In-Plane Carbon Lattice-Defect Regulating Electrochemical Oxygen Reduction to Hydrogen Peroxide Production over Nitrogen-Doped Graphene

Abstract

Carbon-based materials are considered to be active for electrochemical oxygen reduction reaction (ORR) to hydrogen peroxide (H2O2) production. Nevertheless, less attention is paid to the investigation of the influence of in-plane carbon lattice defect on the catalytic activity and selectivity toward ORR. In the present work, graphene precursors were prepared from oxo-functionalized graphene (oxo-G) and graphene oxide (GO) with H2O2 hydrothermal treatment, respectively. Statistical Raman spectroscopy (SRS) analysis demonstrated the increased in-plane carbon lattice defect density in the order of oxo-G, oxo-G/H2O2, GO, GO/H2O2. Furthermore, nitrogen-doped graphene materials were prepared through ammonium hydroxide hydrothermal treatment of those graphene precursors. Rotating ring-disk electrode (RRDE) results indicate that the nitrogen-doped graphene derived from oxo-G with lowest in-plane carbon lattice defects exhibited the highest H2O2 selectivity of >82% in 0.1 M KOH. Moreover, a high H2O2 production rate of 224.8 mmol gcatalyst –1 h–1 could be achieved at 0.2 VRHE in H-cell with faradaic efficiency of >43.6%. Our work provides insights for the design and synthesis of carbon-based electrocatalysts for H2O2 production.

Engineering Facets and Oxygen Vacancies over Hematite Single Crystal for Intensified Electrocatalytic H2O2 Production

“…The catalyst exhibited 454, 378, and 302 mmol g −1 cat h −1 average H 2 O 2 production rates under potentials of 0.1, 0.3, and 0.5 V versus RHE, respectively. Among previously reported noble‐metal‐based [ 13,14,43 ] and carbon‐based [ 21,22,25 ] electrocatalysts, {001}‐Fe 2 O 3– x achieved the highest H 2 O 2 production rate. The room‐temperature H 2 O 2 decomposition test confirmed that {001}‐Fe 2 O 3– x is inactive in the decomposition of H 2 O 2 (Figure S33, Supporting Information).…”

A comparative perspective of electrochemical and photochemical approaches for catalytic H2O2 production

“…100 Nevertheless, most of the reported nitrogen-doped carbon materials led to the four-electron ORR to H 2 O, and only a few samples were reported to exhibit high selectivity toward H 2 O 2 production. 63,97,[101][102][103][104] For example, Anderson's group investigated the ORR performance of nitrogen-doped Ketjenblack for H 2 O 2 production from both experimental and theoretical calculation viewpoints. 105 Experimental results demonstrated that the nitrogen-doped Ketjenblack showed a lower onset potential and mainly followed the two-electron ORR process for H 2 O 2 production.…”

Recent Progress on Carbonaceous Material Engineering for Electrochemical Hydrogen Peroxide Generation

“…2f). The important role of defects for two-electron ORR was also investigated and demonstrated in other carbon materials [26][27][28][29].…”