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聚乙烯亚胺接枝氮掺杂磁性生物炭对六价铬的高效去除:合成与吸附机理研究。

Polyethylenimine-grafted nitrogen-doping magnetic biochar for efficient Cr(VI) decontamination: Insights into synthesis and adsorption mechanisms.

机构信息

School of Resources and Environment, Northeast Agricultural University, Harbin, 150030, China.

School of Resources and Environment, Northeast Agricultural University, Harbin, 150030, China.

出版信息

Environ Pollut. 2022 Nov 15;313:120103. doi: 10.1016/j.envpol.2022.120103. Epub 2022 Sep 5.

Abstract

Herein, polyethylenimine (PEI)-grafted nitrogen (N)-doping magnetic biochar (PEI@MNBC) was synthesized, and characterization results showed that the microwave-assisted PEI grafting and ball milling-assisted N doping introduced abundant amino, pyridine N and pyrrole N structures onto biochar, which possessed high affinity to Cr(VI) in the anion form. The as-prepared PEI@MNBC displayed pH-dependence adsorption performance and high tolerance to co-existing ions with maximum uptake capacity of Cr(VI) identified as 183.02 mg/g. Furthermore, PEI@MNBC could bind Cr(VI) through electrostatic attraction, complexion, precipitation, reduction and pore filling. Especially, effective reduction of Cr(VI) was ascribed to cooperative electron transfer of partial oxygen-containing functional groups, intramolecular pyridine/pyrrole N, protonated amino and Fe on the adsorbent, while oxygen-containing and amino functional groups from N-doping biochar and PEI synergistically complexed Cr(III) via providing lone pair electrons to form coordinate bonds. Furthermore, the stable precipitation was formed between Fe and Cr(III). Additionally, the Cr(VI) elimination efficiency could maintain 95.83% even after four adsorption-desorption cycles, suggesting PEI@MNBC as a high-performance adsorbent for Cr(VI) contaminated water remediation.

摘要

本文合成了接枝聚乙烯亚胺(PEI)的氮(N)掺杂磁性生物炭(PEI@MNBC),表征结果表明,微波辅助接枝和球磨辅助掺杂在生物炭上引入了丰富的氨基、吡啶 N 和吡咯 N 结构,对阴离子形式的 Cr(VI)具有高亲和力。所制备的 PEI@MNBC 表现出 pH 依赖性吸附性能,对共存离子具有高耐受性,最大 Cr(VI)吸附容量为 183.02mg/g。此外,PEI@MNBC 可以通过静电吸引、络合、沉淀、还原和孔填充来结合 Cr(VI)。特别是,部分含氧官能团、分子内吡啶/吡咯 N、质子化氨基和吸附剂上的 Fe 的协同电子转移,有效还原了 Cr(VI),而 N 掺杂生物炭和 PEI 中的含氧和氨基官能团通过提供孤对电子形成配位键协同络合 Cr(III)。此外,Fe 和 Cr(III)之间形成了稳定的沉淀。此外,即使经过四次吸附-解吸循环,Cr(VI)的去除效率仍能保持 95.83%,表明 PEI@MNBC 是一种用于 Cr(VI)污染水修复的高性能吸附剂。

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