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共价三嗪基框架:一种从水溶液中去除全氟烷基酸的有前景的吸附剂。

Covalent triazine-based framework: A promising adsorbent for removal of perfluoroalkyl acids from aqueous solution.

作者信息

Wang Bingyu, Lee Linda S, Wei Chenhui, Fu Heyun, Zheng Shourong, Xu Zhaoyi, Zhu Dongqiang

机构信息

State Key Laboratory of Pollution Control and Resource Reuse/School of the Environment, Nanjing University, Jiangsu, 210046, China.

Department of Agronomy, Purdue University, West Lafayette, IN, 47907, USA.

出版信息

Environ Pollut. 2016 Sep;216:884-892. doi: 10.1016/j.envpol.2016.06.062. Epub 2016 Jul 4.

Abstract

Perfluoroalkyl acids (PFAAs) are highly stable, persistent, and ubiquitous in the environment with significant concerns growing with regards to both human and ecosystem health. Due to the high stability to both biological and chemical attack, the only currently feasible approach for their removal from water is adsorbent technology. The main objective of this study was to assess a covalent triazine-based framework (CTF) adsorbent for removal from aqueous solutions of perfluoro C4, C6, and C8 carboxylates and sulfonates including the two C8s most commonly monitored, perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS). Adsorption affinity and capacity were quantified and compared to three commonly used sorbents: pulverized microporous activated carbon, single-walled carbon nanotubes, and Amberlite IRA-400 anion-exchange resin. CTF adsorbent exhibited pronouncedly higher adsorption affinity and capacity of PFAAs than other test sorbents. The remarkably strong adsorption to CTF can be attributed to the favored electrostatic interaction between the protonated triazine groups on the inner wall of the hydrophobic CTF pore and the negatively charged head groups of the PFAAs intercalated between the CTF layers. The homogeneous, nanosized pores (1.2 nm) of CTF hindered adsorption of a large-sized dissolved humic acid, thus minimizing the suppression of PFAA adsorption. Additionally, regeneration of CTF was easily accomplished by simply raising pH > 11, which inhibited the electrostatic adsorptive interaction of PFAAs.

摘要

全氟烷基酸(PFAA)在环境中高度稳定、持久且普遍存在,人们对其对人类健康和生态系统健康的影响越来越担忧。由于对生物和化学攻击具有高稳定性,目前从水中去除它们的唯一可行方法是吸附剂技术。本研究的主要目的是评估一种基于共价三嗪的框架(CTF)吸附剂从水溶液中去除全氟C4、C6和C8羧酸盐及磺酸盐的能力,包括两种最常监测的C8化合物,全氟辛酸(PFOA)和全氟辛烷磺酸(PFOS)。对吸附亲和力和容量进行了量化,并与三种常用吸附剂进行了比较:粉碎的微孔活性炭、单壁碳纳米管和Amberlite IRA - 400阴离子交换树脂。CTF吸附剂对PFAA的吸附亲和力和容量明显高于其他测试吸附剂。对CTF的超强吸附可归因于疏水CTF孔内壁上质子化的三嗪基团与插层在CTF层之间的PFAA带负电荷的头基之间有利的静电相互作用。CTF均匀的纳米尺寸孔(1.2纳米)阻碍了大尺寸溶解腐殖酸的吸附,从而将对PFAA吸附的抑制降至最低。此外,只需将pH值提高到>11即可轻松实现CTF的再生,这抑制了PFAA的静电吸附相互作用。

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