A Homogeneously Catalyzed Paired Electrolytic Cell for Hydrogen Peroxide Production

用于生产过氧化氢的均相催化双电解池

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Abstract

The two-electron water oxidation reaction (2e(-)-WOR) and oxygen reduction reaction (2e(-)-ORR) represent sustainable and promising processes for the electrochemical synthesis of hydrogen peroxide (H(2)O(2)). The main factor hampering the realization of a paired electrochemical cell for H(2)O(2) production is finding appropriate catalysts for both 2e(-)-ORR and 2e(-)-WOR, able to work under the same experimental conditions. Herein we show that Cu(tmpa)) and Sn-TMPyP are compatible and efficient catalysts for 2e(-)-ORR and 2e(-)-WOR, respectively. They have been used to assemble a paired electrochemical cell for H(2)O(2) production. The latter exhibits a total overpotential of 570 mV, distributed between the two electrodes. During a 3 h bulk electrolysis experiment, the cathodic Faradaic efficiency ranged from 15% to 19% with a H(2)O(2) production rate of 1.6 µmol h(-) (1) cm(-) (2). Meanwhile, at the anode, the Faradaic efficiency stabilized between 40% and 50%, yielding a H(2)O(2) production rate of 3.5 µmol h(-) (1) cm(-) (2). The remarkable activity of Sn-TMPyP as a catalyst for the 2e(-)-WOR, ranking among the highest reported for molecular catalysts, is ascribed to the selection of a carbonate buffer as the electrolyte, which enhanced catalytic performance by facilitating dissociation of H(2)O(2) from the Sn catalyst. This work establishes a new benchmark for homogeneous dual-electrode H(2)O(2) electrosynthesis.

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