An insight into metal organic framework derived N-doped graphene for the oxidative degradation of persistent contaminants: formation mechanism and generation of singlet oxygen from peroxymonosulfate

Author(s): Ping Liang ¹ ^, ² ^, ³ ^, ⁴ , Chi Zhang ¹ ^, ² ^, ³ ^, ⁴ , Xiaoguang Duan ¹ ^, ² ^, ³ ^, ⁴ , Hongqi Sun ⁵ ^, ⁶ ^, ⁷ ^, ⁴ , Shaomin Liu ¹ ^, ² ^, ³ ^, ⁴ , Moses O. Tade ¹ ^, ² ^, ³ ^, ⁴ , Shaobin Wang ¹ ^, ² ^, ³ ^, ⁴

Publication date (Electronic): 2017

Journal: Environmental Science: Nano

Publisher: Royal Society of Chemistry (RSC)

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Abstract

Singlet oxygen produced during peroxymonosulfate activation by N-graphene dominated the pollutants degradation.

Abstract

The synthesis of carbonaceous materials from a metal organic framework (MIL-100), organic linker and N-precursor was comprehensively investigated, and the structures of the products were characterized. It was found that simple pyrolysis of mixed MIL-100 (Fe)/dicyandiamide (DCDA) could produce nitrogen-doped graphene (N-graphene). The N-graphene showed excellent performances in peroxymonosulfate (PMS) activation, which were superior to those of counterparts of graphene, iron( ii, iii) oxide, manganese( iv) oxide and cobalt( ii, iii) oxide. With PMS activation, N-graphene exhibited efficient catalytic degradation of various organic pollutants such as phenol, 2,4,6-trichlorophenol (TCP), sulfachloropyridazine (SCP) and p-hydroxybenzoic acid (PHBA). Electron paramagnetic resonance (EPR) spectroscopy and radical quenching tests were employed to investigate the PMS activation and organic degradation processes. It was found that singlet oxygen ( ¹O ₂) was mainly produced during the activation of PMS by N-graphene, and contributed to the catalytic oxidation instead of sulfate and/or hydroxyl radicals. These findings provide new insights into PMS activation by metal-free carbon catalysis.

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High-performance electrocatalysts for oxygen reduction derived from polyaniline, iron, and cobalt.

Gang Wu, Karren More, Christina Johnston … (2011)

The prohibitive cost of platinum for catalyzing the cathodic oxygen reduction reaction (ORR) has hampered the widespread use of polymer electrolyte fuel cells. We describe a family of non-precious metal catalysts that approach the performance of platinum-based systems at a cost sustainable for high-power fuel cell applications, possibly including automotive power. The approach uses polyaniline as a precursor to a carbon-nitrogen template for high-temperature synthesis of catalysts incorporating iron and cobalt. The most active materials in the group catalyze the ORR at potentials within ~60 millivolts of that delivered by state-of-the-art carbon-supported platinum, combining their high activity with remarkable performance stability for non-precious metal catalysts (700 hours at a fuel cell voltage of 0.4 volts) as well as excellent four-electron selectivity (hydrogen peroxide yield <1.0%).