生物質(zhì)炭對三種不同極性有機污染物的吸附機理研究
發(fā)布時間：2018-09-17 14:36
【摘要】：本項目選擇不同來源的高有機碳固體廢棄物,采用程序升溫法來制備多種生物質(zhì)炭,利用電鏡掃描、元素分析、比表面積分析、光譜分析等手段揭示了不同生物質(zhì)炭的結構特性,并通過酸洗、溫度梯度等措施優(yōu)化生物質(zhì)炭的表面特性;然后將生物質(zhì)炭與不同類型的有機污染物進行批量吸附實驗,并對吸附前后的生物質(zhì)炭與污染物的復合物進行紅外光譜分析,剖析了生物質(zhì)炭對不同有機污染物的表面吸附過程,揭示了生物質(zhì)炭對不同類型有機污染物的吸附機制。結果表明:(1)生物質(zhì)炭的特性明顯受原材料來源和裂解溫度的影響。秸稈生物質(zhì)炭含C量最高,楊樹葉生物質(zhì)炭含H和N量最高,污泥生物質(zhì)炭的灰分含量最高。隨著溫度的升高,生物質(zhì)炭的芳香性增強,比表面積和吸附容量增加,酸洗處理顯著改變生物質(zhì)炭表面官能團振動峰,并能夠增加其表面孔容及中孔數(shù)量,提高了生物質(zhì)炭的吸附性能。(2)2,4-D、阿特拉津和萘這三種有機污染物在生物質(zhì)炭上的吸附過程都是一個先快后慢的過程,生物質(zhì)炭對萘的吸附一般在15 h后達到吸附平衡,而對2,4-D和阿特拉津的吸附需要24 h以上才能達到平衡狀態(tài)。批量吸附實驗表明不同生物質(zhì)炭對2,4-D、阿特拉津和萘的吸附等溫曲線均符合Frendlich模型;對萘的吸附同時也符合Langmuir模型。生物質(zhì)炭對三種有機污染物的吸附能力不同,秸稈生物質(zhì)炭對萘的吸附能力最強,對2,4-D和阿特拉津的吸附能力較弱。(3)生物質(zhì)炭的裂解溫度和顆粒細度會影響其對有機物的吸附特性。隨著生物質(zhì)炭裂解溫度的增加,秸稈炭和楊樹葉炭對三種有機物的吸附能力增加;隨著炭顆粒粒徑的減小,生物質(zhì)炭對有機污染物的平衡吸附量增加。(4)溶液環(huán)境會顯著影響生物質(zhì)炭吸附有機物分子的吸附特性及平衡吸附量。秸稈生物質(zhì)炭對2,4-D和阿特拉津在離子強度為0.01 mol/L吸附量最強,而楊樹葉生物質(zhì)炭對2,4-D和阿特拉津的吸附能力隨溶液中電解質(zhì)強度的增加而增加。溶液環(huán)境為酸性時,生物質(zhì)炭對2,4-D的吸附量最大,溶液環(huán)境為堿性時,炭對阿特拉津的吸附量最大;改變?nèi)芤旱膒H值不會影響秸稈炭對萘的吸附能力。(5)生物質(zhì)炭對3種有機污染物的吸附機制不同。萘在水溶液中為非極性分子,秸稈生物質(zhì)炭對其的吸附機制主要包括范德華力、疏水作用和π-πEDA相互作用。2,4-D分子在水溶液中表現(xiàn)為負極性,秸稈生物質(zhì)炭對2,4-D的吸附過程還會受到范德華力、π-πEDA作用、靜電作用以及氫鍵作用的影響;楊樹葉生物質(zhì)炭對2,4-D的吸附機制除了靜電作用外,還包括范德華力、π-πEDA作用和疏水作用。阿特拉津在水溶液為正極性,秸稈生物質(zhì)炭對阿特拉津的吸附機制包括疏水作用和靜電作用,楊樹葉生物質(zhì)炭對阿特拉津的吸附機制包括范德華力、靜電作用和疏水作用。
[Abstract]:In this project, high organic carbon solid waste from different sources was selected, and a variety of biomass carbon was prepared by temperature programmed method. Scanning electron microscopy, elemental analysis and specific surface area analysis were used. The structural characteristics of different biomass carbon were revealed by spectroscopic analysis, and the surface characteristics of biomass carbon were optimized by acid pickling and temperature gradient, and then the batch adsorption experiments were carried out between biomass carbon and different organic pollutants. The complex of biomass carbon and pollutants before and after adsorption was analyzed by infrared spectroscopy. The surface adsorption process of biomass carbon to different organic pollutants was analyzed, and the adsorption mechanism of biomass carbon to different organic pollutants was revealed. The results showed that: (1) the characteristics of biomass carbon were obviously affected by the source of raw materials and pyrolysis temperature. Straw biomass carbon had the highest content of C, poplar leaf biomass carbon had the highest H and N content, and sludge biomass carbon had the highest ash content. With the increase of temperature, the aromaticity, specific surface area and adsorption capacity of biomass carbon increased. The surface functional group vibration peak of biomass carbon was significantly changed by pickling treatment, and the surface pore volume and the number of mesoporous carbon were increased. The adsorption performance of biomass carbon was improved. (2) the adsorption process of three organic pollutants, atrazine and naphthalene, on biomass carbon was a fast process and then a slow process, and the adsorption equilibrium of naphthalene adsorbed by biomass carbon was generally reached after 15 h. However, it takes more than 24 hours to reach the equilibrium state for the adsorption of 2,4-D and atrazine. Batch adsorption experiments showed that the adsorption isotherm curves of 2h4 D, atrazine and naphthalene for different biomass carbon were in accordance with the Frendlich model, and the adsorption of naphthalene for naphthalene was also consistent with Langmuir model. The adsorption ability of biomass carbon to naphthalene was the highest, and the adsorption ability of biomass carbon to naphthalene was different. (3) the pyrolysis temperature and particle fineness of biomass carbon will affect the adsorption characteristics of organic matter. With the increase of pyrolysis temperature of biomass carbon, the adsorption ability of straw charcoal and poplar leaf charcoal to three organic compounds increased, and the diameter of carbon particles decreased with the increase of biomass carbon pyrolysis temperature. (4) the adsorption characteristics and equilibrium adsorption capacity of organic molecules adsorbed by biomass carbon were significantly affected by the solution environment. The adsorption capacity of straw biomass carbon for 2na-4-D and atrazine was the strongest at ionic strength of 0. 01 mol/L, but the adsorption capacity of poplar leaf biomass charcoal for 2n4-D and atrazine increased with the increase of electrolyte strength in the solution. When the solution environment is acidic, the adsorption capacity of biochar to 2n4-D is the largest, and when the solution environment is alkaline, the adsorption capacity of carbon to atrazine is the largest. The adsorption ability of naphthalene by straw carbon was not affected by changing the pH value of the solution. (5) the adsorption mechanism of three organic pollutants by biomass carbon was different. Naphthalene is a nonpolar molecule in aqueous solution. The adsorption mechanism of naphthalene on straw biomass carbon mainly includes van der Waals force, hydrophobic interaction and 蟺-蟺 EDA interaction. The adsorption process of 2H 4-D by straw biomass carbon was also affected by van der Waals force, 蟺-蟺 EDA, electrostatic action and hydrogen bond interaction, and the adsorption mechanism of poplar leaf biomass charcoal to 2H4 D included van der Waals force, 蟺-蟺 EDA interaction and hydrophobicity. Atrazine has a positive polarity in aqueous solution. The adsorption mechanism of atrazine on straw biomass carbon includes hydrophobic and electrostatic interaction, while the adsorption mechanism of atrazine from poplar leaves includes van der Waals force, electrostatic action and hydrophobic effect.
【學位授予單位】：中國農(nóng)業(yè)大學
【學位級別】：博士
【學位授予年份】：2017
【分類號】：X505
本文編號：2246229
[Abstract]:In this project, high organic carbon solid waste from different sources was selected, and a variety of biomass carbon was prepared by temperature programmed method. Scanning electron microscopy, elemental analysis and specific surface area analysis were used. The structural characteristics of different biomass carbon were revealed by spectroscopic analysis, and the surface characteristics of biomass carbon were optimized by acid pickling and temperature gradient, and then the batch adsorption experiments were carried out between biomass carbon and different organic pollutants. The complex of biomass carbon and pollutants before and after adsorption was analyzed by infrared spectroscopy. The surface adsorption process of biomass carbon to different organic pollutants was analyzed, and the adsorption mechanism of biomass carbon to different organic pollutants was revealed. The results showed that: (1) the characteristics of biomass carbon were obviously affected by the source of raw materials and pyrolysis temperature. Straw biomass carbon had the highest content of C, poplar leaf biomass carbon had the highest H and N content, and sludge biomass carbon had the highest ash content. With the increase of temperature, the aromaticity, specific surface area and adsorption capacity of biomass carbon increased. The surface functional group vibration peak of biomass carbon was significantly changed by pickling treatment, and the surface pore volume and the number of mesoporous carbon were increased. The adsorption performance of biomass carbon was improved. (2) the adsorption process of three organic pollutants, atrazine and naphthalene, on biomass carbon was a fast process and then a slow process, and the adsorption equilibrium of naphthalene adsorbed by biomass carbon was generally reached after 15 h. However, it takes more than 24 hours to reach the equilibrium state for the adsorption of 2,4-D and atrazine. Batch adsorption experiments showed that the adsorption isotherm curves of 2h4 D, atrazine and naphthalene for different biomass carbon were in accordance with the Frendlich model, and the adsorption of naphthalene for naphthalene was also consistent with Langmuir model. The adsorption ability of biomass carbon to naphthalene was the highest, and the adsorption ability of biomass carbon to naphthalene was different. (3) the pyrolysis temperature and particle fineness of biomass carbon will affect the adsorption characteristics of organic matter. With the increase of pyrolysis temperature of biomass carbon, the adsorption ability of straw charcoal and poplar leaf charcoal to three organic compounds increased, and the diameter of carbon particles decreased with the increase of biomass carbon pyrolysis temperature. (4) the adsorption characteristics and equilibrium adsorption capacity of organic molecules adsorbed by biomass carbon were significantly affected by the solution environment. The adsorption capacity of straw biomass carbon for 2na-4-D and atrazine was the strongest at ionic strength of 0. 01 mol/L, but the adsorption capacity of poplar leaf biomass charcoal for 2n4-D and atrazine increased with the increase of electrolyte strength in the solution. When the solution environment is acidic, the adsorption capacity of biochar to 2n4-D is the largest, and when the solution environment is alkaline, the adsorption capacity of carbon to atrazine is the largest. The adsorption ability of naphthalene by straw carbon was not affected by changing the pH value of the solution. (5) the adsorption mechanism of three organic pollutants by biomass carbon was different. Naphthalene is a nonpolar molecule in aqueous solution. The adsorption mechanism of naphthalene on straw biomass carbon mainly includes van der Waals force, hydrophobic interaction and 蟺-蟺 EDA interaction. The adsorption process of 2H 4-D by straw biomass carbon was also affected by van der Waals force, 蟺-蟺 EDA, electrostatic action and hydrogen bond interaction, and the adsorption mechanism of poplar leaf biomass charcoal to 2H4 D included van der Waals force, 蟺-蟺 EDA interaction and hydrophobicity. Atrazine has a positive polarity in aqueous solution. The adsorption mechanism of atrazine on straw biomass carbon includes hydrophobic and electrostatic interaction, while the adsorption mechanism of atrazine from poplar leaves includes van der Waals force, electrostatic action and hydrophobic effect.
【學位授予單位】：中國農(nóng)業(yè)大學
【學位級別】：博士
【學位授予年份】：2017
【分類號】：X505
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