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壳聚糖修饰的两亲性碳点衍生生物炭对水中蒽的吸附去除

Adsorptive removal of anthracene from water by biochar derived amphiphilic carbon dots decorated with chitosan.

作者信息

Hashemzadeh Farzad, Khoshmardan Maede Esmaeili, Sanaei Daryoush, Ghalhari Mohammad Rezvani, Sharifan Hamidreza, Inglezakis Vassilis J, Arcibar-Orozco Javier A, Shaikh Wasim Akram, Khan Eakalak, Biswas Jayanta Kumar

机构信息

Water and Wastewater Research Center, Water Research Institute, Tehran, Iran.

Department of Environmental Health Engineering, Faculty of Public Health and Safety, Shahid Beheshti University of Medical Science, Tehran, Iran.

出版信息

Chemosphere. 2024 Mar;352:141248. doi: 10.1016/j.chemosphere.2024.141248. Epub 2024 Jan 25.

Abstract

Anthracene belongs to the polycyclic aromatic hydrocarbon (PAH) consisting of benzene rings, unusually highly stable through more π-electrons and localized π-bond in entire rings. Aqueous-phase anthracene adsorption using carbon-based materials such as biochar is ineffective. In this paper, carbon dots (CDs) derived from the acid treatment of coconut shell biochar (CDs/MCSB) decorated with chitosan (CS) are successfully synthesized and applied for anthracene removal from aqueous solutions. The h-CDs/MCSB exhibited fast adsorption of anthracene with significant sorption capacity (Q = 49.26 mg g) with 95 % removal efficiency at 60 min. The study suggested chemisorption dominated monolayer anthracene adsorption onto h-CDs/MCSB, where a significant role was played by ion-exchange. Density Functional Theory (DFT) suggested the anthracene adsorption was dominated by the electrostatic interactions and delocalized electron, induced by higher polarizability of functional groups on the surface of hybrid CDs/MCSB assisted by chitosan (h-CDs/MCSB). In addition, the aromatic structure of CDs/MCSB and high polarizability of functional groups provided the strong interactions between benzene rings of anthracene and hybrid adsorbent-assisted multiple π-bond through delocalized π-bond and polarization-induced H-bond interactions. The presence of carboxylic and sulfonic groups on the CDs/MCSB surface also contributed to the effective adsorption of anthracene was confirmed by the fluorescence spectra. The results showed that the hybrid adsorbent was an effective material for removing PAHs, usually difficult to remove from water owing to the presence of benzene rings in their structures. Further, consistency in the DFT results suggested the outstanding binding capacity with the anthracene molecules with h-CDs/MCSB.

摘要

蒽属于由苯环组成的多环芳烃(PAH),通过更多的π电子和整个环中的局部π键异常稳定。使用生物炭等碳基材料对水相中的蒽进行吸附是无效的。本文成功合成了用壳聚糖(CS)修饰的、由椰子壳生物炭酸处理得到的碳点(CDs),即CDs/MCSB,并将其用于从水溶液中去除蒽。h-CDs/MCSB对蒽表现出快速吸附,具有显著的吸附容量(Q = 49.26 mg/g),在60分钟时去除效率达95%。研究表明,化学吸附主导了蒽在h-CDs/MCSB上的单层吸附,其中离子交换起了重要作用。密度泛函理论(DFT)表明,蒽的吸附主要由静电相互作用和离域电子主导,这是由壳聚糖辅助的杂化CDs/MCSB(h-CDs/MCSB)表面官能团的较高极化率所诱导的。此外,CDs/MCSB的芳香结构和官能团的高极化率通过离域π键和极化诱导的氢键相互作用,使得蒽的苯环与杂化吸附剂之间产生了强相互作用。CDs/MCSB表面羧基和磺酸基的存在也有助于蒽的有效吸附,这一点通过荧光光谱得到了证实。结果表明,这种杂化吸附剂是一种有效去除PAHs的材料,PAHs由于其结构中存在苯环,通常很难从水中去除。此外,DFT结果的一致性表明h-CDs/MCSB与蒽分子具有出色的结合能力。

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