Efficient electro-catalyzed PMS activation on a Fe-ZIF-8 based BTNAs/Ti anode: An in-depth investigation on anodic catalytic behavior

被引:15
|
作者
Mo, Fan [1 ]
Zhou, Qixing [1 ]
Hou, Zelin [1 ]
Wang, Shuting [1 ]
Wang, Qi [1 ]
Kang, Weilu [1 ]
机构
[1] Nankai Univ, Coll Environm Sci & Engn, Key Lab Pollut Proc & Environm Criteria, Tianjin Key Lab Environm Remediat & Pollut Control, Tianjin 300350, Peoples R China
基金
中国国家自然科学基金;
关键词
Macroscopic MOFs anode; Strong interfacial coordination; Preferential electron capture; D-band center; Dark photocatalysis; DEGRADATION; PEROXYMONOSULFATE; POLLUTANTS; WATER; UIO-66-NH2; ADSORPTION; SINGLE; SYSTEM; TIO2;
D O I
10.1016/j.envint.2022.107548
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Phenanthrene (PHE), mainly released from coal tar and petroleum distillation, is an important kind of prevalent polycyclic aromatic hydrocarbons (PAHs) contamination in China (up to 2.38 +/- 0.02 mg/kg in soil and 8668 ng/L in surface water) and other countries in the world. Metal-organic frameworks (MOFs) show promising application prospects in the decontamination field, however, suffering from the intrinsic fragility and fine powder forms. Therefore, macroscopic MOFs architecture-sandwich-like Fe-ZIF-8/blue TiO2 nanotube arrays (BTNAs)/Ti substrate (FBTT) anode with strong interfacial bonding (Fe-O-Ti and Fe-2-MIM-Ti coordination) was constructed using innovative in situ growth, condensation-crystallization-deposition, and pyrolysis methods, aiming at exploring the feasibility of MOFs-based anode/peroxymonosulfate (PMS) mediated PHE elimination, revealing the in-depth mechanisms, simultaneously overcoming the intrinsic drawbacks of MOFs. The FBTT-4 (doping content of 30 %) efficiently degraded PHE by 90.01 % and 74.5 % within 10 min at 350 mu g/L and 3 mg/L, respectively, mediated by the center dot OH compared to the SO4 center dot-, O-1(2), and O-2(center dot-). Post-optimized range of anodic potential enabled (i) anodic oxidation, (ii) activation of water and PMS molecules to produce active species, (iii) capture of electrons in reactants to reduce Fe3+/Ti4+ to Fe2+/Ti3+, maintaining the proportion of Fe/Ti with low valence and thus stable PMS activation capacity, and (iv) regulation of the Fe/Ti d-band center to modulate the anode adsorption capacity. The further increment in anodic potential could promote "dark photocatalysis" with a Z-scheme-like mechanism. Thus, it is proposed that the development of macroscopic MOFs-based anode, especially those with small band gaps, represents vast potentials in electrocatalytic contamination elimination. Simultaneously, the MOFs-based anode is expected to fully exploit their catalytic capacities and solve their intrinsic defects as well.
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页数:17
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