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采用响应面法优化的铈基金属有机框架材料Ce-MOF-808负载双金属纳米颗粒实现对硝基苯酚的可持续还原

Sustainable nitrophenol reduction using Ce-mof-808-supported bimetallic nanoparticles optimized by response surface methodology.

作者信息

Hassan Hassan M A, Alruwaili Hala A, Alhumaimess Mosaed S, Alanazi Ahmed Hamad, El-Aassar M R, Alshammari Mutairah S, Hussein Modather F, Alsohaimi Ibrahim Hotan

机构信息

Chemistry Department, College of Science, Jouf University, P.O. Box 2014, Sakaka, Saudi Arabia.

Chemistry Department, College of Science, Jouf University, P.O. Box 2014, Sakaka, Saudi Arabia.

出版信息

Environ Res. 2025 Jan 1;264(Pt 1):120340. doi: 10.1016/j.envres.2024.120340. Epub 2024 Nov 9.

Abstract

This study presents the development and optimization of Ce-MOF-808 nanocrystals supported by metallic and bimetallic nanoparticles (Au, Ag, and Pd) for the efficient reduction of nitrophenol. Using a sol-immobilization method, we synthesized a series of catalysts, including Au/Ce-MOF-808, Au-Ag/Ce-MOF-808, and Au-Pd/Ce-MOF-808, and evaluated their catalytic efficacy of 4-nitrophenol (4-NP) reduction using NaBH₄ under mild conditions. Initially, effects of time (1-18 min), and catalyst dose (1-6 mg) on the reduction of nitrophenol were investigated through the one-factor-at-a-time experiment. Furthermore, the optimized experimental conditions (reduction time of 18 min, and catalyst dose 4.5 mg) were obtained using response surface methodology (RSM). X-ray photoelectron spectroscopy (XPS) and thermogravimetric assessment (TGA) further confirmed the robust interaction between metal nanoparticles and the Ce-MOF-808 framework, contributing to enhanced thermal stability and electron transfer capabilities. Among these, the Au-Ag/Ce-MOF-808 composite exhibited the highest catalytic activity, achieving a 98.3% conversion of 4-NP to 4-aminophenol (4-AP) within 18 min. Kinetic studies confirmed the superior catalytic performance of Au-Ag/Ce-MOF-808, with a rate constant (k) of 0.100 min⁻ and a reduced half-life of 9.6 min, highlighting the synergistic effects of Au and Ag nanoparticles in enhancing electron transfer and increasing active sites. The reusability tests demonstrated that Au-Ag/Ce-MOF-808 maintained high catalytic activity over five consecutive cycles, indicating its stability and suitability for continuous use. These findings underscore the potential of metal-modified Ce-MOF-808 catalysts for sustainable environmental applications, offering high efficiency, durability, and the ability to operate under mild conditions.

摘要

本研究介绍了负载金属和双金属纳米颗粒(金、银和钯)的Ce-MOF-808纳米晶体的开发与优化,用于高效还原硝基苯酚。采用溶胶固定法,我们合成了一系列催化剂,包括Au/Ce-MOF-808、Au-Ag/Ce-MOF-808和Au-Pd/Ce-MOF-808,并在温和条件下使用硼氢化钠评估了它们对4-硝基苯酚(4-NP)还原的催化效果。最初,通过单因素实验研究了时间(1-18分钟)和催化剂用量(1-6毫克)对硝基苯酚还原的影响。此外,使用响应面方法(RSM)获得了优化的实验条件(还原时间18分钟,催化剂用量4.5毫克)。X射线光电子能谱(XPS)和热重分析(TGA)进一步证实了金属纳米颗粒与Ce-MOF-808框架之间的强相互作用,有助于提高热稳定性和电子转移能力。其中,Au-Ag/Ce-MOF-808复合材料表现出最高的催化活性,在18分钟内实现了4-NP向4-氨基苯酚(4-AP)的98.3%转化。动力学研究证实了Au-Ag/Ce-MOF-808的优异催化性能,速率常数(k)为0.100 min⁻¹,半衰期缩短至9.6分钟,突出了金和银纳米颗粒在增强电子转移和增加活性位点方面的协同作用。可重复使用性测试表明,Au-Ag/Ce-MOF-808在连续五个循环中保持了高催化活性,表明其稳定性和连续使用的适用性。这些发现强调了金属改性Ce-MOF-808催化剂在可持续环境应用中的潜力,具有高效、耐用以及在温和条件下运行的能力。

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