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胺功能化还原氧化石墨烯负载的银纳米粒子用于有机污染物的高效催化还原。

Amine-functionalized reduced graphene oxide-supported silver nanoparticles for superior catalytic reduction of organic pollutants.

机构信息

Department of Chemistry, Kannur University, Kannur, Kerala, 670 327, India.

出版信息

Environ Sci Pollut Res Int. 2023 Sep;30(42):96114-96124. doi: 10.1007/s11356-023-29115-2. Epub 2023 Aug 11.

DOI:10.1007/s11356-023-29115-2
PMID:37566329
Abstract

In this work, a simple and environmentally friendly approach has been followed to synthesize amine-functionalized reduced graphene oxide (RGO)-supported silver nanoparticle (AgNPs) having superior catalytic efficiency towards the reduction of organic pollutants. RGO/AgNPs nanohybrid was synthesized by a one-pot hydrothermal reduction of silver nitrate in the presence of amino-propyl trimethoxy silane (APTMS)-functionalized graphene oxide (GO) nanosheets. The structural and morphological characterization of as-synthesized RGO/AgNPs nanohybrid was done by using XRD, SEM, TEM, FT-IR, and Raman spectroscopy techniques. APTMS plays an important role in controlling the size of anchored AgNPs on the nanohybrid in the present study. The -NH groups on the surface of APTMS-modified GO function as effective and well-organized nucleation centers facilitating uniform growth of discrete and smaller-sized spherical AgNPs on the surface of RGO nanosheets. In the absence of APTMS, the nanohybrid comprised of bigger-sized AgNPs with few hundred of nanometers in dimension. The catalytic efficiency of RGO/AgNPs nanohybrid was evaluated for the reduction of two model organic pollutants: 4-nitrophenol (4-NP) and methylene blue (MB). Due to the synergistic effects of RGO, APTMS, and Ag components, RGO/AgNPs nanohybrid developed in the present study exhibited superior catalytic activity towards the reduction of 4-NP and MB in comparison with previously reported graphene/graphene oxide/reduced graphene oxide-supported AgNPs catalysts. The catalytic reduction of 4-NP and MB followed pseudo-unimolecular kinetics and the rate constants were found to be 18.83 × 10 s and 131.5 ×10 s respectively for 4-NP and MB. Furthermore, RGO/AgNPs nanohybrid showed admirable recyclability with negligible loss in its activity until five recycle runs. The superior catalytic activity, favorable kinetic parameters, and sustained catalytic efficiency after recycling make RGO/AgNPs nanohybrid a promising catalyst for the reduction of organic pollutants in environmental remediation.

摘要

在这项工作中,我们采用了一种简单且环保的方法合成了胺功能化还原氧化石墨烯(RGO)负载的银纳米粒子(AgNPs),该纳米粒子在催化还原有机污染物方面具有卓越的效率。RGO/AgNPs 纳米杂化物是通过在氨基丙基三甲氧基硅烷(APTMS)功能化的氧化石墨烯(GO)纳米片存在下,一锅水热还原硝酸银合成的。通过 XRD、SEM、TEM、FT-IR 和拉曼光谱技术对合成的 RGO/AgNPs 纳米杂化物进行了结构和形态表征。在本研究中,APTMS 发挥了重要作用,控制了锚定在纳米杂化物上的 AgNPs 的尺寸。APTMS 修饰的 GO 表面上的-NH 基团作为有效的、组织良好的成核中心,有利于离散的、较小尺寸的球形 AgNPs 在 RGO 纳米片表面上均匀生长。在没有 APTMS 的情况下,纳米杂化物由尺寸为几百纳米的较大尺寸的 AgNPs 组成。评估了 RGO/AgNPs 纳米杂化物对两种模型有机污染物:4-硝基苯酚(4-NP)和亚甲基蓝(MB)的还原效率。由于 RGO、APTMS 和 Ag 成分的协同作用,与之前报道的石墨烯/氧化石墨烯/还原氧化石墨烯负载 AgNPs 催化剂相比,本研究中制备的 RGO/AgNPs 纳米杂化物对 4-NP 和 MB 的还原表现出优异的催化活性。4-NP 和 MB 的催化还原遵循准单分子动力学,4-NP 和 MB 的速率常数分别为 18.83×10 s 和 131.5×10 s。此外,RGO/AgNPs 纳米杂化物具有令人钦佩的可回收性,其活性在五次循环运行中几乎没有损失。优异的催化活性、有利的动力学参数和回收后的持续催化效率使 RGO/AgNPs 纳米杂化物成为环境修复中还原有机污染物的有前途的催化剂。

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