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制备聚丙烯腈/离子共价有机骨架杂化纳米纤维以有效去除水中的六价铬。

Production of polyacrylonitrile/ionic covalent organic framework hybrid nanofibers for effective removal of chromium(VI) from water.

机构信息

Department of Civil Engineering, The University of Memphis, Memphis, TN 38018, USA.

Department of Civil Engineering, The University of Memphis, Memphis, TN 38018, USA.

出版信息

J Hazard Mater. 2022 Apr 5;427:128167. doi: 10.1016/j.jhazmat.2021.128167. Epub 2021 Dec 29.

Abstract

Hexavalent Cr(VI) found in industrial wastewater is a proven carcinogen which causes serious health issues in humans around the world. This study presents a novel method to enhance the Cr(VI) oxyanion removal from wastewater by polyacrylonitrile (PAN) nanofibers through incorporation of a guanidinium-based ionic covalent organic framework (BT-DG) in the nanofibers structure. Simple electrospinning technique was employed to produce PAN nanofibers and BT-DG was synthesized through condensation between benzene-1,3,5-tricarbaldehyde and N,N'-diaminoguanidine monohydrochloride. In-situ polymerization of BT-DG onto PAN nanofibers resulted in generation of hybrid PAN-BT-DG nanofibers. This modified PAN-BT-DG was characterized by obtaining its point of zero charge (PZC), differential scanning calorimeter (DSC), scanning electron microscopy (SEM) morphology and surface elements and oxidation states by X-ray photoelectron spectroscopy (XPS). PAN-BT-DG exhibited positive surface charge below pH 4, making it an outstanding adsorbent, for Cr(VI) removal. Cr(VI) adsorption onto PAN-BT-DG followed pseudo second order kinetics and adsorption data fitted well to Freundlich isotherm model. Highest Cr(VI) removal was obtained at 55 ℃ with a maximum Langmuir adsorption capacity of 173 mg/g at pH 3. Kinetic studies revealed that Cr(VI) adsorption onto PAN-BT-DG is endothermic and thermodynamically feasible. Desorption studies were conducted on PAN-BT-DG using 1 M NaOH as the stripping solvent and PAN-BT-DG exhibited excellent regeneration after five consecutive cycles.

摘要

六价铬(Cr(VI))存在于工业废水中,已被证实是一种致癌物质,会对全球人类健康造成严重问题。本研究提出了一种通过在纳米纤维结构中加入胍基离子共价有机框架(BT-DG)来增强聚丙腈(PAN)纳米纤维从废水中去除 Cr(VI)的新型方法。采用简单的静电纺丝技术制备 PAN 纳米纤维,并通过苯-1,3,5-三甲酰基和 N,N'-二氨基胍单盐酸盐之间的缩合反应合成 BT-DG。BT-DG 原位聚合到 PAN 纳米纤维上,生成混合的 PAN-BT-DG 纳米纤维。通过获得其等电点(PZC)、差示扫描量热法(DSC)、扫描电子显微镜(SEM)形态和表面元素及氧化态的 X 射线光电子能谱(XPS)对改性后的 PAN-BT-DG 进行了表征。PAN-BT-DG 在 pH 值低于 4 时表现出正表面电荷,使其成为一种出色的 Cr(VI)去除吸附剂。Cr(VI)吸附到 PAN-BT-DG 遵循伪二级动力学,吸附数据很好地符合 Freundlich 等温模型。在 pH 值为 3 时,Cr(VI)的去除率最高,最大 Langmuir 吸附容量为 173 mg/g,温度为 55°C。动力学研究表明,Cr(VI)吸附到 PAN-BT-DG 是吸热的,热力学上是可行的。使用 1 M NaOH 作为解吸溶剂对 PAN-BT-DG 进行了脱附研究,PAN-BT-DG 在连续五个循环后表现出优异的再生性能。

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