Li Huanxuan, Xu Shaodan, Du Jia, Tang Junhong, Zhou Qingwei
Hangzhou Dianzi University, College Materials & Environmental Engineering Hangzhou 310018 Zhejiang PR China
The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, South China University of Technology, Guangzhou Higher Education Mega Center Guangzhou 510006 PR China.
RSC Adv. 2019 Mar 25;9(17):9410-9420. doi: 10.1039/c9ra01143a. eCollection 2019 Mar 22.
In this study, for the first time, we describe the single step synthesis of a Cu particle-doped cobalt-based metal-organic framework (Cu@Co-MOF) using a hydrothermal method. The as-prepared materials were characterized by powder X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy-energy disperse spectroscopy, thermogravimetry, and X-ray photoelectron spectroscopy, which confirmed the incorporation of zero-valent copper on the surface of the Co-MOFs. The heterogeneous catalytic activity of Cu@Co-MOFs was tested to activate peroxymonosulfate (PMS) for the removal of methylene blue (MB). The ratio of (Cu)/(Co) in the Cu@Co-MOFs showed a strong impact on the catalytic activity of the Cu@Co-MOFs, whereas a (Cu)/(Co) of 1 : 1 exhibited the best catalytic performance and obtained 100% MB removal within 30 min. The effects of initial pH, reaction temperature, PMS concentration, and catalyst dosages were investigated in this study. The stability and reusability of the Cu@Co-MOFs were also investigated. The results showed a low decline in the MB removal with the increase in cycle numbers, whereas 100% MB was removed by prolonging the reaction time. Heterogeneous reactions taking place in the pores and surface of the Cu@Co-MOFs played an important role in the generation of the sulfate radicals (SO˙) and hydroxyl radicals (·OH) that were the primary reactive species responsible for MB degradation.
在本研究中,我们首次描述了采用水热法一步合成铜颗粒掺杂的钴基金属有机框架(Cu@Co-MOF)。通过粉末X射线衍射、傅里叶变换红外光谱、扫描电子显微镜-能谱、热重分析和X射线光电子能谱对所制备的材料进行了表征,证实了零价铜掺入到了Co-MOFs的表面。测试了Cu@Co-MOFs的非均相催化活性,以活化过一硫酸盐(PMS)来去除亚甲基蓝(MB)。Cu@Co-MOFs中(Cu)/(Co)的比例对其催化活性有很大影响,而(Cu)/(Co)为1:1时表现出最佳催化性能,在30分钟内可实现100%的MB去除率。本研究考察了初始pH值、反应温度、PMS浓度和催化剂用量的影响。还研究了Cu@Co-MOFs的稳定性和可重复使用性。结果表明,随着循环次数的增加,MB去除率下降幅度较小,而通过延长反应时间可实现100%的MB去除。在Cu@Co-MOFs的孔道和表面发生的非均相反应在生成硫酸根自由基(SO˙)和羟基自由基(·OH)中起重要作用,这些自由基是负责MB降解的主要活性物种。