双功能 Ni-(O-C )位促进的双氧水辅助苯电化学氧化为苯酚。
Hydrogen Peroxide Assisted Electrooxidation of Benzene to Phenol over Bifunctional Ni-(O-C ) Sites.
机构信息
Key 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.
University of Science and Technology of China, Hefei, 230026, China.
出版信息
Adv Sci (Weinh). 2022 Dec;9(35):e2204043. doi: 10.1002/advs.202204043. Epub 2022 Oct 30.
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 H O and H O -assisted benzene oxidation to phenol. The Ni-(O-C ) sites in Ni-O-C ar proven to be the catalytic active centers for bifunctional 2e ORR and H O -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 H O 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 .
直接电化学氧化苯被认为是一种很有前途的方法，可以得到高附加值的苯酚产物，但这仍然是一个巨大的挑战。在这里，我们报道了一种氧配位的镍单原子催化剂（Ni-O-C），它对两电子氧还原反应（2e ORR）到 H 2 O 和 H 2 O 辅助的苯氧化到苯酚具有双功能电催化活性。在 Ni-O-C 中，Ni-(O-C)位点被证明是双功能 2e ORR 和 H 2 O 辅助苯氧化过程的催化活性中心。因此，在 0.1 m KOH 电解质中，在 1.5 V（相对于 RHE）下，Ni-O-C 在 H 2 O 的帮助下，可以将苯的转化率高达 96.4%±3.6%，苯酚的选择性为 100%，法拉第效率（FE）为 80.2%±3.2%。在单个电化学电池中，Ni-O-C 同时作为阴极和阳极的概念验证实验表明，在 10 mA cm 下，苯的转化率为 33.4%±2.2%，苯酚的选择性为 100%，FE 为 44.8%±3.0%。
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