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Prussian blue analogues derived porous nitrogen-doped carbon microspheres as high-performance metal-free peroxymonosulfate activators for non-radical-dominated degradation of organic pollutants

Abstract

Nitrogen-doped carbon materials are becoming a new type of metal-free heterogeneous catalysts in advanced oxidation processes (AOPs) for wastewater treatment and environmental remediation. In this study, porous nitrogen-doped carbon (PNC) microspheres derived from Zn-Co Prussian blue analogues (Zn-Co PBAs) are employed as heterogeneous catalysts in peroxymonosulfate (PMS) activation. The unique configuration of metal centers/clusters bounded by cyanide groups (−C≡N) of Zn-Co PBAs offers PNC microspheres abundant porosity, high graphitization degree, and rich nitrogen substitution, which are in favor of the improvement of catalytic performance. PNC-800 (pyrolyzed at 800 °C) exhibits better performance than other common carbon materials and homologous nitrogen-doped carbocatalysts derived from ZIF-8/ZIF-67. Based on the radical quenching and trapping experiments, a non-radical pathway is proposed to dominate methylene blue (MB) degradation; and high graphitization degree and rich surface graphitic N sites of PNC-800 are two key factors to induce the non-radical pathway. Some influential factors, including catalyst dosage, PMS concentration, pH value, and reaction temperature are investigated in details. Notably, MB degradation over PNC-800 is almost insusceptible to those common ions and nature organic matters, and maintains its catalytic efficiency under some actual water background conditions. More interestingly, this non-radical pathway and good catalytic performance of PNC-800/PMS system are universal in the degradation of other typical organic pollutants. We believe that PNC microspheres may be a promising green heterogeneous catalyst for the degradation of organic pollutants, and this study can be used for the design of high performance carbocatalysts in non-radical systems in the future.

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Publication details

The article was received on 25 Sep 2017, accepted on 14 Nov 2017 and first published on 14 Nov 2017


Article type: Paper
DOI: 10.1039/C7TA08472B
Citation: J. Mater. Chem. A, 2017, Accepted Manuscript
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    Prussian blue analogues derived porous nitrogen-doped carbon microspheres as high-performance metal-free peroxymonosulfate activators for non-radical-dominated degradation of organic pollutants

    N. Wang, W. Ma, Z. Ren, Y. Du, P. Xu and X. Han, J. Mater. Chem. A, 2017, Accepted Manuscript , DOI: 10.1039/C7TA08472B

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