日光、超声波、微波促进Fenton体系氧化降解直接桃红12B的研究
摘要
在染料工业的发展中,直接染料已经有一百多年的商业生产历史,是一类很重要的染料类别。而其生产废水也是当前的水体重要的污染源之一。由于这类废水成分复杂,往往含有多种有机染料及其中间体,其特点为色度深、毒性强、难降解、pH波动大、组分变化大,且浓度高,水量大,一直是工业废水处理的难点。染料废水的处理因而成为当今环境领域的一大研究热点。
Fenton氧化法是一种典型的高级氧化技术。它能产生氧化能力极强的羟基自由基?OH,羟基自由基能够有效的降解有机物,甚至彻底地将有机物转化为无害的无机物。论文将可见光、超声波、微波引入Fenton反应体系促进氧化降解偶氮类染料——直接桃红12B,研究内容包括:通过单因素试验,研究Photo/Fenton、US/Fenton、微波辐射Fenton法氧化降解偶氮类染料直接桃红12B反应中重要影响因素(pH值,Fe~(2+)用量,H_2O_2用量、超声功率或微波功率)对色度去除率的影响;在单因素试验的基础上利用正交实验设计得到最优化实验条件;Photo/Fenton、US/Fenton、微波辐射Fenton协同效应研究;通过控制性试验得到Photo/Fenton、US/Fenton、微波辐射Fenton氧化反应降解目标有机物的动力学方程。
实验结果表明:
Photo/Fenton处理直接桃红12B溶液具有协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.5,Fe~(2+)投加量为220uL,H_2O_2投加量为50uL。在优化条件下,光照30min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到77.8%。在初始pH=3.5条件下,Photo/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=1.4×10~(-2)×P~(0.39)×F~(1.7)×E~(0.33)
US/Fenton处理直接桃红12B溶液具有协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.0,Fe~(2+)投加量为160uL,H_2O_2投加量为40uL,超声功率为100W。在优化条件下,超声处理30min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到79.5%。在初始pH=3.0条件下,US/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=7.5×10~(-7)×P~(0.78)×F~(2.05)×E~(0.91)×H~(0.93)
微波辐射Fenton处理直接桃红12B溶液具有很好的协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,同时还能降低芬顿试剂的用量。对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.5,Fe~(2+)投加量为15uL,H_2O_2投加量为15uL,微波功率为320W。在优化条件下,微波处理10min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到85.8%。在初始pH=3.0条件下,US/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=5.4×10~(-11)×P~(3.26)×F~(1.66)×E~(1.28)×H~(1.71)
Direct dyes have been produced commercially for over 100 years.As an important and widely used type of dyes,its wastewater are also complicated, which involves various organic dyes and their intermediates. What’s more, the wastewater usually has those characters: deep color, high concentrations, long resistance to biodegradation, strong toxicity, wide fluctuation of pH, great variation of ingredients, large waste streams and so on. Therefore, dye wastewater treatment has increasingly become one of the heated topics in the field of environmental engineering.
Fenton hydrocarbonylation, being a senior oxidation technique, brings about hydroxyl free radical(?OH) which is efficacious to degrade organic compounds, even to completely transforming organic compounds into harmless inorganic substances. In this paper, sunlight,ultrosonic and microwave are introduced into Fenton reaction system, aiming to improving degradation of polycyclic aromatic hydrocarbon dyes—Dirct pink 12B. The following contents are included: deriving the optimum experimental condition from orthogonal experimental design based on single-factor experiment; investigations on photo-Fenton,ultrosonic-Fenton,microwave-Fenton synergistic effects; via controlling experiment, kinetic equation for photo-Fenton, ultrosonic-Fenton, microwave-Fenton oxidizing reaction to degrade target organics is obtained.
By experiments, it is suggested that the couple of sunlight-Fenton prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.5, 50uL 30%H_2O_2, 220uL 18mmol L-1Fe~(2+)and 30min sunlight interactions. Then, 100% of Direct pink is removed and 77.8% for COD. On original condition that pH=3.5, kinetic equation for Fenton reaction in case of sunlight radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=1.4×10~(-2)×P~(0.39)×F~(1.7)×E~(0.33)
Combination of ultrosonic and Fenton agents prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.0, 40uL 30%H_2O_2, 160uL 18mmol L-1Fe~(2+), ultrosonic power 100W and 30min ultrosonic interactions. Then, 100% of Direct pink is removed and 79.5% for COD. On original condition that pH=3.0, kinetic equation for Fenton reaction in case of ultrosonic radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=7.5×10~(-7)×P~(0.78)×F~(2.05)×E~(0.91)×H~(0.93)
Couple of microwave-Fenton prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.5, 15uL 30%H_2O_2, 15uL 18mmol L-1 Fe~(2+), Microwave power 320W and 10min Microwave irradiation interactions. Then, 100% of Direct pink is removed and 79.5% for COD. On original condition that pH=3.0, kinetic equation for Fenton reaction in case of ultrosonic radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=5.4×10~(-11)×P~(3.26)×F~(1.66)×E~(1.28)×H~(1.71)
Fenton氧化法是一种典型的高级氧化技术。它能产生氧化能力极强的羟基自由基?OH,羟基自由基能够有效的降解有机物,甚至彻底地将有机物转化为无害的无机物。论文将可见光、超声波、微波引入Fenton反应体系促进氧化降解偶氮类染料——直接桃红12B,研究内容包括:通过单因素试验,研究Photo/Fenton、US/Fenton、微波辐射Fenton法氧化降解偶氮类染料直接桃红12B反应中重要影响因素(pH值,Fe~(2+)用量,H_2O_2用量、超声功率或微波功率)对色度去除率的影响;在单因素试验的基础上利用正交实验设计得到最优化实验条件;Photo/Fenton、US/Fenton、微波辐射Fenton协同效应研究;通过控制性试验得到Photo/Fenton、US/Fenton、微波辐射Fenton氧化反应降解目标有机物的动力学方程。
实验结果表明:
Photo/Fenton处理直接桃红12B溶液具有协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.5,Fe~(2+)投加量为220uL,H_2O_2投加量为50uL。在优化条件下,光照30min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到77.8%。在初始pH=3.5条件下,Photo/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=1.4×10~(-2)×P~(0.39)×F~(1.7)×E~(0.33)
US/Fenton处理直接桃红12B溶液具有协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.0,Fe~(2+)投加量为160uL,H_2O_2投加量为40uL,超声功率为100W。在优化条件下,超声处理30min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到79.5%。在初始pH=3.0条件下,US/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=7.5×10~(-7)×P~(0.78)×F~(2.05)×E~(0.91)×H~(0.93)
微波辐射Fenton处理直接桃红12B溶液具有很好的协同效应,能有效地提高直接桃红12B的色度去除率和COD去除率,同时还能降低芬顿试剂的用量。对于处理100mL,500mg/L直接桃红12B溶液的优化试验条件是:pH值为3.5,Fe~(2+)投加量为15uL,H_2O_2投加量为15uL,微波功率为320W。在优化条件下,微波处理10min,直接桃红12B溶液的色度去除率达到100%,COD去除率达到85.8%。在初始pH=3.0条件下,US/Fenton反应氧化处理直接桃红12B的动力学方程为: V=-((dP)/(dt))=5.4×10~(-11)×P~(3.26)×F~(1.66)×E~(1.28)×H~(1.71)
Direct dyes have been produced commercially for over 100 years.As an important and widely used type of dyes,its wastewater are also complicated, which involves various organic dyes and their intermediates. What’s more, the wastewater usually has those characters: deep color, high concentrations, long resistance to biodegradation, strong toxicity, wide fluctuation of pH, great variation of ingredients, large waste streams and so on. Therefore, dye wastewater treatment has increasingly become one of the heated topics in the field of environmental engineering.
Fenton hydrocarbonylation, being a senior oxidation technique, brings about hydroxyl free radical(?OH) which is efficacious to degrade organic compounds, even to completely transforming organic compounds into harmless inorganic substances. In this paper, sunlight,ultrosonic and microwave are introduced into Fenton reaction system, aiming to improving degradation of polycyclic aromatic hydrocarbon dyes—Dirct pink 12B. The following contents are included: deriving the optimum experimental condition from orthogonal experimental design based on single-factor experiment; investigations on photo-Fenton,ultrosonic-Fenton,microwave-Fenton synergistic effects; via controlling experiment, kinetic equation for photo-Fenton, ultrosonic-Fenton, microwave-Fenton oxidizing reaction to degrade target organics is obtained.
By experiments, it is suggested that the couple of sunlight-Fenton prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.5, 50uL 30%H_2O_2, 220uL 18mmol L-1Fe~(2+)and 30min sunlight interactions. Then, 100% of Direct pink is removed and 77.8% for COD. On original condition that pH=3.5, kinetic equation for Fenton reaction in case of sunlight radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=1.4×10~(-2)×P~(0.39)×F~(1.7)×E~(0.33)
Combination of ultrosonic and Fenton agents prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.0, 40uL 30%H_2O_2, 160uL 18mmol L-1Fe~(2+), ultrosonic power 100W and 30min ultrosonic interactions. Then, 100% of Direct pink is removed and 79.5% for COD. On original condition that pH=3.0, kinetic equation for Fenton reaction in case of ultrosonic radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=7.5×10~(-7)×P~(0.78)×F~(2.05)×E~(0.91)×H~(0.93)
Couple of microwave-Fenton prossess of synergistic effects which enable enhance color and COD removal rate of Direct pink 12B.For the direct pink 12B solution with the volume of 100mL and the concentration of 500mg/L, the optimum experimental condition is resulted: pH=3.5, 15uL 30%H_2O_2, 15uL 18mmol L-1 Fe~(2+), Microwave power 320W and 10min Microwave irradiation interactions. Then, 100% of Direct pink is removed and 79.5% for COD. On original condition that pH=3.0, kinetic equation for Fenton reaction in case of ultrosonic radiation to degrade Direct pink 12B is as: V=-((dP)/(dt))=5.4×10~(-11)×P~(3.26)×F~(1.66)×E~(1.28)×H~(1.71)
引文
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