Title

N-Doped graphene from metal-organic frameworks for catalytic oxidation of p-Hydroxylbenzoic acid: N-Functionality and mechanism

Document Type

Journal Article

Publisher

ACS Publications

School

School of Engineering

RAS ID

24673

Comments

Liang, P., Zhang, C., Duan, X., Sun, H., Liu, S., Tade, M. O., & Wang, S. (2017). N-Doped Graphene from Metal–Organic Frameworks for Catalytic Oxidation of p-Hydroxylbenzoic Acid: N-Functionality and Mechanism. ACS Sustainable Chemistry & Engineering, 5(3), 2693-2701. Available here

Abstract

N-doped graphene has been considered as a promising catalyst with surface metal-free active sites for environmental remediation. Several MIL-100 (Fe)-templated N-doped graphene samples were synthesized using dicyandiamide, melamine, and urea as the nitrogen precursors. Excellent catalytic oxidation of p-hydroxylbenzoic acid (PHBA) was observed on the as-synthesized samples via peroxymonosulfate (PMS) activation. The mechanism was investigated by both electron paramagnetic resonance (EPR, 5,5-dimethyl-1-pyrroline N-oxide and 2,2,6,6-tetramethyl-4-piperidinol as the trapping agents) and quenching tests (ethanol and sodium azide as the radical scavengers). Benzoic acid and furfuryl alcohol were also employed as probing reagents for hydroxyl/sulfate radicals and singlet oxygen, respectively. The results confirmed that singlet oxygen was generated and dominated the PHBA degradation on N-doped graphene, rather than hydroxyl/sulfate radicals. With the novel N-doped graphene, this study illustrates the formation mechanism of nitrogen functionalities for reactive radicals via PMS activation for removal of organic contaminants in water.

DOI

10.1021/acssuschemeng.6b03035

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