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Carboxylated Hexagonal Boron Nitride/Graphene Configuration for Electrosynthesis of High-Concentration Neutral
Zhixin Song1, Xiao Chi2, Shu Dong1
1State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 211816, China.
Abstract:
The electrosynthesis of hydrogen peroxide (H2 O2 ) via two-electron (2e- ) oxygen (O2 ) reduction reaction (ORR) has great potential to replace the traditional energy-intensive anthraquinone process, but the design of low-cost and highly active and selective catalysts is greatly challenging for the long-term H2 O2 production under industrial relevant current density, especially under neutral electrolytes. To address this issue, this work constructed a carboxylated hexagonal boron nitride/graphene (h-BN/G) heterojunction on the commercial activated carbon through the coupling of B, N co-doping with surface oxygen groups functionalization. The champion catalyst exhibited a high 2e- ORR selectivity (>95 %), production rate (up to 13.4 mol g-1 h-1 ), and Faradaic efficiency (FE, >95 %). The long-term H2 O2 production under the high current density of 100 mA cm-2 caused the cumulative concentration as high as 2.1 wt %. The combination of in situ Raman spectra and theoretical calculation indicated that the carboxylated h-BN/G configuration promotes the adsorption of O2 and the stabilization of the key intermediates, allowing a low energy barrier for the rate-determining step of HOOH* release from the active site and thus improving the 2e- ORR performance. The fast dye degradation by using this electrochemical synthesized H2 O2 further illustrated the promising practical application.
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