Junyan Kuang, Qishi Si, Wanqian Guo, Fang Ma
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology
HaiJuan Guo
School of Environment, Liaoning University
Abstract
Large-scale production of high-valent iron-oxo species (Fe(V)=O) for the efficient removal of organic pollutants has been a challenge due to the high activation energy barrier of the Fe (III)-oxidant complex. Here, we propose a novel heterogeneous system using Fe (III)-doped g-C3N4 with three-coordinate nitrogen vacancies (FNCN) as a catalyst for the activation of peracetic acid (PAA). Our investigations and calculations indicate that Fe (III) is the primary active site, and illustrate a nonradical mechanism of two-electron transfer mechanism to produce Fe (V)=O species. Meanwhile, the abundant nitrogen vacancies (Nvs) strengthen the electron distribution of the Fe (III) sites to promote reactivity, and reduce the energy barrier to break the O− O bond of PAA in the Fe (III)− PAA complex, to achieve the rapid accumulation of Fe(V)=O species. As a result, this heterogeneous system has excellent selectivity and anti-interference in removal of pollutants. Our work offers a unique viewpoint to strengthen a nonradical pathway in PAA activation.
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87-Nitrogen vacancies regulated the local electron density of iron sites in g C3N4 to boost the generation of high valent iron oxo species in a peracetic acid based Fenton like process.pdf
