Herein, we developed a partially controlled pyrolysis strategy to create evenly distributed NiO nanoparticles within NiFe-MOF nanosheets (MOF NSs) for electrochemical synthesis of H2 O2 by a two-electron oxygen reduction reaction (ORR). The elemental Ni can be partially transformed to NiO and uniformly distributed on the surface of the MOF NSs, which is crucial for the formation of the particular structure. The optimized MOF NSs-300 exhibits the highest activity for ORR with near-zero overpotential and excellent H2 O2 selectivity (ca. 99 %) in 0.1 m KOH solution. A high-yield H2 O2 production rate of 6.5 mol gcat -1 h-1 has also been achieved by MOF NSs-300 in 0.1 m KOH and at 0.6 V (vs. RHE). In contrast to completely pyrolyzed products, the enhanced catalytic activities of partially pyrolyzed MOF NSs-300 originates mainly from the retained MOF structure and the newly generated NiO nanoparticles, forming the coordinatively unsaturated Ni atoms and tuning the performance towards electrochemical H2 O2 synthesis.
Keywords: electrocatalysis; hydrogen peroxide; metal-organic frameworks; oxygen reduction reaction; pyrolysis.
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