通讯作者：Chen, S (reprint author), Dalian Univ Technol, Sch Environm Sci & Technol, Minist Educ, Key Lab Ind Ecol & Environm Engn, Dalian 116024, Peoples R China.
合写作者：Chen, Shuo,Zhang, Haiguang,Fan, Xinfei,Gao, Cong,Yu, Hongtao,Quan, Xie
发表刊物：FRONTIERS OF ENVIRONMENTAL SCIENCE & ENGINEERING
关键字：Heterogeneous Fenton-like catalysts; MIL-88B-Fe; CNTs; Organic pollutants; Mechanism
摘要：Iron-based metal organic frameworks have been verified to be efficient heterogeneous Fenton catalysts due to their open pore channels and highly uniform distribution of metallic centers. In these catalysts, however, the iron element is mainly in the form of Fe(III), which results in a process required to reduce Fe(III) to Fe(II) to initiate Fenton reaction. To address this problem, carbon nanotubes (CNTs) with electron-rich oxygen-functional groups on the surface were incorporated into the metal organic frameworks (MIL-88B-Fe) to improve Fe(II) content for an enhanced Fenton-like performance. The prepared CNT@MIL-88B-Fe (C@M) showed much stronger catalytic ability toward H2O2 than MIL-88B-Fe. The pseudo-first-order kinetic constant for phenol degradation by C@M (0.32 min(-1)) was about 7 times that of MIL-88B-Fe, and even higher than or comparable to the values of reported heterogeneous Fenton-like catalysts. Moreover, the Fenton-like system could effectively degrade various kinds of refractory organic pollutants and exhibited excellent catalytic activity over a wide pH range (4-9). XPS analysis confirmed that Fe(II) content of the catalyst gradually increased with CNT loadings. Electron spin resonance analysis showed that the signal intensity (center dot OH) of C@M was much higher than MIL-88B-Fe, which was consistent with the degradation efficiency of pollutants. Furthermore, the Fe(II) content of the catalyst gradually increased along with the oxygen-functional group content of CNTs. The result demonstrated that oxygen-containing functional groups of CNTs have a significant impact on the enhanced catalytic performance of C@M. This study provides a new insight to enhance Fenton reaction by using nanocarbon materials.