In:
Journal of Materials Chemistry A, Royal Society of Chemistry (RSC), Vol. 9, No. 46 ( 2021), p. 26019-26027
Abstract:
Electroreduction of O 2 into H 2 O 2 holds great promise to replace the energy-intensive anthraquinone process that is currently used as an industry standard, but its practical feasibility still requires materials with high catalytic efficiencies. It is now shown that a Co-tetramethoxyphenylporphyrin–carbon nanotube (CoTMPP/CNT) nanohybrid acts as a high-performance catalyst with fast electron delivery to active sites toward electrochemically generating H 2 O 2 under acidic aqueous conditions, achieving a H 2 O 2 selectivity of over 95% and achieving strong stability. More impressively, it reduces O 2 to H 2 O 2 with an unprecedented mass activity of 9694 A g −1 and a high turnover frequency of up to 6.95 s −1 (0.6 V RHE ), representing the most active molecule-based two-electron O 2 reduction reaction (ORR) electrocatalyst under an acidic environment so far. It also performs efficiently in neutral media. Taking advantage of the well-defined structure of the TMPP unit, we systematically study the trends in catalytic activity as well as selectivity toward the ORR at the M–N 4 site (M = Mn, Fe, Co, Ni, Cu) with an identical chemical environment of TMPP. In situ attenuated total reflection infrared spectroscopy and density functional theory calculations were used to reveal further the catalytic mechanism.
Type of Medium:
Online Resource
ISSN:
2050-7488
,
2050-7496
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2021
detail.hit.zdb_id:
2702232-8
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