木质素磺酸盐氧化降解的研究
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摘要
造纸业每年排放大量的木质素。由于木质素其本身结构特点,在环境中难以被转化和消除,造成了严重的环境污染和资源浪费。如何解决造纸废水的污染问题、开发造纸废水处理新技术、实现可持续发展,是至今尚未完全解决的技术难题,也是世界各国造纸业和环境保护部门的研究重点。
低温等离子体技术是近年来新兴起的一项新型水处理氧化技术,它兼具高能电子辐射、紫外光解、臭氧氧化等方面的共同作用,具有降解速率快、处理范围广、无污染、易操作等优点。本文利用介质阻挡放电低温等离子体,采取空气气动雾化方法,对木质素磺酸盐进行降解；同时还研究木质素的臭氧氧化降解,以期获得一种工业废液的高效绿色处理方法,为解决日益严重的环境问题提供帮助。
臭氧氧化降解实验结果表明,在常温常压下木质素就能被臭氧氧化降解。反应时间、催化剂种类等对反应的影响较大,而超声波、温度等条件的影响很小。在实验条件下,CuSO4或TiO2/α-Al2O3催化剂有利于木质素磺酸钠的臭氧氧化降解反应,而且,臭氧氧化降解反应在木质素降解率为80%左右时达到平衡。
以紫外可见光谱(UV)、红外光谱(FTIR)和1H NMR谱等对木质素磺酸盐降解前后进行了表征结果说明,介质阻挡放电低温等离子体空气气动雾化法可以降解木质素磺酸盐水溶液。木质素磺酸盐降解率的高低受电极间隙、输出电压、催化剂种类、催化剂用量、反应时间等工艺条件的影响。本实验的优化条件为：以硫酸铜为催化剂,电极间隙2 cm、输出电压3000 V、频率10 KHz、反应时间2.3 ms、催化剂用量3.2%条件下,浓度1g/L的木质素磺酸盐,降解率可达50%。
The emissions of a large number of lignin from paper industry results in serious environmental pollution and resource waste. Because of having its own structural characteristics, lignin is very difficult to be transformed and eliminated in the nature environment. How to solve the problem of water pollution, develop new treatment technology for papermaking wastewater, realize society sustainable development are the difficult problems which haven't been fully solved in the international paper industry till now and have become the research priorities of paper industry and environmental protecting departments of countries all over the world.
Non-thermal plasma oxidation is a new advanced oxidation technology developed recently, which has the synergystic degradation function from high energy electron radiation, UV photolysis, pyrolysis to ozone oxidation. It is different from the traditional degradation method, this new oxidation technology with the advantages of speedy degradation rate, wide handling range, no pollution, and easy to operate can effectively remove hardly degradable substances from industry wastewater. In this thesis we used dielectric barrier discharge (DBD) plasma or used ozone to degrade lignin.
The results of ozone oxidation showed that lignin can be degraded under ambient temperature and atmosphere pressure. Among process condition, catalyst or reaction time had remarkable effect on lignin oxidative degradation rate. However, reaction temperature or ultrasonic had little effect on the degradation rate. CUSO4 or TiO2 /α-Al2O3 catalyst was beneficial to the reaction of lignin oxidative degradation. Under test conditions the reaction of lignin oxidative degradation would reach equilibrium when the lignin degradation rate was about 80%.
The reaction of lignin oxidation degradation using DBD plasma carried out by gas-jet expansion method. The degradation of lignosulfonate during this process was characterized by UV, FTIR and 1H NMR spectroscopy. The test results indicated that non-thermal plasma technology was effective to degrade lignosulfonate. The effect of electrode spacing, plasma voltage, catalysts, concentration of catalyst or reaction times on degradation rate was separately studied. Optimum process condition were determined:concentration of lignosulfonate was 1 g/L, electrode spacing was 2 cm, the amount of catalyst CUSO4 was 3.2%, plasma voltage was 3 KV, plasma frequency was 10 KHz, plasma reaction time was 2.3 ms. Under this reaction condition the degradation rate of lignosulfonate can achieved to 50%.
低温等离子体技术是近年来新兴起的一项新型水处理氧化技术,它兼具高能电子辐射、紫外光解、臭氧氧化等方面的共同作用,具有降解速率快、处理范围广、无污染、易操作等优点。本文利用介质阻挡放电低温等离子体,采取空气气动雾化方法,对木质素磺酸盐进行降解；同时还研究木质素的臭氧氧化降解,以期获得一种工业废液的高效绿色处理方法,为解决日益严重的环境问题提供帮助。
臭氧氧化降解实验结果表明,在常温常压下木质素就能被臭氧氧化降解。反应时间、催化剂种类等对反应的影响较大,而超声波、温度等条件的影响很小。在实验条件下,CuSO4或TiO2/α-Al2O3催化剂有利于木质素磺酸钠的臭氧氧化降解反应,而且,臭氧氧化降解反应在木质素降解率为80%左右时达到平衡。
以紫外可见光谱(UV)、红外光谱(FTIR)和1H NMR谱等对木质素磺酸盐降解前后进行了表征结果说明,介质阻挡放电低温等离子体空气气动雾化法可以降解木质素磺酸盐水溶液。木质素磺酸盐降解率的高低受电极间隙、输出电压、催化剂种类、催化剂用量、反应时间等工艺条件的影响。本实验的优化条件为：以硫酸铜为催化剂,电极间隙2 cm、输出电压3000 V、频率10 KHz、反应时间2.3 ms、催化剂用量3.2%条件下,浓度1g/L的木质素磺酸盐,降解率可达50%。
The emissions of a large number of lignin from paper industry results in serious environmental pollution and resource waste. Because of having its own structural characteristics, lignin is very difficult to be transformed and eliminated in the nature environment. How to solve the problem of water pollution, develop new treatment technology for papermaking wastewater, realize society sustainable development are the difficult problems which haven't been fully solved in the international paper industry till now and have become the research priorities of paper industry and environmental protecting departments of countries all over the world.
Non-thermal plasma oxidation is a new advanced oxidation technology developed recently, which has the synergystic degradation function from high energy electron radiation, UV photolysis, pyrolysis to ozone oxidation. It is different from the traditional degradation method, this new oxidation technology with the advantages of speedy degradation rate, wide handling range, no pollution, and easy to operate can effectively remove hardly degradable substances from industry wastewater. In this thesis we used dielectric barrier discharge (DBD) plasma or used ozone to degrade lignin.
The results of ozone oxidation showed that lignin can be degraded under ambient temperature and atmosphere pressure. Among process condition, catalyst or reaction time had remarkable effect on lignin oxidative degradation rate. However, reaction temperature or ultrasonic had little effect on the degradation rate. CUSO4 or TiO2 /α-Al2O3 catalyst was beneficial to the reaction of lignin oxidative degradation. Under test conditions the reaction of lignin oxidative degradation would reach equilibrium when the lignin degradation rate was about 80%.
The reaction of lignin oxidation degradation using DBD plasma carried out by gas-jet expansion method. The degradation of lignosulfonate during this process was characterized by UV, FTIR and 1H NMR spectroscopy. The test results indicated that non-thermal plasma technology was effective to degrade lignosulfonate. The effect of electrode spacing, plasma voltage, catalysts, concentration of catalyst or reaction times on degradation rate was separately studied. Optimum process condition were determined:concentration of lignosulfonate was 1 g/L, electrode spacing was 2 cm, the amount of catalyst CUSO4 was 3.2%, plasma voltage was 3 KV, plasma frequency was 10 KHz, plasma reaction time was 2.3 ms. Under this reaction condition the degradation rate of lignosulfonate can achieved to 50%.
引文
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