4.8 Article

Overlooked role of nitrogen dopant in carbon catalysts for peroxymonosulfate activation: Intrinsic defects or extrinsic defects?

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 295, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120291

关键词

Carbon catalyst; Topological defects; Peroxymonosulfate; Nitrogen doping

资金

  1. National Natural Science Foundation of China [51508451]
  2. Natural Science Foundation of Shaanxi Province of China [Z20180121]
  3. New Style Think Tank of Shaanxi Universities, and Technology Innovation Leading Program of Shaanxi [2020CGXNG021]

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The study uncovered the role of nitrogen dopant in carbon catalysts, where nitrogen is partially evaporated at high temperature to form topological intrinsic defects, promoting the activation of peroxymonosulfate and organic degradation through an electron-transfer mechanism. The findings suggest that surface-activated PMS complex is the main reactive oxidation species for organic degradation.
Nitrogen was usually doped into carbon matrix to boost its catalytic activity owing to its electronic adjusting activity toward the topological carbon structure. Herein, an overlooked role of nitrogen dopant was unraveled. The nitrogen dopant was firstly incorporated into the carbon matrix and then partially evaporated, leaving the newly generated topological intrinsic defects under high temperature. It was confirmed that peroxymonosulfate (PMS) could be activated by topological defects-rich carbon catalysts. Surface-activated PMS complex was found to be the dominant reactive oxidation species for organic degradation through electron-transfer mechanism. The distinct current density attenuation revealed that N-rich carbon catalysts possessed more effective stoichiometric reaction between the surface-activated PMS and adsorbed organic than topological defects-rich carbon. Findings from this work confirmed the roles of topological defects and extrinsic defects in PMS activation and provided new insight into the synthesis of defects-rich carbon catalysts.

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