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Hydrogen Peroxide Assisted Electrooxidation of Benzene to Phenol over Bifunctional Ni-(O-C2 )4 Sites
Shengbo Zhang1,2, Meng Jin1,2, Hui Xu1,2
1Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031, China.
Abstract:
Direct electrocatalytic oxidation of benzene has been regarded as a promising approach for achieving high-value phenol product, but remaining a huge challenge. Here an oxygen-coordinated nickel single-atom catalyst (Ni-O-C) is reported with bifunctional electrocatalytic activities toward the two-electron oxygen reduction reaction (2e- ORR) to H2 O2 and H2 O2 -assisted benzene oxidation to phenol. The Ni-(O-C2 )4 sites in Ni-O-C ar proven to be the catalytic active centers for bifunctional 2e- ORR and H2 O2 -assisted benzene oxidation processes. As a result, Ni-O-C can afford a benzene conversion as high as 96.4 ± 3.6% with a phenol selectivity of 100% and a Faradaic efficiency (FE) of 80.2 ± 3.2% with the help of H2 O2 in 0.1 m KOH electrolyte at 1.5 V (vs RHE). A proof of concept experiment with Ni-O-C concurrently as cathode and anode in a single electrochemical cell demonstrates a benzene conversion of 33.4 ± 2.2% with a phenol selectivity of 100% and a FE of 44.8 ± 3.0% at 10 mA cm-2 .
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