鐵酸鎳復(fù)合天然礦石的制備及微波催化降解水中有機(jī)污染物
發(fā)布時(shí)間：2018-10-17 10:10
【摘要】：近年來,微波(MW)催化技術(shù)應(yīng)用于治理水環(huán)境污染的研究引起人們關(guān)注。以鐵酸鹽作為催化劑的微波催化氧化技術(shù)更是近年來研究的熱點(diǎn),成為了處理難降解有機(jī)廢水的新型有效方法。然而,在鐵酸鎳微波催化降解技術(shù)中,存在著成本高,“熱點(diǎn)”分散不均勻的問題。為了降低成本和分散鐵酸鎳在微波照射下表面產(chǎn)生的“熱點(diǎn)”,本研究對(duì)Ni Fe_2O_4進(jìn)行改性。以天然礦石為載體,采用Ni Fe_2O_4復(fù)合天然礦石,在微波照射下降解水中有機(jī)污染物。本研究采用微波水熱法制備鐵酸鎳復(fù)合海泡石(Ni Fe_2O_4/sepiolite)、鐵酸鎳復(fù)合硅藻土(Ni Fe_2O_4/diatomite)和鐵酸鎳復(fù)合高嶺土(Ni Fe_2O_4/kaolinite),并應(yīng)用于微波催化降解水中有機(jī)污染物,并對(duì)其催化活性進(jìn)行比較。通過X射線衍射光譜(XRD)、電子掃描電鏡光譜(SEM)和傅里葉轉(zhuǎn)換紅外光譜(FTIR)進(jìn)行表征;考察了微波水熱壓力和時(shí)間,鐵酸鎳和天然礦石的摩爾比、前驅(qū)體p H值、微波照射時(shí)間、使用次數(shù)等因素對(duì)有機(jī)污染物降解效率的影響;比較了Ni Fe_2O_4/natural ore/MW體系中十二烷基苯磺酸鈉(SDBS)、甲基對(duì)硫磷(MP)、結(jié)晶紫(CVL)和偶氮品紅(AF)溶液的降解動(dòng)力學(xué)。結(jié)果表明,在Ni Fe_2O_4/natural ore/MW體系中,有機(jī)污染物可以被有效降解。三種催化劑的微波催化活性由大到小順序?yàn)?Ni Fe_2O_4/sepioliteNi Fe_2O_4/diatomiteNi Fe_2O_4/kaolinite。它們的粒徑從小到大順序?yàn)?Ni Fe_2O_4/海泡石Ni Fe_2O_4/硅藻土Ni Fe_2O_4/高嶺土。當(dāng)Ni Fe_2O_4和天然礦石的摩爾比為9:1,微波水熱壓力為1.5 MPa,微波水熱時(shí)間為30 min時(shí)和前軀體p H值為12.0時(shí),得到的催化劑的活性最高。當(dāng)投加量為3.2g/L和微波降解功率為750 W時(shí),10.0 mg/L甲基對(duì)硫磷(MP)降解5.0 min時(shí),降解率為100%;另外,以偶氮品紅(AF)為目標(biāo)污染物,降解時(shí)間為3 min時(shí),偶氮品紅溶液可以被完全去除。此外,在Ni Fe_2O_4/natural ore/MW體系中SDBS、MP、CVL和AF)水溶液可以被有效的降解。它們的降解速度從快到慢的順序?yàn)?SDBSAFMPCVL。計(jì)算CVL,MP,AF和SDBS在Ni Fe_2O_4/海泡石/MW體系中的降解速率常數(shù)(k)分別為1.864、0.782、0.472和0.329 min-1。當(dāng)Ni Fe_2O_4/海泡石重復(fù)使用三次時(shí),催化劑仍具有一定的催化活性。因此,在有機(jī)廢水處理中,Ni Fe_2O_4/天然礦石結(jié)合微波催化降解技術(shù)表現(xiàn)出巨大的潛力。
[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.
【學(xué)位授予單位】：遼寧大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TQ426;X703
本文編號(hào)：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.
【學(xué)位授予單位】：遼寧大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TQ426;X703
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