Insight into the difference in activation of peroxymonosulfate with nitrogen-doped and non-doped carbon catalysts to degrade bisphenol A. Issue 4 (August 2021)

• Record Type: Journal Article
• Authors: Chen, Chen; Jiang, Caiyun; Cao, Wang; Zhou, Haifei; Wang, Yuping
• Is Part Of: Journal of environmental chemical engineering. Volume 9:Issue 4(2021)
• Publication Date: 2021-08
• Subjects: Graphitized carbon -- Peroxymonosulfate -- Surface chemistry -- Electron transfer -- Singlet oxygen -- Synergy; Chemical engineering -- Environmental aspects -- Periodicals; Environmental engineering -- Periodicals; Chemical engineering -- Environmental aspects; Environmental engineering; Periodicals; 660.0286
• DOI: 10.1016/j.jece.2021.105492
• Languages: English
• ISSNs: 2213-2929

Abstract

Abstract: Heteroatom-modified carbon-based catalysts (especially nitrogen-doped) have been reported to be effective in activating peroxymonosulfate (PMS). Nevertheless, here our study found that graphitized carbon nanomaterial (GC800) exhibited a similar catalytic capacity as the nitrogen-doped graphitized carbon nanomaterial (NGC800) in the degradation of bisphenol A (BPA) via activating PMS, however, the degradation rate constant of the former was approximately 1.72-times greater than that of the latter. Meanwhile, GC800 showed admirable versatility, wide application range of pH value and excellent stability. Furthermore, the connection between the difference in surface chemistry (surface functional groups, electronic properties) and reaction rate between GC800 and NGC800 was discussed. Quenching experiments combined with electron paramagnetic resonance (EPR) and electrochemical measurements revealed the existence of a multi-pathway synergy in GC800/PMS system dominated by the non-radical electron-transfer pathway and complemented by radical (O2 − )/non-radical ( 1 O2 ) pathway. The high proportion of carbonyl groups and sp 2 -hybridized carbon as the main parameters affected the electron density of GC800 in the process of non-radical electron transfer. In contrast, NGC800/PMS system only followed the non-radical oxidation pathway with singlet oxygen being the predominant ROS. Pyrrolic N affected the non-radical oxidation pathway of NGC800. This work verifies the significant role of surface chemistry of carbon materials and the synergy between non-radical electron transfer and radical/non-radical oxidation on the catalytic velocity. And it presents a novel thought in the design of high-efficiency carbon-based catalysts toward green and sustainable ecological restoration. Graphical Abstract: Take catalytic activity of catalysts as the object of study, the mechanism differences and determining factors of GC800/PMS/BPA system and NGC800/PMS/BPA system were investigated. ga1 Highlights: ● N-doped and non-doped graphitized catalysts were prepared by thermal annealing. ● GC800 shows much higher rate constant than NGC800 in activating PMS to degrade BPA. ● Surface chemistry of GC800 and NGC800 are key factor affecting catalytic velocity. ● Activation of PMS on GC800 mainly relied on the synergy of multi-reaction pathway. ● Activation of PMS on NGC800 followed non-radical pathway mainly producing 1 O2 .