Confining manganese-based peroxymonosulfate activation in carbon nanotube membrane for phenol degradation: Combined effect of oxygen vacancy defects and nanoconfinement

被引:21
作者
Ma, Huanran [1 ]
Zhang, Xiao [1 ]
Xu, Xiaohan [1 ]
Feng, Guoqing [1 ]
Pan, Zonglin [1 ]
Xu, Ruisong [2 ]
Wang, Pengcheng [3 ]
Yu, Yingtao [1 ]
Wang, Guanlong [4 ]
Fan, Xinfei [1 ]
Song, Chengwen [1 ]
机构
[1] Dalian Maritime Univ, Coll Environm Sci & Engn, 1 Linghai Rd, Dalian 116026, Peoples R China
[2] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, 2 Linggong Rd, Dalian 116024, Peoples R China
[3] Univ Houston, Dept Mech Engn, Houston, TX 77204 USA
[4] Dalian Polytech Univ, Sch Light Ind & Chem Engn, Dalian 116034, Peoples R China
基金
中国国家自然科学基金;
关键词
Carbon nanotube membrane; Nano-confined manganese catalyst; Oxygen vacancy defects; Peroxymonosulfate activation; Phenol degradation; CATALYTIC-OXIDATION; ORGANIC POLLUTANTS; POROUS CARBON; CHLOROPHENOLS; CONFINEMENT; RADICALS; REMOVAL; MNO2;
D O I
10.1016/j.cej.2023.144323
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, an open ends carbon nanotube (OCNT) membrane, which confined fine-tuned oxygen vacancy defects (Odef) modified MnOx inside OCNT (MnOx-in-OCNT), was developed for enhancing peroxymonosulfate (PMS) activation towards phenol (PE) removal. The MnOx-in-OCNT membrane filtration coupled with PMS activation process (MFPA process) achieved outstanding removal (100%) of PE at a high permeate flux of 585.0 L m2 h-1 bar � 1 (residence time of only 8.8 s). The unit degradation rate (2 min running time) and mass transfer rate of MnOx-in-OCNT were 2.0 and 8.4 times higher than that of CCNT (closed caps CNT) membrane with surface-loaded MnOx (MnOx-out-CCNT) MFPA process, and its catalytic performance was much superior to MnOx-in-OCNT powder reactions and MnOx-in-OCNT membrane batch reactions. The PMS activation mechanism experienced an obvious enhancement yield of reactive oxygen species (ROS) from MnOx-out-CCNT to MnOx-inOCNT MFPA process. The enhanced PMS activation and boosted ROS yield of MnOx-in-OCNT was mainly attributed to the co-effect of the fine-tuned Odef and nanoconfinement. The contact frequency between PMS, pollutant and Odef was greatly enhanced via nanoconfinement effect, leading to the enhanced yield of SO4 & BULL;� and & BULL;OH. Meanwhile, the O2 was enriched and reacts with enhanced Odef under nanoconfined-space to produce O2 & BULL;� and 1O2. Then, the co-enhanced ROS (SO4 & BULL;� , & BULL;OH, 1O2 and O2 & BULL;� ) displayed wide applicability for phenolic pollutants removal owing to their presence of -OH. Finally, the possible degradation pathway of PE was deduced by DFT calculations and HPLC analysis.
引用
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页数:13
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