本文選題：金屬亞鐵氰化物 + 羧甲基纖維素鈉��； 參考：《西南科技大學(xué)》2017年碩士論文

【摘要】：自2011年福島核電站發(fā)生核事故以來,放射性核素的廢液處理技術(shù)已經(jīng)成為重點(diǎn)研究的內(nèi)容之一,而銫在放射性核素中占很大的份額,由于其半衰期長,對(duì)人類的健康帶來嚴(yán)重的危害,因此,除去廢水中的銫離子十分必要。吸附法因其成本低、工藝簡單和高效而備受關(guān)注,但是其除銫效果受吸附劑的制約。金屬亞鐵氰化物具有獨(dú)特的選擇性、極高的化學(xué)穩(wěn)定性等優(yōu)點(diǎn),因此,此材料一直以來是放射性銫廢水處理領(lǐng)域的研究熱點(diǎn)之一。羧甲基纖維素是一種水溶性纖維素醚,由于其在多價(jià)離子的存在下可以形成凝膠微球而常作為增稠劑、包埋劑等。本文以羧甲基纖維素鈉為載體,以金屬亞鐵氰化物為活性成分,采用包埋法、原位合成法等固化技術(shù)分別制備了羧甲基纖維素鈉/普魯士藍(lán)交聯(lián)鑭凝膠微球(CMC/PB-La)、普魯士藍(lán)微球(CMC-PB)和亞鐵氰化銅復(fù)合顆粒(CMC-KCu FC)吸附材料,詳細(xì)探討三種吸附材料對(duì)模擬含銫廢水中Cs+的吸附去除性能,并研究了三種吸附劑對(duì)銫離子的吸附動(dòng)力學(xué)、熱力學(xué)及吸附等溫模型,以及吸附劑的洗脫和可能的吸附機(jī)理,主要研究結(jié)果如下:1、利用包埋法制備了CMC/PB-La凝膠微球吸附劑,考察了p H、吸附劑用量、反應(yīng)時(shí)間、初始銫離子濃度和輻射穩(wěn)定性等因素對(duì)銫的吸附性能影響。得出制備CMC/PB-La凝膠微球的最佳吸附條件為:吸附劑用量為1 g/L,吸附時(shí)間為1000 min,溫度為298.15 K,溶液中K+的存在會(huì)影響吸附劑除銫效果;吸附過程符合Freundlich等溫吸附模型和準(zhǔn)二級(jí)動(dòng)力學(xué)模型,當(dāng)溫度低于328.15 K,CMC/PB-La凝膠微球吸附銫離子是自發(fā)的吸熱過程,具有較好的輻射穩(wěn)定性;并通過SEM、FT-IR、EDX和XPS對(duì)吸附劑進(jìn)行表征測試。推測CMC/PB-La凝膠微球吸附銫離子的機(jī)理是物理吸附和化學(xué)吸附共同作用的結(jié)果。2、采用原位合成法制備了CMC-PB凝膠微球吸附材料,并研究了其吸附銫離子的特性。結(jié)果表明吸附銫離子的優(yōu)化條件為:p H為5,吸附劑的量為1.2 g/L,吸附時(shí)間為60 min,吸附銫離子起主要作用的是CMC-PB微球上的PB晶體。并對(duì)等溫模型、動(dòng)力學(xué)模型及熱力學(xué)進(jìn)行了研究,結(jié)果表明:吸附過程符合Langmuir等溫模型及準(zhǔn)二級(jí)動(dòng)力學(xué)模型,最大吸附量為115.04 mg·g~(-1),從計(jì)算的熱力學(xué)數(shù)據(jù)可知,CMC-PB吸附銫離子是自發(fā)的吸熱過程。通過IR、XRD和XPS等手段有效的證明了PB被成功負(fù)載到了CMC載體上。其對(duì)銫離子吸附機(jī)理主要是化學(xué)離子交換吸附和物理吸附的作用。3、采用原位合成法制備了CMC-KCu FC復(fù)合顆粒吸附劑;批量實(shí)驗(yàn)考察了p H、吸附劑用量、接觸時(shí)間、初始銫離子濃度和共存離子等對(duì)CMC-KCu FC復(fù)合顆粒吸附性能的影響;采用SEM、FTIR、EDX和XRD等手段對(duì)合成的材料進(jìn)行分析。得出CMC-KCu FC復(fù)合微球吸附銫離子的優(yōu)化條件為:p H為5,吸附劑的量為0.4 g/L,吸附時(shí)間為600 min,溫度為298.15 K,且在K~+、Na~+、Ca~(2+)、Mg~(2+)和Li~+等陽離子共存條件下,其對(duì)銫的分配系數(shù)影響大小順序?yàn)?K~+Na~+Ca~(2+)Mg~(2+)Li~+。1.0 mol·L~(-1) KNO_3對(duì)銫離子的脫附率最大,其脫附率為36.8%。CMC-KCu FC復(fù)合顆粒吸附Cs~+的過程符合擬二階動(dòng)力學(xué)模型,可用Freundlich模型來描述。通過SEM、IR和XRD手段有效的證明了KCu FC被成功負(fù)載到了CMC載體上。4、討論了柱高、流速和銫離子的濃度對(duì)CMC-KCu FC復(fù)合顆粒動(dòng)態(tài)吸附的影響,結(jié)果表明,穿透點(diǎn)和耗竭點(diǎn)隨著柱高的增加而延后,穿透點(diǎn)和耗竭點(diǎn)隨著濃度和流速的的升高而縮短。
[Abstract]:Since the nuclear accident in Fukushima nuclear power plant occurred in 2011, the treatment technology of radioactive nuclide waste liquid has become one of the key research contents, and cesium occupies a large share in the radionuclide. Because of its long half-life, it has brought serious harm to human health. Therefore, it is necessary to remove cesium ions from the wastewater. Low, simple and efficient technology has attracted much attention, but its removal of cesium is restricted by adsorbents. Metal ferrocyanide has the advantages of unique selectivity and high chemical stability. Therefore, this material has always been a hot spot in the field of radioactive cesium wastewater treatment. Carboxymethyl cellulose is a water-soluble cellulose ether, which is a kind of water-soluble cellulose ether. In the presence of polyvalent ions, gel microspheres can be formed and often used as thickeners and embedding agents. In this paper, carboxymethyl fibrin sodium / Prussian blue crosslinked lanthanum Gel Microspheres (CMC/PB-La) were prepared by encapsulation and in situ synthesis using sodium carboxymethyl cellulose as the carrier and metal ferrocyanide as the active component. Prussian blue microspheres (CMC-PB) and copper ferrocyanide composite particles (CMC-KCu FC) adsorbents were used to investigate the adsorption and removal of Cs+ in simulated cesium containing wastewater by three kinds of adsorbents. The adsorption kinetics, thermodynamics and adsorption isothermal model of three kinds of adsorbents for cesium ions were studied, and the elution and possible adsorption mechanism of adsorbents were also studied. The main results are as follows: 1, the CMC/PB-La gel microsphere adsorbent was prepared by the embedding method. The effects of P H, the amount of adsorbents, the reaction time, the initial concentration of cesium ions and the radiation stability on the adsorption properties of cesium were investigated. The optimum adsorption conditions for the preparation of CMC/PB-La gel microspheres were obtained as follows: the dosage of adsorbents was 1 g/L and the adsorption time was 10. 00 min, the temperature is 298.15 K, the presence of K+ in the solution affects the effect of the adsorbents in the removal of cesium; the adsorption process conforms to the Freundlich isothermal adsorption model and the quasi two stage kinetic model. When the temperature is below 328.15 K, the adsorption of cesium ions by CMC/PB-La gel microspheres is a spontaneous endothermic process, with good radiation stability, and through SEM, FT-IR, EDX and XPS pairs. The mechanism of adsorbents was tested. The mechanism of the adsorption of cesium ions by CMC/PB-La gel microspheres was the result of the interaction of physical adsorption and chemical adsorption.2. The adsorption materials of CMC-PB gel microspheres were prepared by in situ synthesis method, and the characteristics of the adsorption of cesium ions were studied. The results showed that the optimum conditions for the absorption of cesium ions were as follows: P H was 5, adsorbents were adsorbents. The adsorption time is 1.2 g/L and the adsorption time is 60 min. The adsorption of cesium ions is the main function of the PB crystal on the CMC-PB microspheres. The isothermal model, kinetic model and thermodynamics are studied. The results show that the adsorption process conforms to the Langmuir isothermal model and the quasi two order kinetic model, the maximum adsorption amount is 115.04 mg. G~ (-1), from the calculated heat. It is known that CMC-PB adsorption of cesium ions is a spontaneous endothermic process. By means of IR, XRD and XPS, it is proved that PB has been successfully loaded onto the CMC carrier. The mechanism of the adsorption of cesium ions is mainly the action of chemical ion exchange adsorption and physical adsorption, and the CMC-KCu FC composite particle adsorbent is prepared by in situ synthesis method. The effects of P H, amount of adsorbents, contact time, initial concentration of cesium ions and coexisting ions on the adsorption properties of CMC-KCu FC composite particles were investigated. The synthetic materials were analyzed by means of SEM, FTIR, EDX and XRD. The optimum conditions for the adsorption of cesium ions by CMC-KCu FC composite microspheres were as follows: P H was 5, and the amount of adsorbent was 0.4. With a time of 600 min and a temperature of 298.15 K, and under the coexistence of K~+, Na~+, Ca~ (2+), Mg~ (2+) and Li~+, the order of the influence on the distribution coefficient of cesium is: K~+Na~+Ca~ (2+) Mg~. The two order kinetic model can be described by the Freundlich model. By means of SEM, IR and XRD, it is proved that KCu FC is successfully loaded onto.4 on the CMC carrier. The influence of column height, velocity and concentration of cesium ions on the dynamic adsorption of CMC-KCu FC composite particles is discussed. The results show that the penetration point and the exhaustion point are postponed with the increase of column height. The point and exhaustion point shorten with the increase of concentration and velocity.
【學(xué)位授予單位】：西南科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O647.3

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