Ye Jian, Dai Jiangdong, Wang Lulu, Li Chunxiang, Yan Yongsheng, Yang Guoyu
Institute of Green Chemistry and Chemical Technology, Advanced Chemical Engineering Laboratory of Green Materials and Energy of Jiangsu Province, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.
Department of Chemistry, Beijing Institute of Technology, Beijing 100081, China.
J Colloid Interface Sci. 2021 Mar 15;586:178-189. doi: 10.1016/j.jcis.2020.10.082. Epub 2020 Oct 26.
Currently, carbon-based catalysts integrated with macroporous catalytic membrane have aroused considerable attention for environmental remediation because of its practicability and high efficiency. Herein, nitrogen doped carbon nanotube hybrids (Fe-Co@NC-CNTs) decorated with multiple active species (FeCo/CoFeO@Fe/CoNC) were designed through N-molecule assisted pyrolysis of bimetallic (Fe/Co) metal-organic frameworks, and then immobilized on poly(vinylidene fluoride) (PVDF) membrane to construct macroporous Fe-Co@NC-CNTs/PVDF catalytic membrane via directional freezing technique, where active sites were efficiently exposed for oxidants and target pollutants. As expected, Fe-Co@NC-CNTs/PVDF membrane successfully achieved almost 100% bisphenol A (BPA) degradation after 40 min via PMS activation, which was significantly overperformed the majority of conventional carbon-based catalysts. Besides, we found that Fe-Co@NC-CNTs/PVDF membrane not only exhibited ideal catalytic and self-cleaning property in humic acid (HA)-BPA coexistence system, but also maintained the excellent reusability and ultrahigh water flux (10464.45 L m h) even after 5 cycles. Notably, in EPR analysis and quenching experiments, it was found that sulfate radicals (SO· and ·OH) and singlet oxygen (O) participated the degradation process while O made a major contribution. More significantly, this study is very meaningful for the development of novel catalytic self-cleaning membranes with PMS activation.
目前,集成有大孔催化膜的碳基催化剂因其实用性和高效性在环境修复方面引起了广泛关注。在此,通过双金属(Fe/Co)金属有机框架的N分子辅助热解设计了装饰有多种活性物种(FeCo/CoFeO@Fe/CoNC)的氮掺杂碳纳米管杂化物(Fe-Co@NC-CNTs),然后将其固定在聚偏二氟乙烯(PVDF)膜上,通过定向冷冻技术构建大孔Fe-Co@NC-CNTs/PVDF催化膜,其中活性位点有效地暴露于氧化剂和目标污染物。正如预期的那样,Fe-Co@NC-CNTs/PVDF膜通过PMS活化在40分钟后成功实现了几乎100%的双酚A(BPA)降解,这明显优于大多数传统的碳基催化剂。此外,我们发现Fe-Co@NC-CNTs/PVDF膜不仅在腐殖酸(HA)-BPA共存体系中表现出理想的催化和自清洁性能,而且即使在5个循环后仍保持优异的可重复使用性和超高水通量(10464.45 L m h)。值得注意的是,在EPR分析和猝灭实验中,发现硫酸根自由基(SO·和·OH)和单线态氧(O)参与了降解过程,而O起到了主要作用。更重要的是,这项研究对于开发具有PMS活化的新型催化自清洁膜具有重要意义。