本文選題：重金屬?gòu)U水 + 碳基復(fù)合材料�。� 參考：《江蘇大學(xué)》2017年碩士論文

【摘要】：近年來(lái),由于工農(nóng)業(yè)的飛速發(fā)展,所伴隨的環(huán)境污染問(wèn)題日益嚴(yán)重,其中重金屬污染問(wèn)題尤為突出,如何有效解決重金屬污染問(wèn)題,一直是研究人員的研究重點(diǎn)。碳基復(fù)合材料由于其優(yōu)異的理化特性,非常適合應(yīng)用在重金屬?gòu)U水的處理過(guò)程中。本文制備了三種富含羧基的碳基復(fù)合材料:片狀Fe_3O_4/羧基碳復(fù)合材料、TiO_2/羧基碳復(fù)合材料、Fe_3O_4/羧基碳復(fù)合材料,并將三種碳基復(fù)合材料分別應(yīng)用于含鉻廢水中Cr(Ⅵ)的光催化還原以及含銅廢水中銅離子的吸附。此外,以鋼廠酸洗含鐵廢水和電鍍含鎳廢水為原料制備了基于NiFe_2O_4的重金屬污泥,將該重金屬污泥作為電極材料組裝成水系對(duì)稱(chēng)電池并進(jìn)行了電池性能的研究。主要研究?jī)?nèi)容如下:(1)以FeSO_4·7H_2O、葡萄糖和EDTA為原料,通過(guò)低溫碳化法一步合成了富含羧酸鐵配合物的片狀Fe_3O_4/羧基碳復(fù)合材料。片狀Fe_3O_4/羧基碳復(fù)合材料以片狀無(wú)定形碳作為載體,Fe_3O_4納米顆粒均勻地分散在碳片中,并與EDTA中羧基配位形成羧酸鐵配合物(Fe~Ⅱ(R-COO_)n~(2-n)和 Fe~Ⅲ(R-COO)_n~(3-n))。片狀Fe_3O_4/羧基碳復(fù)合材料中存在大量的羧酸鐵配合物,使得該材料具有優(yōu)異的可見(jiàn)光吸收能�？梢�(jiàn)光照射下,Fe~Ⅱ(R-COO)_n~(2-n)和Fe~Ⅲ(R-COO)_n~(3-n)之間的Fe(Ⅱ)/Fe(Ⅲ)光催化循環(huán),使得片狀Fe_3O_4/羧基碳復(fù)合材料具有優(yōu)異的可見(jiàn)光光催化還原Cr(Ⅵ)能力。此外,反應(yīng)完成后,片狀Fe_3O_4/羧基碳復(fù)合材料可通過(guò)磁性分離。(2)以鈦酸四丁酯、葡萄糖和EDTA為原料,通過(guò)低溫碳化法合成了TiO_2/羧基碳復(fù)合材料。通過(guò)Raman,SEM,EDS和TEM的表征,證實(shí)了TiO_2/羧基碳復(fù)合材料為納米TiO_2顆粒均勻地分散在片狀無(wú)定形碳中的結(jié)構(gòu)。通過(guò)FT-IR和XPS譜圖證明了TiO_2/羧基碳復(fù)合材料中含有大量羧基,并與TiO_2顆粒形成了TiO_2/EDTA配合物。TiO_2/羧基碳復(fù)合材料具有優(yōu)異的可見(jiàn)光吸收性能和光催化還原Cr(Ⅵ)能力�？梢�(jiàn)光下,TiO_2/EDTA配合物通過(guò)配體到金屬的電荷轉(zhuǎn)移過(guò)程(ligand-to-metal charge transfer,LMCT)實(shí)現(xiàn)對(duì)Cr(Ⅵ)的光催化還原。(3)以FeSO_4·7H_2O和葡萄糖酸鈉作為原料,通過(guò)一步低溫碳化法合成Fe_3O_4/羧基碳復(fù)合材料。葡萄糖酸鈉中的羧基與Fe(Ⅱ)配位形成羧酸鐵配合物。在低溫碳化過(guò)程中,部分羧酸鐵配合物熱分解為Fe_3O_4,大量的羧基仍保留在無(wú)定形碳中。Fe_3O_4/羧基碳復(fù)合材料富含的羧基有利于對(duì)水中Cu(Ⅱ)的吸附。Fe_3O_4/羧基碳復(fù)合材料具有優(yōu)異的Cu(Ⅱ)吸附性能,其最大吸附容量為66.67 mg/g。以Fe_3O_4/羧基碳復(fù)合材料為吸附劑,進(jìn)行了吸附動(dòng)力學(xué)與熱力學(xué)的研究。在各種動(dòng)力學(xué)和等溫線(xiàn)模型中,準(zhǔn)二級(jí)動(dòng)力學(xué)模型和Langmuir模型更符合Fe_3O_4/羧基碳復(fù)合材料對(duì)Cu(Ⅱ)的吸附過(guò)程。吸附結(jié)束后,Fe_3O_4/羧基碳復(fù)合材料可通過(guò)磁性分離。Fe_3O_4/羧基碳復(fù)合材料具有優(yōu)異的穩(wěn)定性,在酸性溶液中脫附后,可循環(huán)使用。(4)以鋼廠酸洗含鐵廢水和電鍍含鎳廢水為原料,經(jīng)中和沉淀以及水熱反應(yīng),獲得基于NiFe_2O_4的重金屬污泥。將基于NiFe_2O_4的重金屬污泥作為電極材料,構(gòu)建NiFe_2O_4//NiFe_2O_4水系對(duì)稱(chēng)電池。經(jīng)電化學(xué)性能測(cè)試分析,Ni Fe2O4//NiFe_2O_4水系對(duì)稱(chēng)電池在放電電流密度為0.5 A/g時(shí),比容量為23.1 mAh/g。NiFe_2O_4//NiFe_2O_4水系對(duì)稱(chēng)電池也具有一定的循環(huán)壽命,在500次充放電循環(huán)后,比容量仍能維持在最大比容量的90%。通過(guò)XRD和毒性浸出實(shí)驗(yàn)的檢測(cè)分析,經(jīng)過(guò)500次充放電循環(huán)后,NiFe_2O_4仍表現(xiàn)出良好的穩(wěn)定性,可視為一般的工業(yè)廢物。
[Abstract]:In recent years, due to the rapid development of industry and agriculture, the problem of environmental pollution is becoming more and more serious, and the problem of heavy metal pollution is particularly prominent. How to effectively solve the problem of heavy metal pollution has always been the research focus of the researchers. Because of its excellent physical and chemical properties, carbon based composites are very suitable for the treatment of heavy metal wastewater. In this paper, three kinds of carbon based composites rich in carboxyl were prepared: sheet Fe_3O_4/ carboxy carbon composites, TiO_2/ carboxy carbon composites, Fe_3O_4/ carboxy carbon composites, and three kinds of carbon based composites used in the photocatalytic reduction of Cr (VI) in chromium containing wastewater and copper ions in copper waste water. The heavy metal sludge based on NiFe_2O_4 was prepared by acid washing iron containing wastewater and electroplated nickel containing wastewater. The heavy metal sludge was assembled into a symmetrical battery of water system and the performance of the battery was studied. The main contents are as follows: (1) FeSO_4. 7H_2O, glucose and EDTA were used as raw materials, and a one-step synthesis by low temperature carbonization was made. Sheet like Fe_3O_4/ carboxyl carbon composites rich in carboxylic iron complexes. The sheet like Fe_3O_4/ carboxy carbon composites are dispersed in carbon slices with flaky amorphous carbon and Fe_3O_4 nanoparticles are evenly distributed in the carbon sheets and formed with carboxyl groups in EDTA to form iron carboxylic complexes (Fe~ (R-COO_) n~ (2-N) and Fe~ III (R-COO) _n~ (3-N)). There are a large number of carboxylic iron complexes in carbon composites, which make the material have excellent visible absorption energy. Under visible light, the Fe (II) /Fe (III) photocatalytic cycle between Fe~ II (R-COO) _n~ (2-N) and Fe~ III (R-COO) _n~ (3-N) makes the flaky Fe_3O_4/ carboxy carbon composites have excellent visible light photocatalytic reduction Cr (VI) capacity. In addition, after the reaction was completed, the Fe_3O_4/ carboxyl carbon composites could be separated by magnetic separation. (2) the TiO_2/ carboxyl carbon composites were synthesized with four butyl titanate, glucose and EDTA as raw materials by low temperature carbonization. Through the characterization of Raman, SEM, EDS and TEM, it was proved that the TiO_2/ carboxyl carbon composite was dispersed uniformly in the nanometer TiO_2 particles in the tablet. The structure in amorphous carbon is shown by FT-IR and XPS spectra. It is proved that the TiO_2/ carboxyl carbon composite contains a large number of carboxyl groups, and the TiO_2/EDTA complex,.TiO_2/ carboxyl carbon composite, has excellent visible absorption properties and photocatalytic reduction of Cr (VI) ability with TiO_2 particles. Under visible light, TiO_2/EDTA complexes pass through the ligand to the ligand. The photocatalytic reduction of Cr (VI) was realized by the charge transfer process (ligand-to-metal charge transfer, LMCT). (3) Fe_3O_4/ carboxyl carbon composite was synthesized by one step low temperature carbonization with FeSO_4 7H_2O and sodium gluconate. The carboxyl group in sodium gluconate and Fe (II) coordination formed a carboxylic acid iron complex. During the process, partial carboxyl iron complexes are heated to Fe_3O_4, and a large number of carboxyl groups remain in amorphous carbon and carboxyl rich in.Fe_3O_4/ carboxyl carbon composites are favorable for the adsorption of Cu (II) on the adsorption of.Fe_3O_4/ carboxyl carbon composites in water Cu (II), and the maximum adsorption capacity is 66.67 mg/g. with Fe_3O_4/ carboxyl carbon composite The adsorption kinetics and thermodynamics were studied as adsorbents. In various kinetic and isotherm models, the quasi two stage kinetic model and the Langmuir model were more consistent with the adsorption process of Fe_3O_4/ carboxy carbon composites on Cu (II). After the adsorption, the Fe_3O_4/ carboxyl carbon composites could be compound by magnetic separation of.Fe_3O_4/ carboxyl carbon. The material has excellent stability and can be recycled in acid solution. (4) the heavy metal sludge based on NiFe_2O_4 is obtained by neutralization and precipitation and hydrothermal reaction. The heavy metal sludge based on NiFe_2O_4 is used as the electrode material to construct NiFe_2O_4//NiFe_2O_4 water. When the discharge current density is 0.5 A/g, the symmetric cell of Ni Fe2O4//NiFe_2O_4 water system also has a certain cycle life when the discharge current density is 23.1 mAh/g.NiFe_2O_4//NiFe_2O_4. After the 500 charge discharge cycle, the specific volume can still be maintained at the maximum specific capacity of 90%. through XRD and. After testing and analysis of toxic leaching experiments, after 500 charge and discharge cycles, NiFe_2O_4 still showed good stability, which could be regarded as a general industrial waste.
【學(xué)位授予單位】：江蘇大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類(lèi)號(hào)】：X703

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