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基于负载在交联乙烯基聚合物上的银纳米颗粒制备一种用于还原硝基苯酚的高效多相催化剂。

Establishing a productive heterogeneous catalyst based on silver nanoparticles supported on a crosslinked vinyl polymer for the reduction of nitrophenol.

作者信息

Aggour Y A, Kenawy El-Refaie, Magdy Marwa, Elbayoumy Elsayed

机构信息

Chemistry Department, Faculty of Science, Damietta University New Damietta 34517 Egypt

Polymer Research Group, Chemistry Department, Faculty of Science, Tanta University Tanta 31527 Egypt

出版信息

RSC Adv. 2024 Sep 23;14(41):30127-30139. doi: 10.1039/d4ra05186f. eCollection 2024 Sep 18.

Abstract

The treatment of toxic nitrophenols in industrial wastewater is urgently needed from environmental, health, and economic points of view. The current study addresses the synthesis of the crosslinked vinyl polymer poly(acrylonitrile--2-acrylamido-2-methylpropane sulfonic acid) (poly(AN--AMPS)) through free radical copolymerization techniques using acrylonitrile (AN) and 2-acrylamido-2-methylpropane sulfonic acid (AMPS) monomers with different ratios and potassium persulfate (KPS) as an initiator in an aqueous medium. The prepared copolymer was utilized as a supporting matrix for silver nanoparticles (AgNPs) the chemical reduction of silver nitrate within the copolymer framework. Different techniques were employed to characterize the prepared poly(AN--AMPS) and Ag/poly(AN--AMPS) composites, such as Fourier transform infrared (FTIR) spectroscopy, thermal gravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscopy (TEM), and Brunauer-Emmett-Teller (BET) analysis. The results exhibit that silver metal was excellently dispersed across the surface of poly(AN--AMPS) without any agglomeration, presenting as nanocrystals with an average particle size equal to 6.21 nm. Also, BET analysis confirmed that the Ag/poly(AN--AMPS) composite exhibits mesoporous characteristics with a surface area of 59.615 m g. Moreover, the Ag/poly(AN--AMPS) composite was effectively applied as a heterogeneous catalyst for the catalytic reduction of hazardous 4-nitrophenols (4-NP) with a rate constant equal to 0.28 min and half-life time equal to 2.47 min to a less toxic compound in the presence of NaBH as a reductant. Furthermore, the reusability experiment confirmed the excellent stability of Ag/poly(AN--AMPS). The catalyst can be easily separated from the reaction mixture using a simple centrifuge and directly reused for up to four successive cycles without a remarkable decrease in its catalytic activity. The conversion percentage of 4-NP after the four cycles was found to be 93%.

摘要

从环境、健康和经济角度来看,工业废水中有毒硝基酚的处理迫在眉睫。当前研究通过自由基共聚技术,以不同比例的丙烯腈(AN)和2-丙烯酰胺基-2-甲基丙烷磺酸(AMPS)单体以及过硫酸钾(KPS)作为引发剂,在水介质中合成了交联乙烯基聚合物聚(丙烯腈-2-丙烯酰胺基-2-甲基丙烷磺酸)(聚(AN-AMPS))。所制备的共聚物被用作银纳米颗粒(AgNPs)的支撑基质,通过在共聚物框架内化学还原硝酸银来制备。采用了不同技术对所制备的聚(AN-AMPS)和Ag/聚(AN-AMPS)复合材料进行表征,如傅里叶变换红外(FTIR)光谱、热重分析(TGA)、X射线衍射(XRD)、透射电子显微镜(TEM)和布鲁诺尔-埃米特-泰勒(BET)分析。结果表明,银金属在聚(AN-AMPS)表面均匀分散,无任何团聚现象,呈现为平均粒径等于6.21 nm的纳米晶体。此外,BET分析证实,Ag/聚(AN-AMPS)复合材料具有介孔特性,表面积为59.615 m²/g。而且,在NaBH作为还原剂的情况下,Ag/聚(AN-AMPS)复合材料被有效地用作多相催化剂,用于催化还原有害的4-硝基酚(4-NP),其速率常数等于0.28 min⁻¹,半衰期等于2.47 min,将其还原为毒性较小的化合物。此外,可重复使用性实验证实了Ag/聚(AN-AMPS)具有出色的稳定性。使用简单离心机即可轻松将催化剂从反应混合物中分离出来,并直接重复使用多达四个连续循环,而其催化活性无显著下降。四个循环后4-NP的转化率为93%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/eb54/11417678/05dc0b33e101/d4ra05186f-f1.jpg

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