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一种具有氧化还原活性的共价有机框架,可有效检测和去除水合肼。

A redox-active covalent organic framework for the efficient detection and removal of hydrazine.

机构信息

Key Laboratory of Photochemical Biomaterials and Energy Storage Materials, Heilongjiang Province and College of Chemistry and Chemical Engineering, Harbin Normal University, Harbin 150025, PR China.

Department of Chemistry and Chemical Engineering, Hebei Normal University for Nationalities, Chengde 067000, PR China.

出版信息

J Hazard Mater. 2020 Jan 5;381:120983. doi: 10.1016/j.jhazmat.2019.120983. Epub 2019 Aug 10.

Abstract

The removal and detection of soluble hydrazine is of importance due to its harm to soil and subterranean water, but challenging. Herein, we preferentially disposed a porous and redox active covalent-organic framework (DAAQ-TFP COF, denoted as DQ-COF) to simultaneously removal and detect hydrazine. Electroactive sites (anthraquinone units) can be intelligently incorporated into the channel walls/pores of COF. DQ-COF has high crystallinity and good thermal stability, and DQ-COF dropped onto nickel matrix (DQ-COF/Ni composite) still retains high surface area, characterized by PXRD, FT-IR, nitrogen adsorption and TGA. Subsequently, a detailed study of DQ-COF towards hydrazine uptake and detection potentials is explored. DQ-COF as adsorbent unfolds strong removal ability towards hydrazine, the maximum removal capacity of which is up to 1108 mg g, following Friedrich and pseudo-second-order kinetic models. Meanwhile, the DQ-COF supported on nickel renders attractive electrochemical properties, which is efficiently responsive to hydrazine at a part per billion (ppb) level, coupled with a wide linear range (0.5 ˜ 1223 μM), low detection limit (0.07 μM) and high anti-interference ability. There is no other COFs with such a favorable capability in synchronous removal and selective detection towards hydrazine, probably applying in superintending water quality and disposing wastewater.

摘要

由于其对土壤和地下水的危害,去除和检测可溶性肼非常重要,但具有挑战性。在此,我们优先选择一种多孔且氧化还原活性的共价有机框架(DAAQ-TFP COF,记为 DQ-COF)来同时去除和检测肼。电化学活性位点(蒽醌单元)可以智能地整合到 COF 的通道壁/孔中。DQ-COF 具有高结晶度和良好的热稳定性,并且 DQ-COF 负载在镍基体上(DQ-COF/Ni 复合材料)仍然保留高表面积,其通过 PXRD、FT-IR、氮气吸附和 TGA 进行表征。随后,详细研究了 DQ-COF 对肼的吸收和检测潜力。作为吸附剂的 DQ-COF 对肼具有很强的去除能力,最大去除容量高达 1108 mg g,遵循 Friedrich 和拟二级动力学模型。同时,负载在镍上的 DQ-COF 呈现出吸引人的电化学性能,能够在十亿分之一(ppb)的水平上对肼做出高效响应,同时具有宽线性范围(0.5 ˜ 1223 μM)、低检测限(0.07 μM)和高抗干扰能力。在同步去除和选择性检测肼方面,没有其他 COFs 具有如此有利的能力,可能适用于监督水质和处理废水。

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