超声降解反应,但从综合考虑出发,本研究反应温度控制在50℃。
还研究了US/H_2O_2系统催化氧化降解糖蜜酒精废水的效果和降解机理,详细探讨了影响US/H_2O_2氧化工艺降解糖蜜酒精废水的因素。实验结果表明:在200W超声功率下,单独的超声波辐射下反应3.0小时,废水的降解率仅为5.1%;在同等条件下加入过氧化氢氧化(加入量为5.0mL/L),3.0小时后废水的降解率达到55.91%,在此基础上进一步加入过渡金属离子,则降解率进一步提高,其中以Fe~(2+)为64.8%、Cu~(2+)为53.26%、Fe~(3+)为48.31%、Ni~(2+)为53.46%,且反应时间大为缩短,在60min以内基本达到最高降解率。进一步得知US/H_2O_2系统中存在US、H_2O_2和羟基自由基(·OH)三部分协同作用的降解机理。在超声/H_2O_2和亚铁离子体系处理糖蜜酒精废水的降解动力学研究中,发现反应符合表观一级反应,给出动力学方程及有关动力学参数的比较结果。
In this dissertation,the sources and characteristics of molasses fermentation wastewater had been analysed systematicly and degradation of molasses fermentation wastewater under individual ultrasonic(US)radiation or combined US/H_2O_2 system,and US/H_2O_2/transition-metal-ion system had been studied.
The resouts showed that ultrasonic intensty,pH value and initial concentration altered noticeably the reaction rates under individual ultrasonic radiation with preferable operating conditions as low pH,low temperature and using abundance oxygen as saturating gas et al.basing the study on degration effect and mechamism and various influence factors of molasses fermentation wastewater by homogeneous catalysis during the sonochemical experiments.
The influence factors including concentration of H_2O_2,molasses fermentation wastewater and some transition metal ions are investigated during the sonochemical experiments by using US/H_2O_2 system in a bench scale.It was found that degradation rate was merely 5.1%under individual ultrasonic radiation and the addition of H_2O_2 increased the the removal of COD up to 55.91%,that showed that the addition of H_2O_2 was favorable to the removal of COD,however,the excess of H_2O_2 does not significantly affect the removal efficiency.The co-existence of transition metal ions has significant influence upon the reaction rates.The addition of Fe~(2+)increases the reaction rates up to 64.8%,and Cu~(2+)53.26%、Fe~(3+)48.31%、Ni~(2+)53.46%,and the reaction had been shortened visibly.This indicated that there existed synergetic effects in the individual US and Fenton reagent oxidation process.In this paper,the synergetic kinetics of molasses fermentation wastewater treatment by using US/H_2O_2 system was studied.It was found that molasses fermentation wastewater degradation followed pseudo-first order reaction under individual US radiation or individual Fenton reagent oxidation system process,while it significantly enhanced in the combined US/Fenton reagent oxidation system.
在单频超声化学实验中,研究了单频超声波催化氧化降解糖蜜酒精废水的效果和降解机理,详细探讨了影响糖蜜酒精废水降解的各种因素。实验结果表明:单独超声降解糖蜜酒精废水时,溶液pH值对降解速率影响显著,低pH值有利于降解;降低糖蜜酒精废水溶液的初始浓度,提高声强都能提高糖蜜酒精废水的降解速率;超声降解糖蜜酒精废水的机理以·OH自由基氧化为主;不同气体饱和时,降解速率的大小顺序为Ar＞O_2＞空气＞N_2;低温有利于超声降解反应,但从综合考虑出发,本研究反应温度控制在50℃。
还研究了US/H_2O_2系统催化氧化降解糖蜜酒精废水的效果和降解机理,详细探讨了影响US/H_2O_2氧化工艺降解糖蜜酒精废水的因素。实验结果表明:在200W超声功率下,单独的超声波辐射下反应3.0小时,废水的降解率仅为5.1%;在同等条件下加入过氧化氢氧化(加入量为5.0mL/L),3.0小时后废水的降解率达到55.91%,在此基础上进一步加入过渡金属离子,则降解率进一步提高,其中以Fe~(2+)为64.8%、Cu~(2+)为53.26%、Fe~(3+)为48.31%、Ni~(2+)为53.46%,且反应时间大为缩短,在60min以内基本达到最高降解率。进一步得知US/H_2O_2系统中存在US、H_2O_2和羟基自由基(·OH)三部分协同作用的降解机理。在超声/H_2O_2和亚铁离子体系处理糖蜜酒精废水的降解动力学研究中,发现反应符合表观一级反应,给出动力学方程及有关动力学参数的比较结果。
In this dissertation,the sources and characteristics of molasses fermentation wastewater had been analysed systematicly and degradation of molasses fermentation wastewater under individual ultrasonic(US)radiation or combined US/H_2O_2 system,and US/H_2O_2/transition-metal-ion system had been studied.
The resouts showed that ultrasonic intensty,pH value and initial concentration altered noticeably the reaction rates under individual ultrasonic radiation with preferable operating conditions as low pH,low temperature and using abundance oxygen as saturating gas et al.basing the study on degration effect and mechamism and various influence factors of molasses fermentation wastewater by homogeneous catalysis during the sonochemical experiments.
The influence factors including concentration of H_2O_2,molasses fermentation wastewater and some transition metal ions are investigated during the sonochemical experiments by using US/H_2O_2 system in a bench scale.It was found that degradation rate was merely 5.1%under individual ultrasonic radiation and the addition of H_2O_2 increased the the removal of COD up to 55.91%,that showed that the addition of H_2O_2 was favorable to the removal of COD,however,the excess of H_2O_2 does not significantly affect the removal efficiency.The co-existence of transition metal ions has significant influence upon the reaction rates.The addition of Fe~(2+)increases the reaction rates up to 64.8%,and Cu~(2+)53.26%、Fe~(3+)48.31%、Ni~(2+)53.46%,and the reaction had been shortened visibly.This indicated that there existed synergetic effects in the individual US and Fenton reagent oxidation process.In this paper,the synergetic kinetics of molasses fermentation wastewater treatment by using US/H_2O_2 system was studied.It was found that molasses fermentation wastewater degradation followed pseudo-first order reaction under individual US radiation or individual Fenton reagent oxidation system process,while it significantly enhanced in the combined US/Fenton reagent oxidation system.
引文
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