Guo Pucan, Tang Lin, Tang Jing, Zeng Guangming, Huang Binbin, Dong Haoran, Zhang Yi, Zhou Yaoyu, Deng Yaocheng, Ma Linlin, Tan Shiru
College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, PR China.
College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, PR China.
J Colloid Interface Sci. 2016 May 1;469:78-85. doi: 10.1016/j.jcis.2016.01.063. Epub 2016 Jan 28.
A highly efficient method for removal of p-nitrophenol and its conversion p-aminophenol from water was proposed using a novel catalyst-adsorbent composite of gold nanoparticles supported on functionalized mesoporous carbon (Au@CMK-3-O). The immobilized gold nanoparticles presented excellent catalytic ability to converse p-nitrophenol into p-aminophenol with the help of sodium borohydride, and the oxidized mesoporous carbon (CMK-3-O) serving as both carrier and adsorbent also exhibited high efficiency to remove p-aminophenol. The morphology and structure of the composite were characterized via SEM, TEM, FTIR and XPS analysis. Moreover, the mechanism of reaction process and the parameters of kinetics and thermodynamics were investigated. The activation energy was figured as 86.8 kJ mol(-1) for the adsorption and reduction of p-nitrophenol to p-aminophenol. The thermodynamic analysis based on the rate constants evaluated by pseudo-first-order model reveals that the adsorption-reduction process is an endothermic procedure with the rise of randomness. The anti-oxidation and regeneration study indicates that Au@CMK-3-O can be reused for 6 times with more than 90% conversion efficiency and keep high activity after exposing in air for 1 month, which possesses great prospects in application of nitroaromatic pollutant removal.
提出了一种高效的从水中去除对硝基苯酚并将其转化为对氨基酚的方法,该方法使用了一种新型的负载在功能化介孔碳上的金纳米颗粒催化剂-吸附剂复合材料(Au@CMK-3-O)。固定化的金纳米颗粒在硼氢化钠的帮助下表现出优异的催化能力,可将对硝基苯酚转化为对氨基酚,而作为载体和吸附剂的氧化介孔碳(CMK-3-O)也表现出高效去除对氨基酚的能力。通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、傅里叶变换红外光谱(FTIR)和X射线光电子能谱(XPS)分析对复合材料的形态和结构进行了表征。此外,还研究了反应过程的机理以及动力学和热力学参数。对硝基苯酚吸附还原为对氨基酚的活化能为86.8 kJ mol(-1)。基于伪一级模型评估的速率常数进行的热力学分析表明,吸附-还原过程是一个吸热过程,且随机性增加。抗氧化和再生研究表明,Au@CMK-3-O可以重复使用6次,转化效率超过90%,在空气中暴露1个月后仍保持高活性,在硝基芳烃污染物去除应用中具有广阔前景。