Citation: Wang Xinhao, Pu Xueting, Yuan Yue, Xiang Yunjie, Zhang Yuling, Xiong Zhaokun, Yao Gang, Lai Bo. An old story with new insight into the structural transformation and radical production of micron-scale zero-valent iron on successive reactivities[J]. Chinese Chemical Letters, ;2020, 31(10): 2634-2640. doi: 10.1016/j.cclet.2020.08.007 shu

An old story with new insight into the structural transformation and radical production of micron-scale zero-valent iron on successive reactivities

Wang Xinhao ^a,b ,
Pu Xueting ^a,b ,
Yuan Yue ^c ,
Xiang Yunjie ^a,b ,
Zhang Yuling ^a,b ,
Xiong Zhaokun ^a,b,*, ,
Yao Gang ^b,d ,
Lai Bo ^a,b,*,

a.
State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China
b.
Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China
c.
National Engineering Laboratory for Clean Technology of Leather Manufacture, College of Biomass Science and Engineering, Sichuan University, Chengdu 610065, China
d.
Institute of Environmental Engineering, RWTH Aachen University, Aachen 52062, Germany

scuxzk@scu.edu.cn

laibo@scu.edu.cn

Received Date: 30 June 2020
Revised Date: 15 July 2020
Accepted Date: 5 August 2020
Available Online: 23 August 2020

Figures(5)

It is generally recognized that the formation and accumulation of iron oxides on the surface of zero-valent iron (Fe⁰) resulting in significant decrease of contaminant degradation rates during the long-term reactions. However, in this study, we found that the removal efficiencies of p-nitrophenol (PNP) by micro zero-valent iron (mFe⁰) could maintain at the satisfactory level in the process of continuous reactions (20 cycles). The removal rate constant (0.1779 min^-1) of the 5^th cycle was 6.74 times higher than that of the 1^st reaction (0.0264 min^-1), even the 20^th cycle (0.0371 min^-1) was higher than that of the 1^st reaction. Interestingly, almost no dissolved iron was detected in the solution, and the total iron concentrations decreased dramatically with the process of continuous reactions. The results of scanning electron microscope and energy dispersive spectrometry (SEM-EDS) and X-ray diffraction (XRD) revealed that the structure and composition of corrosion products change from amorphous to highly crystal with the increase of the number of cycles. The corrosion products were mainly magnetite (Fe₃O₄) and a small part of maghemite (γ-Fe₂O₃), which were in the form of microspheres on the surface of mFe⁰. The formation of surface oxidation shell hindered the release of Fe²⁺. X-ray photoelectron spectroscopy (XPS) results illustrated that partial Fe₃O₄ could be converted into γ-Fe₂O₃. Electrochemical analysis proved that the electron transfer rate of mFe⁰ increased with the formation of the oxides shell. However, the consumption of iron core and thicker oxide film weakened the electron transfer rate. Besides, the quenching experiments indicated that the reaction activity of mFe⁰ could be enhanced with the addition of scavengers. This study deepened the understanding of the structural transformation and radical production of mFe⁰ in continuous reactions.
- Zero-valent iron,
- Iron oxides,
- p-Nitrophenol,
- Structural transformation,
- Successive reactivities
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