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Facile Synthesis of Natural Kaolin-Based CuO Catalyst: An Efficient Heterogeneous Catalyst for the Catalytic Reduction of 4-Nitrophenol

机译:天然高岭土基CuO催化剂的简单合成:一种催化还原4-硝基苯酚的高效非均相催化剂

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摘要

Water contamination by nitro compounds from various industrial processes has significantly contributed to environmental pollution and severely threatened aquatic ecosystems. Inexpensive, efficient, and environmentally benign catalysts are required for the catalytic reduction of such nitro compounds. This study reports the fabrication of various nanocomposites (NCs) of copper oxide nanoparticles (CuO NPs) supported on a kaolin sheet using straightforward and simple one-pot synthesis procedures that control the metal precursor to kaolin ratios. The selected as-synthesized CuO/kaolin NC was characterized using a range of advanced spectroscopic and microscopic methods, such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), ultraviolet–visible (UV–vis) spectroscopy, field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), high-angle annular dark-field scanning TEM (HAADF-STEM), and N2 adsorption/desorption analysis. The characterization results confirmed the successful incorporation of CuO NPs into the kaolin sheets, which had an average size of about 18.7 nm. The fabricated CuO/kaolin NC was used as a heterogeneous catalyst for the efficient reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) in the presence of sodium borohydride (NaBH4) in an aqueous system at room temperature. The catalyst demonstrated superior catalytic performance with high 4-NP conversion into 4-AP (>99%) in the aqueous phase (50 mL, 20 mg L–1) within 6 min. In addition, the reaction kinetics of 4-NP reduction was also investigated, and the reaction followed the pseudo-first-order kinetics equation with the apparent rate constant of 1.76 min–1. Furthermore, the Arrhenius and Eyring parameters for the catalytic hydrogenation reaction of 4-NP were calculated in order to investigate the catalytic reaction process in more detail. Moreover, the catalyst exhibited excellent reusability and stability over seven repeated catalytic test cycles without any noticeable decline in catalytic activity. Therefore, this paper could provide a novel, efficient, and environmentally promising clay-based non-noble metal oxide nanocatalyst to reduce nitro compounds in the aqueous system.
机译:各种工业过程中的硝基化合物对水的污染严重造成了环境污染,并严重威胁了水生生态系统。此类硝基化合物的催化还原需要廉价、高效且环保的催化剂。本研究报告了使用简单明了的一锅法合成程序制造了负载在高岭土片上的氧化铜纳米颗粒 (CuO NPs) 的各种纳米复合材料 (NC),这些程序控制金属前驱体与高岭土的比率。使用一系列先进的光谱和显微方法对所合成的 CuO/高岭土 NC 进行了表征,例如 X 射线衍射 (XRD)、傅里叶变换红外光谱 (FT-IR)、紫外-可见光 (UV-vis) 光谱、场发射扫描电子显微镜 (FE-SEM)、透射电子显微镜 (TEM)、能量色散 X 射线光谱 (EDX)、高角度环形暗场扫描 TEM (HAADF-STEM) 和 N2 吸附/解吸分析。表征结果证实了 CuO NPs 成功掺入高岭土片中,其平均尺寸约为 18.7 nm。制备的 CuO/高岭土 NC 用作非均相催化剂,在硼氢化钠 (NaBH4) 存在下,在室温下在水性体系中将 4-硝基苯酚 (4-NP) 高效还原为 4-氨基苯酚 (4-AP)。该催化剂表现出优异的催化性能,在 6 分钟内在水相 (50 mL, 20 mg L–1) 中将 4-NP 高转化率转化为 4-AP (>99%)。此外,还研究了 4-NP 还原的反应动力学,反应遵循准一级动力学方程,表观速率常数为 1.76 min–1。此外,计算了 4-NP 催化加氢反应的 Arrhenius 和 Eyring 参数,以便更详细地研究催化反应过程。此外,该催化剂在 7 次重复催化测试循环中表现出优异的可重用性和稳定性,催化活性没有明显下降。因此,本文可以提供一种新颖、高效且具有环保前景的粘土基非贵金属氧化物纳米催化剂,以还原水性体系中的硝基化合物。

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