活性炭吸附1,1,2,2-四氯乙烷的脱氯氢反应:碳基材料在土壤/沉积物修复中的应用
ehydrochlorination of activated carbon-bound 1,1,2,2-tetrachloroethane: Implications for carbonaceous material-based soil/sediment remediation
碳基材料如活性炭做为一种有效的吸附剂能够吸附一系列的有机污染物,并经常用在土壤和沉积物的修复中用于锁定有机污染物。然而,关于碳基材料吸附的有机污染的非生物转化活性的研究却很少(特别是长期的效应)。因此本论文研究了17种不同物理化学性质的活性炭吸附的低浓度TeCA (~1.25 mg/g)的碱催化动力学。在一定的pH条件下活性炭吸附的TeCA的反应动力学常数是溶解态TeCA反应动力学常数的13~70%,说明活性炭吸附的TeCA仍具有显著的反应活性。活性炭主要通过两种机制影响TeCA的反应活性。首先,去质子化的表面官能团(羧基和酚羟基)做为共轭碱促进TeCA的脱氯氢反应。其次,低浓度的TeCA可能主要富集在活性炭的微孔中(特别是直径为0.67~1.6 nm微孔中),这些微孔限制了OH- (与TeCA反应的亲核试剂)的进入。多孔碳基材料不仅能够用于锁定污染物,也能够对污染物进行原位降解,对碳基材料在环境中的应用具有重要的意义
arbonaceous materials such as activated carbon (AC) are effective adsorbents for a number of organic contaminants, and are often used in soil and sediment remediation to sequester organic contaminants. However, little is known about the abiotic reactivity (and thus, the long-term fate) of the carbonaceous material-bound contaminants. We studied the base-promoted dehydrochlorination kinetics of low-level ( 1.25 mg/g) 1,1,2, 2-tetrachloroethane (TeCA) adsorbed to 17 different ACs varying in origin and physicochemical properties. Activated carbon-bound TeCA exhibited significant reactivity-at a given pH the apparent reaction kinetic constants of AC-bound TeCA are 13-70% of the respective kinetic constants of dissolved TeCA. Binding to ACs likely have affected the reactivity of TeCA via two important mechanisms. First, the deprotonated surface O-functional groups (e.g., carboxyl and phenolic groups) catalyzed the base-promoted dehydrochlorination reaction by serving as the conjugate bases. Second, at low contaminant loadings TeCA molecules likely resided primarily in the micropores of ACs (particularly, micropores with diameters of 0.67-1.6 nm), wherein mass transfer of OH- (the nucleophile that reacts with TeCA) was inhibited. An important environmental implication is that carbonaceous materials not only sequester contaminants, but also allow contaminants to be slowly degraded in situ
陈卫峰、王昕喆、李尧
环境污染、环境污染防治环境科学技术现状化学工业经济有机化学工业
环境化学活性炭1,122-四氯乙烷脱氯氢
environmental chemistryactivated carbon1122-tetrachloroethanedehydrochlorination
陈卫峰,王昕喆,李尧.活性炭吸附1,1,2,2-四氯乙烷的脱氯氢反应:碳基材料在土壤/沉积物修复中的应用[EB/OL].(2016-07-11)[2025-06-25].http://www.paper.edu.cn/releasepaper/content/201607-132.点此复制
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