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Enhanced Uptake of Natural Organic Matter by Modified Granular Activated Carbons 改性颗粒活性炭对天然有机物的吸收
发布日期: 2003-06-15
碳文献中有丰富的碳合成方法和表面改性制备方法 具有特定应用类型所需物理化学性质的材料。我们的 过去,人们对溶解有机物(DOM)及其被颗粒活性炭(GAC)吸附的认识有了很大的提高 二十年。因此,本研究的主要目的是开发定制的激活剂 碳用于增强和选择性去除天然水体中的DOM。基于大型 根据DOM的大小,假设适合该应用的吸附剂类型 应具有足够的中孔度(即,较大的孔隙体积和 表面积应在孔隙中(gt2nm)。同时,DOM是一种异质混合物 在天然水中具有带负电荷和酸性功能的极性分子。由于 它们的亲水性,溶剂性- 动机吸附(即疏水性效应)不受影响 预计将在GAC从水中去除DOM分子方面发挥重要作用。 因此,进一步假设,为了增强和有效去除DOM,碳 表面应具有基本性质,携带总的正电荷,携带特定的电荷 功能,或所有这些特性的最佳组合。 可以通过选择不同的起始材料来控制碳孔隙率 使用不同处理方案的吸收剂的孔隙率或扩大微孔。二者都 本研究采用了多种方法。三种活性炭(微孔F400,介孔WVBMESO 选择WVB-MACRO作为吸附剂。获得了virgin和 本文介绍并讨论了改性F400碳。类似的研究 介孔碳正在研究中。 使用三种主要方法对每个碳表面进行了修改: He或He下的热处理 氢气气氛;在低温和高温下进行NH3处理,有无预氧化 用硝酸;还有,浸铁。热处理和氨水处理提高了水的碱度 碳表面。此外,不同温度下的氨处理会带来不同的影响 碳表面的含氮功能,可能与DOM相互作用 组件。氨处理后的氧化会扩大碳孔,同时 增加表面碱度值和含氮功能的数量。 分散在碳表面的铁阳离子,甚至零价铁,可以显著地 增强DOM组分对碳表面的亲和力。最近获得的结果 在制定强化凝血指南的过程中,我们发现 与铝混凝剂相比,使用铁混凝剂去除更多DOC(Randtke等) 艾尔。 , 1999; 爱德华兹,1997年)。数据还表明,不可移动DOM的某些部分 明矾可以用氯化铁去除。因此,预计GAC对DOM的吸收 通过促进:阳离子铁物种和 阴离子DOM分子;和/或在铁和DOM之间形成有利的络合物 种 由于采用了不同的处理方法来制备不同的吸附剂,因此改性后的吸附剂 碳被命名为描述所用处理程序的缩写代码: He:在900℃下氦流下热处理2小时;H:在900℃下热处理2小时 在氢气流动下;16NO:用沸腾的浓硝酸氧化1小时; 8N2H:在800℃下用氨处理2小时;4N1H:在 400摄氏度1小时;Fe3E和FeS:离子交换浸铁和初期浸铁 分别采用湿润法。例如F400- He-16NO是F400的碳原子,是热原子 在氦气下处理,然后用浓硝酸氧化。处女和改良 通过比表面积和孔径分布分析、pHPZC、, 元素分析、水蒸气吸附、酸碱吸收和铁分析 样品。 我们
Carbon literature is rich in methods on carbon synthesis and surface modification to prepare materials with desired physicochemical properties for a particular type of application. Our understanding about dissolved organic matter (DOM) and its adsorption by granular activated carbon (GAC) have greatly improved within the past two decades. Therefore, the main objective of this research was to develop tailored activated carbons for enhanced and selective removal of DOM from natural waters. Based on the large size of the DOM, it is hypothesized that the proper type of adsorbents for this application should have a sufficient amount of mesoporosity (i.e., a larger fraction of pore volume and surface area should be in the pores >2nm). At the same time, DOM is a heterogenous mixture of polar molecules with negatively charged and acidic functionalities in natural waters. Due to their hydrophilic nature, solvent-motivated adsorption (i.e., hydrophobicity effect) is not expected to play a major role in the removal of DOM molecules by GAC from water. Therefore, it is further hypothesized that for enhanced and effective DOM removal, the carbon surface should have basic properties, carry an overall positive charge, carry specific functionalities, or an optimum combination of all these characteristics. It is possible to control carbon porosity by either selecting starting materials with different porosities or enlarging micropores of a sorbent using different treatment schemes. Both approaches were used in this study. Three GACs (microporous F400, mesoporous WVBMESO and WVB-MACRO) were selected as sorbents. Obtained results of virgin and modified F400 carbons are presented and discussed in this paper. A similar study of mesoporous carbons is in progress. Each carbon surface was modified using three main approaches: heat treatment under He or H2 atmosphere; NH3 treatment at low and high temperatures with or without pre-oxidation with HNO3; and, iron impregnation. Heat and ammonia treatments enhance the basicity of carbon surface. In addition, ammonia treatment at different temperatures introduces various nitrogen-containing functionalities to the carbon surface, which may interact with DOM components. Oxidation followed by ammonia treatment enlarges carbon pores while increasing the value of surface basicity and the number of nitrogen-containing functionalities. Iron cations, or even zero-valent iron, dispersed on the carbon surface can significantly enhance affinity of DOM components toward the carbon surface. Recent results obtained during the development of enhanced coagulation guidelines indicated that it is possible to remove more DOC using iron coagulants, compared with aluminum coagulants (Randtke, et al., 1999; Edwards, 1997). Data indicated also that some fractions of non-removable DOM by alum could be removed by iron chloride. Therefore, it is expected that DOM uptake by GACs be increased by promoting: electrostatic attractions between cationic iron species and anionic DOM molecules; and/or favorable complex formation between the iron and DOM species. Since various treatment routes have been used to prepare different sorbents, the modified carbons were named with abbreviation codes describing the treatment procedures employed: He: heat treatment at 900C for 2hr under helium flow; H: heat treatment at 900C for 2hr under hydrogen flow; 16NO: oxidation by using boiling concentrated nitric acid for 1hr; 8N2H: treatment with ammonia at 800C for 2hr; 4N1H: treatment with ammonia at 400C for 1hr; and, Fe3E and FeS: iron impregnation by ion exchange and incipient wetness methods, respectively. For example F400-He-16NO is the F400 carbon that was heat treated under helium and then oxidized with concentrated nitric acid. Virgin and modified carbons were characterized by surface area and pore size distribution analysis, pHPZC, elemental analysis, water vapor adsoption, acid/base uptake, and iron analysis of digested samples. DOM samples we
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发布单位或类别: 美国-美国给水工程协会
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