铁酸镍复合天然矿石的制备及微波催化降解水中有机污染物
发布时间：2018-10-17 10:10
【摘要】：近年来,微波(MW)催化技术应用于治理水环境污染的研究引起人们关注。以铁酸盐作为催化剂的微波催化氧化技术更是近年来研究的热点,成为了处理难降解有机废水的新型有效方法。然而,在铁酸镍微波催化降解技术中,存在着成本高,“热点”分散不均匀的问题。为了降低成本和分散铁酸镍在微波照射下表面产生的“热点”,本研究对Ni Fe_2O_4进行改性。以天然矿石为载体,采用Ni Fe_2O_4复合天然矿石,在微波照射下降解水中有机污染物。本研究采用微波水热法制备铁酸镍复合海泡石(Ni Fe_2O_4/sepiolite)、铁酸镍复合硅藻土(Ni Fe_2O_4/diatomite)和铁酸镍复合高岭土(Ni Fe_2O_4/kaolinite),并应用于微波催化降解水中有机污染物,并对其催化活性进行比较。通过X射线衍射光谱(XRD)、电子扫描电镜光谱(SEM)和傅里叶转换红外光谱(FTIR)进行表征;考察了微波水热压力和时间,铁酸镍和天然矿石的摩尔比、前驱体p H值、微波照射时间、使用次数等因素对有机污染物降解效率的影响;比较了Ni Fe_2O_4/natural ore/MW体系中十二烷基苯磺酸钠(SDBS)、甲基对硫磷(MP)、结晶紫(CVL)和偶氮品红(AF)溶液的降解动力学。结果表明,在Ni Fe_2O_4/natural ore/MW体系中,有机污染物可以被有效降解。三种催化剂的微波催化活性由大到小顺序为:Ni Fe_2O_4/sepioliteNi Fe_2O_4/diatomiteNi Fe_2O_4/kaolinite。它们的粒径从小到大顺序为:Ni Fe_2O_4/海泡石Ni Fe_2O_4/硅藻土Ni Fe_2O_4/高岭土。当Ni Fe_2O_4和天然矿石的摩尔比为9:1,微波水热压力为1.5 MPa,微波水热时间为30 min时和前躯体p H值为12.0时,得到的催化剂的活性最高。当投加量为3.2g/L和微波降解功率为750 W时,10.0 mg/L甲基对硫磷(MP)降解5.0 min时,降解率为100%;另外,以偶氮品红(AF)为目标污染物,降解时间为3 min时,偶氮品红溶液可以被完全去除。此外,在Ni Fe_2O_4/natural ore/MW体系中SDBS、MP、CVL和AF)水溶液可以被有效的降解。它们的降解速度从快到慢的顺序为:SDBSAFMPCVL。计算CVL,MP,AF和SDBS在Ni Fe_2O_4/海泡石/MW体系中的降解速率常数(k)分别为1.864、0.782、0.472和0.329 min-1。当Ni Fe_2O_4/海泡石重复使用三次时,催化剂仍具有一定的催化活性。因此,在有机废水处理中,Ni Fe_2O_4/天然矿石结合微波催化降解技术表现出巨大的潜力。
[Abstract]:In recent years, the application of microwave (MW) catalytic technology in the treatment of water pollution has attracted people's attention. Microwave catalytic oxidation with ferrate as catalyst has been a hot topic in recent years and has become a new effective method for the treatment of refractory organic wastewater. However, in the microwave catalytic degradation of nickel ferrate, there are many problems such as high cost and uneven dispersion of hot spots. In order to reduce the cost and the "hot spot" produced by dispersed nickel ferrate under microwave irradiation, Ni Fe_2O_4 was modified in this paper. Using natural ore as carrier, Ni Fe_2O_4 compound natural ore was used to degrade organic pollutants in water under microwave irradiation. In this study, nickel ferrate composite sepiolite (Ni Fe_2O_4/sepiolite), nickel ferrate composite diatomite (Ni Fe_2O_4/diatomite) and nickel ferrate composite kaolin (Ni Fe_2O_4/kaolinite) were prepared by microwave hydrothermal method. X-ray diffraction spectroscopy (XRD), electron scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) were used to characterize the results. The microwave hydrothermal pressure and time, molar ratio of nickel ferrate to natural ore, precursor pH value, microwave irradiation time were investigated. The degradation kinetics of sodium dodecylbenzene sulfonate (SDBS), methyl parathion (MP), crystal violet (CVL) and azo fuchsin (AF) solution in Ni Fe_2O_4/natural ore/MW system was compared. The results showed that organic pollutants could be effectively degraded in Ni Fe_2O_4/natural ore/MW system. The order of microwave catalytic activity of the three catalysts is as follows: Ni Fe_2O_4/sepioliteNi Fe_2O_4/diatomiteNi Fe_2O_4/kaolinite. The order of their particle size is: Ni Fe_2O_4/ sepiolite, Ni Fe_2O_4/ diatomite, Ni Fe_2O_4/ kaolin. When the molar ratio of Ni Fe_2O_4 to natural ore is 9: 1, the microwave hydrothermal pressure is 1.5 MPa, the microwave hydrothermal time is 30 min and the pH value of the precursor is 12.0, the catalyst has the highest activity. When the dosage of 3.2g/L was 750W and the microwave power was 750W, the degradation rate of 10.0 mg/L methylparathion (MP) was 100 min, and the azo fuchsin solution could be completely removed when the azo fuchsin (AF) was used as the target pollutant and the degradation time was 3 min. In addition, SDBS,MP,CVL and AF aqueous solution can be effectively degraded in Ni Fe_2O_4/natural ore/MW system. The order in which they degrade from fast to slow is: SDBSAFMPCVL. The degradation rate constants (k) of CVL,MP,AF and SDBS in Ni Fe_2O_4/ sepiolite / MW system were calculated to be 1.864% 0.782C 0.472 and 0.329 min-1., respectively. When Ni Fe_2O_4/ sepiolite was reused for three times, the catalyst still had certain catalytic activity. Therefore, in organic wastewater treatment, Ni Fe_2O_4/ natural ore combined with microwave catalytic degradation technology shows great potential.
【学位授予单位】：辽宁大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ426;X703
本文编号：2276321
[Abstract]:In recent years, the application of microwave (MW) catalytic technology in the treatment of water pollution has attracted people's attention. Microwave catalytic oxidation with ferrate as catalyst has been a hot topic in recent years and has become a new effective method for the treatment of refractory organic wastewater. However, in the microwave catalytic degradation of nickel ferrate, there are many problems such as high cost and uneven dispersion of hot spots. In order to reduce the cost and the "hot spot" produced by dispersed nickel ferrate under microwave irradiation, Ni Fe_2O_4 was modified in this paper. Using natural ore as carrier, Ni Fe_2O_4 compound natural ore was used to degrade organic pollutants in water under microwave irradiation. In this study, nickel ferrate composite sepiolite (Ni Fe_2O_4/sepiolite), nickel ferrate composite diatomite (Ni Fe_2O_4/diatomite) and nickel ferrate composite kaolin (Ni Fe_2O_4/kaolinite) were prepared by microwave hydrothermal method. X-ray diffraction spectroscopy (XRD), electron scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR) were used to characterize the results. The microwave hydrothermal pressure and time, molar ratio of nickel ferrate to natural ore, precursor pH value, microwave irradiation time were investigated. The degradation kinetics of sodium dodecylbenzene sulfonate (SDBS), methyl parathion (MP), crystal violet (CVL) and azo fuchsin (AF) solution in Ni Fe_2O_4/natural ore/MW system was compared. The results showed that organic pollutants could be effectively degraded in Ni Fe_2O_4/natural ore/MW system. The order of microwave catalytic activity of the three catalysts is as follows: Ni Fe_2O_4/sepioliteNi Fe_2O_4/diatomiteNi Fe_2O_4/kaolinite. The order of their particle size is: Ni Fe_2O_4/ sepiolite, Ni Fe_2O_4/ diatomite, Ni Fe_2O_4/ kaolin. When the molar ratio of Ni Fe_2O_4 to natural ore is 9: 1, the microwave hydrothermal pressure is 1.5 MPa, the microwave hydrothermal time is 30 min and the pH value of the precursor is 12.0, the catalyst has the highest activity. When the dosage of 3.2g/L was 750W and the microwave power was 750W, the degradation rate of 10.0 mg/L methylparathion (MP) was 100 min, and the azo fuchsin solution could be completely removed when the azo fuchsin (AF) was used as the target pollutant and the degradation time was 3 min. In addition, SDBS,MP,CVL and AF aqueous solution can be effectively degraded in Ni Fe_2O_4/natural ore/MW system. The order in which they degrade from fast to slow is: SDBSAFMPCVL. The degradation rate constants (k) of CVL,MP,AF and SDBS in Ni Fe_2O_4/ sepiolite / MW system were calculated to be 1.864% 0.782C 0.472 and 0.329 min-1., respectively. When Ni Fe_2O_4/ sepiolite was reused for three times, the catalyst still had certain catalytic activity. Therefore, in organic wastewater treatment, Ni Fe_2O_4/ natural ore combined with microwave catalytic degradation technology shows great potential.
【学位授予单位】：辽宁大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TQ426;X703
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