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基于胺基结合化学的功能化氧化石墨烯/藻酸盐杂化物的工程设计,用于同时高效去除痕量重金属:迈向饮用水处理

Engineering of amine-based binding chemistry on functionalized graphene oxide/alginate hybrids for simultaneous and efficient removal of trace heavy metals: Towards drinking water.

作者信息

Majdoub Mohammed, Amedlous Abdallah, Anfar Zakaria, Jada Amane, El Alem Noureddine

机构信息

Laboratory of Materials, Catalysis & Valorization of Natural Resources, Hassan II University, Casablanca 20000, Morocco.

Laboratory of Materials & Environment, Ibn Zohr University, Agadir 80000, Morocco; Institute of Materials Science of Mulhouse, Haute Alsace University, Mulhouse 68100, France; Strasbourg University, Strasbourg 67081, France.

出版信息

J Colloid Interface Sci. 2021 May;589:511-524. doi: 10.1016/j.jcis.2021.01.029. Epub 2021 Jan 16.

DOI:10.1016/j.jcis.2021.01.029
PMID:33486286
Abstract

Engineering of versatile binding chemistry on graphene oxide surface using nucleophilic substitution/amidation reactions for highly efficient adsorption of Cd (II), Cu (II) and Pb (II) is herein proposed. Graphene oxide (GO) was used as a precursor for covalent bonding of hexamethylenediamine (HMDA) molecules via the nucleophilic substitution/amidation reactions on epoxy (COC) and carboxyl (COOH) groups to yield hexamethylenediamine functionalized graphene oxide (GO-HMDA) with multiple binding chemistries such as oxygen and nitrogen. Afterwards, GO-HMDA was encapsulated in alginate hydrogel beads with different loadings 5, 10, 15 and 20 wt% to produce Alg/GO-HMDA hybrid adsorbents for the removal of trace heavy metal ions from aqueous solution. Batch adsorption studies showed remarkable adsorption rates reaching 100% for Pb (II), 98.18% for Cu (II) and 95.19 for Cd (II) (~1 mg L) with only 15 wt% of GO-HMDA incorporated into the alginate beads. Moreover, Alg/GO-HMDA showed high removal efficiencies of heavy metals from tap water with a removal order of (Pb > Cu > Cd) similar to that observed in single aqueous solution. In Addition, the Alg/GO-HMDA adsorbents displayed excellent regeneration ability for six consecutive adsorption-desorption cycles confirming the high performance and potential of these adsorbents, for real heavy metals remediation in environment and in drinking waters in both single and multiple systems. Finally, the adsorption mechanism of traces heavy metals resulted from several phenomena including the electrostatic interactions occurring between the COOH groups of Alginate and the GO-HMDA surface groups as well as, through chelation interactions occurring between the metal cations and amino-functionalized groups of Alg/GO-HMDA 15 hybrid adsorbent.

摘要

本文提出了一种利用亲核取代/酰胺化反应在氧化石墨烯表面构建多功能结合化学,以高效吸附镉(II)、铜(II)和铅(II)的方法。氧化石墨烯(GO)被用作前体,通过环氧基(COC)和羧基(COOH)上的亲核取代/酰胺化反应,与六亚甲基二胺(HMDA)分子进行共价键合,从而得到具有氧和氮等多种结合化学的六亚甲基二胺功能化氧化石墨烯(GO-HMDA)。之后,将GO-HMDA以5、10、15和20 wt%的不同负载量封装在海藻酸盐水凝胶珠中,制备出Alg/GO-HMDA杂化吸附剂,用于从水溶液中去除痕量重金属离子。批量吸附研究表明,仅将15 wt%的GO-HMDA掺入海藻酸盐珠中时,对铅(II)的吸附率可达100%,对铜(II)为98.18%,对镉(II)为95.19%(~1 mg/L)。此外,Alg/GO-HMDA对自来水中重金属的去除效率很高,去除顺序为(铅>铜>镉),与在单一水溶液中观察到的顺序相似。此外,Alg/GO-HMDA吸附剂在连续六个吸附-解吸循环中表现出优异的再生能力,证实了这些吸附剂在单一和多个系统中对环境和饮用水中实际重金属修复的高性能和潜力。最后,痕量重金属的吸附机制源于多种现象,包括海藻酸盐的COOH基团与GO-HMDA表面基团之间发生的静电相互作用,以及金属阳离子与Alg/GO-HMDA 15杂化吸附剂的氨基官能团之间发生的螯合相互作用。

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