Enhanced photocatalytic ozonation of organic pollutants using an iron-based metal-organic framework 机翻标题: 暂无翻译,请尝试点击翻译按钮。

来源
Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications
年/卷/期
2019 / 251 /
页码
66-75
ISSN号
0926-3373
作者单位
Zhejiang Sci Tech Univ, Minist Educ, Engn Res Ctr Ecodyeing & Finishing Text, Hangzhou 310018, Zhejiang, Peoples R China;Zhejiang Sci Tech Univ, Minist Educ, Engn Res Ctr Ecodyeing & Finishing Text, Hangzhou 310018, Zhejiang, Peoples R China;Zhejiang Sci Tech Univ, Minist Educ, Engn Res Ctr Ecodyeing & Finishing Text, Hangzhou 310018, Zhejiang, Peoples R China;Georgia Inst Technol, Sch Civil & Environm Engn, Brook Byers Inst Sustainable Syst, Atlanta, GA 30332 USA;
作者
Yu, Deyou;Li, Lubiao;Wu, Minghua;Crittenden, John C.;
摘要
The photocatalytic activity of metal-organic frameworks (MOFs) is drawing great attention in the field of environmental remediation. However, the efficiency of MOFs still remains low because of the rapid recombination of valence band holes and conduction band electrons (a.k.a., charge carriers). The combination of photocatalysis and electron acceptors such as ozone are believed to be an efficient strategy to reduce the charge carrier recombination. Herein, we report that photocatalytic ozonation (PCO) using an Fe-based MOF (MIL-88A(Fe)) has greater destruction than photocatalysis and/or catalytic ozonation in terms of 4-nitrophenol (4-NP) degradation and mineralization. It is worth noting that our Fe-based MOF has a large number of Lewis acid sites (LAS). The pseudo-first order kinetic rate constants (k) of 4-NP degradation using PCO, photocatalysis and catalytic ozonation systems are 0.1632, 0.0143 and 0.0840 min(-1), respectively. The TOC removal of 4-NP in the PCO system is approximately 75.4% ([4-NP] = 100 ppm, ozone input dosage = 1.5 mg/min-L, UV light intensity = 3.46 x 10(-6) Einstiens/L-s, treatment time = 30 min) and this is much greater than those of photocatalysis (17.6%) and catalytic ozonation (38.7%). Most importantly, both the k value and TOC removal in the PCO system are much higher than the sum of those in other two processes, implying a strong synergistic effect in the PCO process. Mechanistic studies were conducted using electrochemical impedance spectroscopy (EIS) and photoluminescence (PL) measurements and demonstrate that the synergistic effect may originate from the enhanced photoinduced carrier separation using ozone as an electron acceptor. Furthermore, (OH)-O-center dot, O-center dot(2)-, and O-1(2) are found to be the principal reactive oxygen species (ROS) for 4-NP degradation and mineralization. Integrating the analysis of band structure, EPR and scavenging experiment results, ozone is not only able to reduce charge carrier recombination but also can be catalytically decomposed to generate more ROS on the LAS of MIL-88A(Fe). This study provides deep insights into the use of MOFs as effective advanced oxidation processes (AOPs).
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关键词/主题词
Photocatalytic ozonation;Lewis acid sites;Metal-organic frameworks;Synergistic effect;Reactive oxygen species;
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