辉光放电电解等离子体引发制备凹凸棒高分子材料及其应用
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摘要
辉光放电电解是一种新型的电化学过程,属于非法拉第电解过程,其中等离子体由电极和电解质液面之间的直流辉光放电来维持。当两极间的电压足够高时,常规电解自动转化为辉光放电电解,从而产生等离子体。等离子体中的某些高活性组分如H·,·OH,H_2O_2,e~-_(aq),HO_2·为各种类型的溶液化学反应提供了高能活性粒子。本文研究了辉光放电电解等离子体技术在制备高分子材料方面的应用,主要内容如下:
第一章简单介绍了等离子体的特征,低温等离子体的产生方法和主要应用领域,并综述了辉光放电电解等离子体在废水处理、化学合成以及高分子材料方面的应用和研究进展。
第二章以丙烯酸和凹凸棒土为原料,N,N’-亚甲基双丙烯酰胺为交联剂,采用辉光放电等离子体引发聚合法在水溶液中一步制得凹凸棒/聚丙烯酸高吸水性复合材料。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对树脂吸水率的影响,并用红外光谱(FTIR)、扫描电子显微镜(SEM)和热重分析(TGA)表征了复合材料的结构、形态和性能。结果表明:在最佳条件下,复合材料性能良好,吸水率为1281 g/g,对0.9% NaCl水溶液的吸附率为111 g/g。
第三章研究了制备的聚丙烯酸/凹凸棒复合材料对Cu~(2+)吸附行为。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对吸附率的影响,结果表明:该吸附剂对水溶液中的铜离子具有较高的去除率。吸附过程动力学符合假二级速率方程。在所研究的浓度范围内,铜离子的吸附符合Langmuir吸附。
第四章以丙烯酸、丙烯酰胺和凹凸棒土为原料,N,N’-亚甲基双丙烯酰胺为交联剂,采用辉光放电电解等离子体引发聚合法在水溶液中一步制得凹凸棒/聚丙烯酸高吸水性复合材料。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对树脂吸水率的影响,并用红外光谱(FTIR)、扫描电镜(SEM)和热重分析(TGA)表征了复合材料的结构、形态和性能。结果表明:在最佳条件下,复合材料性能良好,吸水率为1350 g/g。第五章研究了制备的聚丙烯酸/丙烯酰胺/凹凸棒复合材料对水溶液中Cu~(2+),Pb~(2+)的吸附行为,考查了放电电压、交联剂用量、单体质量比及凹凸棒土含量等对复合材料吸附量的影响,从动力学和热力学角度分别分析了该吸附剂对Cu~(2+)和Pb~(2+)的吸附过程。结果表明该吸附剂对铜离子、铅离子有较高的去除率。吸附过程动力学符合假二级速率方程Langmuir吸附模型。
Glow discharge electrolysis is a kind of novel electrochemical process and non-Faraday electrolysis process. The plasma is sustained by a direct current (DC) glow discharge between an electrode and the surface of electrolyte. The conventional electrolysis turned into glow discharge electrolysis when the applied voltage is high enough in aqueous media. There are a lot of energetic species to produce by glow discharge electrolysis, such as H_2O_2,·OH,·H, e~-_(aq), HO_2·and so on, and these energetic species can diffuse into the solution around the anode. Therefore, glow discharge plasma can provide rich active intermediates for many kinds of chemical reactions in aqueous solution under ordinary conditions. In this work, glow discharge plasma technology is employed to synthesize polymer materials.
This main conclusions are summaried as below:
(1) The characteristics of plasma were described. Methods to produce cold plasma and their applications in wastewater treatment, chemical synthesis and polymer materials were also discussed in brief.
(2) Amounts of graft polymerization of acrylic acid on attapulgite substrate was carried out and a novel polyacrylic acid/attapulgite composite superabsorbent was prepared by using glow discharge electrolysis plasma initiating, in which acrylic acid and attapulgite were used as raw materials and N,N’-methylenebisacrylamide as the crosslinking agent. Effects of the experimental conditions such as discharge voltage, amounts of crosslinking agent, attapulgite and acrylic acid on the absorbency was discussed in detail and the resulting product was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM). The resulting superabsorbent has higher water absorbency which reaches 1281g/g for distilled water and 111g/g for 0.9% NaCl solution, respectively.
(3) Adsorption of synthesized polyacrylic/attapulgite composite adsorbent to Cu~(2+) was Investigated. It was found that the adsorbent had higher removal effenciey for Cu~(2+) and the adsorption process obeyed pseudo-second-order dynamic equation and Langmuir model.
(4) Polyacrylic/acrylamide/attapulgite composite superabsorbent was synthesized through a graft polymerization initiated by glow discharge electrolysis plasma, where acrylic acid and attapulgite were used as raw materials and N, N’-methylenebisacrylamide as the crosslinking agent. Effects of the discharge voltage, amounts of crosslinking agent, attapulgite, the ratio of amounts of acrylic acid to acryylamide and neutralization on the absorbency were discussed in detail. The resulting product was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM). The prepared superabsorbent has very high water absorbency of 1350g/g for distilled water.
(5) Adsorption behavbious of synthesized poly acrylic/acrylamide/attapulgite composite adsorbent were studied to Cu(II) and Pb(II). The adsorption process obeyed pseudo-second-order dynamic equation and Langmuir model.
第一章简单介绍了等离子体的特征,低温等离子体的产生方法和主要应用领域,并综述了辉光放电电解等离子体在废水处理、化学合成以及高分子材料方面的应用和研究进展。
第二章以丙烯酸和凹凸棒土为原料,N,N’-亚甲基双丙烯酰胺为交联剂,采用辉光放电等离子体引发聚合法在水溶液中一步制得凹凸棒/聚丙烯酸高吸水性复合材料。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对树脂吸水率的影响,并用红外光谱(FTIR)、扫描电子显微镜(SEM)和热重分析(TGA)表征了复合材料的结构、形态和性能。结果表明:在最佳条件下,复合材料性能良好,吸水率为1281 g/g,对0.9% NaCl水溶液的吸附率为111 g/g。
第三章研究了制备的聚丙烯酸/凹凸棒复合材料对Cu~(2+)吸附行为。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对吸附率的影响,结果表明:该吸附剂对水溶液中的铜离子具有较高的去除率。吸附过程动力学符合假二级速率方程。在所研究的浓度范围内,铜离子的吸附符合Langmuir吸附。
第四章以丙烯酸、丙烯酰胺和凹凸棒土为原料,N,N’-亚甲基双丙烯酰胺为交联剂,采用辉光放电电解等离子体引发聚合法在水溶液中一步制得凹凸棒/聚丙烯酸高吸水性复合材料。考查了放电电压、交联剂用量、单体浓度及凹凸棒土含量对树脂吸水率的影响,并用红外光谱(FTIR)、扫描电镜(SEM)和热重分析(TGA)表征了复合材料的结构、形态和性能。结果表明:在最佳条件下,复合材料性能良好,吸水率为1350 g/g。第五章研究了制备的聚丙烯酸/丙烯酰胺/凹凸棒复合材料对水溶液中Cu~(2+),Pb~(2+)的吸附行为,考查了放电电压、交联剂用量、单体质量比及凹凸棒土含量等对复合材料吸附量的影响,从动力学和热力学角度分别分析了该吸附剂对Cu~(2+)和Pb~(2+)的吸附过程。结果表明该吸附剂对铜离子、铅离子有较高的去除率。吸附过程动力学符合假二级速率方程Langmuir吸附模型。
Glow discharge electrolysis is a kind of novel electrochemical process and non-Faraday electrolysis process. The plasma is sustained by a direct current (DC) glow discharge between an electrode and the surface of electrolyte. The conventional electrolysis turned into glow discharge electrolysis when the applied voltage is high enough in aqueous media. There are a lot of energetic species to produce by glow discharge electrolysis, such as H_2O_2,·OH,·H, e~-_(aq), HO_2·and so on, and these energetic species can diffuse into the solution around the anode. Therefore, glow discharge plasma can provide rich active intermediates for many kinds of chemical reactions in aqueous solution under ordinary conditions. In this work, glow discharge plasma technology is employed to synthesize polymer materials.
This main conclusions are summaried as below:
(1) The characteristics of plasma were described. Methods to produce cold plasma and their applications in wastewater treatment, chemical synthesis and polymer materials were also discussed in brief.
(2) Amounts of graft polymerization of acrylic acid on attapulgite substrate was carried out and a novel polyacrylic acid/attapulgite composite superabsorbent was prepared by using glow discharge electrolysis plasma initiating, in which acrylic acid and attapulgite were used as raw materials and N,N’-methylenebisacrylamide as the crosslinking agent. Effects of the experimental conditions such as discharge voltage, amounts of crosslinking agent, attapulgite and acrylic acid on the absorbency was discussed in detail and the resulting product was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM). The resulting superabsorbent has higher water absorbency which reaches 1281g/g for distilled water and 111g/g for 0.9% NaCl solution, respectively.
(3) Adsorption of synthesized polyacrylic/attapulgite composite adsorbent to Cu~(2+) was Investigated. It was found that the adsorbent had higher removal effenciey for Cu~(2+) and the adsorption process obeyed pseudo-second-order dynamic equation and Langmuir model.
(4) Polyacrylic/acrylamide/attapulgite composite superabsorbent was synthesized through a graft polymerization initiated by glow discharge electrolysis plasma, where acrylic acid and attapulgite were used as raw materials and N, N’-methylenebisacrylamide as the crosslinking agent. Effects of the discharge voltage, amounts of crosslinking agent, attapulgite, the ratio of amounts of acrylic acid to acryylamide and neutralization on the absorbency were discussed in detail. The resulting product was characterized by Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA) and scanning electron microscopy (SEM). The prepared superabsorbent has very high water absorbency of 1350g/g for distilled water.
(5) Adsorption behavbious of synthesized poly acrylic/acrylamide/attapulgite composite adsorbent were studied to Cu(II) and Pb(II). The adsorption process obeyed pseudo-second-order dynamic equation and Langmuir model.
引文
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