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鐵基納米粒子@沙棘枝炭復(fù)合材料的制備及其廢水處理性能研究

發(fā)布時間:2018-06-27 12:54

  本文選題:沙棘枝炭 + 復(fù)合材料; 參考:《長安大學(xué)》2017年碩士論文


【摘要】:活性炭吸附法,是一種廣泛用于去除水中污染物的廢水處理方法,但是成本較高的商用活性炭,增加了廢水處理的運(yùn)行成本;诖,利用農(nóng)業(yè)廢棄生物質(zhì)制備活性炭近年來得到了廣泛關(guān)注。沙棘是一種落葉灌木,廣泛分布在高海拔地區(qū)。然而,在沙棘果采摘過程中產(chǎn)生的沙棘枝條,因?yàn)殡S意丟棄和就地焚燒,已經(jīng)引起了一系列的環(huán)境污染問題。沙棘枝條作為一個典型的富碳、廉價、資源量豐富的農(nóng)業(yè)固體廢物,是一種可持續(xù)生產(chǎn)的、天然來源的生物碳,適用于制備活性炭。但是單一的沙棘枝炭吸附無法達(dá)到低成本、高效率和無二次污染等目的。因此,在沙棘枝炭的表面引入鐵基納米粒子,增加比表面積提高吸附性能的同時,構(gòu)建起非均相Fenton體系,實(shí)現(xiàn)吸附劑的循環(huán)再生,防止二次污染進(jìn)一步降低成本,得到新型的復(fù)合吸附材料。將所制備的復(fù)合吸附材料應(yīng)用于抗生素廢水和染料廢水處理領(lǐng)域,并考察了該復(fù)合材料的吸附和再生性能。具體研究內(nèi)容如下:(1)以廢棄沙棘枝條為基體,浸漬鐵離子后,通過熱裂解法制備了Fe_3O_4@沙棘枝炭復(fù)合吸附劑。SEM和EDS結(jié)果表明納米Fe_3O_4顆粒粒徑約為40 nm,在炭表面呈部分覆蓋,單分散態(tài)。XRD表明生成的納米Fe_3O_4為面心立方晶型,碳為無晶型。以強(qiáng)力霉素廢水為處理對象,探討了pH、吸附時間及初始濃度對吸附去除性能的影響,并對吸附過程進(jìn)行了動力學(xué)、等溫模型和熱力學(xué)分析。結(jié)果表明復(fù)合吸附劑在堿性條件下表現(xiàn)出較好的吸附能力,吸附量隨著時間的增加而增加,初始濃度越大,平衡吸附量也越大,但去除率卻隨之降低。吸附過程符合準(zhǔn)二級動力學(xué)方程和Freundlich型等溫模型,該吸附是自發(fā)的吸熱過程,吸附機(jī)理包括化學(xué)吸附和物理吸附。通過構(gòu)造非均相Fenton反應(yīng)體系,表面富集有強(qiáng)力霉素的Fe_3O_4@沙棘枝炭吸附劑可實(shí)現(xiàn)有效再生,重復(fù)使用。(2)通過熱裂解法經(jīng)一步合成了Fe_3O_4@沙棘枝炭復(fù)合吸附劑。進(jìn)行了XRD、SEM結(jié)構(gòu)表征和磁性檢測。結(jié)果表明沙棘枝炭呈無定形態(tài),Fe_3O_4晶型為面心立方型。粒徑約為41 nm,在沙棘枝炭表面呈孤島狀分布。微觀負(fù)載Fe_3O_4納米顆粒使得Fe_3O_4@沙棘枝炭復(fù)合吸附劑展示出了宏觀磁性。運(yùn)用BBD型響應(yīng)面法,建立了Fe_3O_4@沙棘枝炭固定床吸附去除亞甲藍(lán)固定床反應(yīng)器的吸附模型,對其響應(yīng)面進(jìn)行了分析。結(jié)果表明響應(yīng)面法建立的模型可準(zhǔn)確描述吸附過程,且濃度、流速、pH、濃度平方和pH平方效應(yīng)顯著。隨著流速的降低、濃度的降低和pH的升高,去除率增大。進(jìn)行了再生實(shí)驗(yàn),并探討了再生機(jī)理,表明該鐵系非均相Fenton氧化可有效實(shí)現(xiàn)吸附劑的再生重復(fù)利用。(3)在不使用交聯(lián)劑的條件下,通過簡單的低溫水熱法合成β-FeOOH@沙棘枝炭復(fù)合吸附劑。對其進(jìn)行XRD、SEM和EDS表征,在表征的基礎(chǔ)上,提出β-FeOOH@沙棘枝炭復(fù)合吸附劑的合成機(jī)理。在固定床反應(yīng)器中處理抗生素廢水,探討了抗生素廢水初始濃度(22-32 mg·L-1)、流速(1-3 mL·min-1)、床高(0.7-1.5 cm)和pH(2-11)對吸附去除性能的影響,并使用Thomas和Yoon-Nelson模型對吸附過程進(jìn)行了擬合。此后對β-FeOOH@沙棘枝炭復(fù)合吸附劑進(jìn)行了原位再生實(shí)驗(yàn),在沙棘枝炭的吸附性能和β-FeOOH氧化性能的協(xié)同作用下,復(fù)合吸附劑有效再生。表明β-FeOOH@沙棘枝炭復(fù)合吸附劑在水處理領(lǐng)域是一種廉價有效的具有應(yīng)用前景的新型材料。
[Abstract]:Activated carbon adsorption is a widely used wastewater treatment method for removing pollutants in water, but high cost commercial activated carbon has increased the operating cost of wastewater treatment. Based on this, the preparation of activated carbon from agricultural waste biomass has been widely concerned in recent years. Seabuckthorn is a deciduous shrub, widely distributed in high altitude areas. However, the Seabuckthorn branches produced during the harvest of seabuckthorn fruit have caused a series of environmental pollution problems because of the random discarding and in-situ incineration. As a typical carbon rich, cheap and abundant agricultural solid waste, the Seabuckthorn branch is a sustainable and natural source of biological carbon, which is suitable for the preparation of activated carbon. But single Seabuckthorn charcoal adsorption can not achieve the purpose of low cost, high efficiency and no two pollution. Therefore, the introduction of iron based nanoparticles on the surface of seabuckthorn branch carbon, increasing the surface area to improve the adsorption performance, construction of heterogeneous Fenton system, to realize the recycling of adsorbents, to prevent the two pollution to further reduce costs, The composite adsorbents were applied to the treatment of antibiotic wastewater and dye wastewater, and the adsorption and regeneration properties of the composite were investigated. The contents of the study were as follows: (1) the carbon composite of Fe_3O_4@ Seabuckthorn was prepared by thermal cracking after impregnating the abandoned Seabuckthorn branches and impregnating iron ions. The results of adsorbents.SEM and EDS show that the particle size of nano Fe_3O_4 particles is about 40 nm, which is partially covered on the surface of carbon, and the monodisperse.XRD shows that the nanoscale Fe_3O_4 is a surface centered cubic crystal and the carbon is amorphous. The effects of pH, adsorption time and initial concentration on the adsorption removal performance are discussed, and the adsorption is adsorbed on the adsorption and adsorption properties. The kinetics, isothermal model and thermodynamic analysis showed that the adsorption capacity of the composite adsorbent was better under the alkaline condition. The adsorption amount increased with the time, the larger the initial concentration, the greater the equilibrium adsorption, but the removal rate decreased. The adsorption process was in accordance with the quasi two stage kinetic equation and Freundlich. The adsorption is a spontaneous endothermic process. The adsorption mechanism includes chemical adsorption and physical adsorption. By constructing an heterogeneous Fenton reaction system, the surface enrichment of Fe_3O_4@ Seabuckthorn charcoal adsorbents with doxycycline can be effectively regenerated and reused. (2) the carbon composite absorption of Fe_3O_4@ Seabuckthorn was synthesized by thermal decomposition. The structure characterization and magnetic detection of XRD, SEM are carried out. The results show that the charcoal of seabuckthorn is amorphous and the Fe_3O_4 crystal is face centered cubic. The particle size is about 41 nm, and it is isolated in the surface of the charcoal surface of seabuckthorn branches. The micro load Fe_3O_4 nanoparticles show the macro magnetic properties of the Fe_3O_4@ Seabuckthorn branch carbon compound absorption agent, and use the BBD response surface. The adsorption model of Fe_3O_4@ Seabuckthorn branch carbon fixed bed adsorbed to remove methylene blue fixed bed reactor was established. The response surface of the reactor was analyzed. The results showed that the model established by the response surface method could accurately describe the adsorption process, and the concentration, flow rate, pH, concentration square and pH square effect should be significant. With the decrease of velocity, the decrease of concentration and the rise of pH. The regeneration experiment was carried out, and the regeneration mechanism was carried out, and the regeneration mechanism was discussed. It was shown that the iron-based heterogeneous Fenton oxidation could effectively reuse the adsorbents. (3) under the condition of without crosslinking agent, a simple low temperature hydrothermal method was used to synthesize the carbon composite adsorbents of the beta -FeOOH@ Seabuckthorn branch carbon. It was characterized by XRD, SEM and EDS. On the basis of the sign, the synthesis mechanism of -FeOOH@ Seabuckthorn branch carbon composite adsorbent was proposed. Treatment of antibiotic wastewater in a fixed bed reactor was carried out. The initial concentration of antibiotic wastewater (22-32 mg. L-1), flow rate (1-3 mL. Min-1), bed height (0.7-1.5 cm) and pH (2-11) on the absorption and removal performance were investigated, and the adsorption of the adsorbents by Thomas and Yoon-Nelson models was used. The process was fitted. The in situ regeneration experiment was carried out on the carbon composite adsorbent of -FeOOH@ Seabuckthorn branch. The compound adsorbent was effectively regenerated under the synergistic effect of the adsorption property of the charcoal and the oxidation performance of the beta -FeOOH. The results showed that the compound adsorbent for the beta -FeOOH@ Seabuckthorn branch carbon composite adsorbent was a cheap and effective application prospect in the field of water treatment. A new type of material.
【學(xué)位授予單位】:長安大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:TB33;TQ424

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