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PEO‐b‐PS Block Copolymer Templated Mesoporous Carbons: A Comparative Study of Nitrogen and Sulfur Doping in the Oxygen Reduction Reaction to Hydrogen Peroxide
Author(s) -
Perazzolo Valentina,
Daniel Giorgia,
Brandiele Riccardo,
Picelli Luca,
Rizzi Gian Andrea,
Isse Abdirisak Ahmed,
Durante Christian
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202003355
Subject(s) - inorganic chemistry , catalysis , mesoporous material , heteroatom , carbon fibers , chemistry , electrolysis , sulfur , electrocatalyst , electrochemistry , materials science , organic chemistry , electrode , ring (chemistry) , composite number , electrolyte , composite material
Carbon materials slightly doped with heteroatoms such as nitrogen (N‐RFC) or sulfur (S‐RFC) are investigated as active catalysts for the electrochemical bielectronic oxygen reduction reaction (ORR) to H 2 O 2 . Mesoporous carbons with wide, accessible pores were prepared by pyrolysis of a resorcinol‐formaldehyde resin using a PEO‐b‐PS block copolymer as a sacrificial templating agent and the nitrogen and sulfur doping were accomplished in a second thermal treatment employing 1,10‐phenanthroline and dibenzothiophene as nitrogen and sulfur precursors, respectively. The synthetic strategy allowed to obtain carbon materials with very high surface area and mesopore volume without any further physicochemical post treatment. Voltammetric rotating ring‐disk measurements in combination with potentiostatic and galvanostatic bulk electrolysis measurements in 0.5 m H 2 SO 4 demonstrated a pronounced effect of heteroatom doping and mesopores volume on the catalytic activity and selectivity for H 2 O 2 . N‐RFC electrode was employed as electrode material in a 45 h electrolysis showing a constant H 2 O 2 production of 298 mmol g −1 h −1 (millimoles of H 2 O 2 divided by mass of catalyst and electrolysis time), with a faradic efficiency (FE) up to 61 % and without any clear evidence of degradation. The undoped carbon RFC showed a lower production rate (218 mmol g −1 h −1 ) but a higher FE of 76 %, while the performances drastically dropped when S‐RFC (production rate 11 mmol g −1 h −1 and FE=39 %) was used.