A COOH-terminated nitrogen-doped carbon aerogel as a bulk electrode for completely selective two-electron oxygen reduction to H₂O₂

Abstract

A COOH-terminated nitrogen-doped carbon aerogel exhibited 100% selectivity to two-electron oxygen reduction, exceeding reported carbonaceous and noble metal catalysts.

Recent Progress on Carbonaceous Material Engineering for Electrochemical Hydrogen Peroxide Generation

“…Similar to N-doped carbon catalysts that activated π electrons and induced charge redistribution, fluorine [22,48], multiple elements [23,25], doped carbon, and metal-nonmetal co-doped carbon [24,49] also exhibited excellent performance for two-electron ORR. Zhao et al [22] discussed fluorine-doped HPC for two-electron reduction.…”

“…As determined by DFT calculations, the interface between h-BN domains and graphene exhibited unique catalytic behavior that can preferentially drive the production of H 2 O 2 [23]. Considering the promising activity and selectivity of oxygen functional groups and the nitrogen-doping modification in decreasing the overpotential, Zhao et al [25] examined the synergistic effect of nitrogen dopants and -COOH groups on carbonaceous materials. Through theoretical calculations, the researchers found that the theoretical overpotential for two-electron ORR would be lower when the two groups combined in one carbon.…”

“…Through theoretical calculations, the researchers found that the theoretical overpotential for two-electron ORR would be lower when the two groups combined in one carbon. To amplify the synergistic effect, they also designed metal-free carbon aerogel integrated with nitrogen dopants and surface -COOH groups for H 2 O 2 production, which exhibited complete 100% selectivity to H 2 O 2 with high yields and stability [25]. Furthermore, Cardoso et al [50] discussed the performance varieties before and after electrochemically stabilized measurements on the N and O group-modified graphene and graphene oxide nanoribbons.…”

“…an optimized adsorption/desorption energy to the reaction intermediate (*OOH). Thus, numerous strategies, including defect design [13,17] and heteroatom doping [12,[18][19][20][21][22][23][24][25], have been adopted to optimize the electronic structure to improve the activity and selectivity of carbon materials (Fig. 1).…”

Metal-free carbocatalysis for electrochemical oxygen reduction reaction: Activity origin and mechanism

“…The underlying interpretation on such an abnormal phenomenon still remains a puzzle. A recent research deduced that the nitrogen doping effect on promoting the four-electron ORR can be screened by the termination of −COOH group [94] . Instead, the COOH-modified N-doped carbon exhibits a high reactivity toward two-electron ORR in alkali to produce peroxide with nearly 100% selectivity.…”