Ultrathin Two-Dimensional Bimetal-Organic Framework Nanosheets as High-Performance Electrocatalysts for Benzyl Alcohol Oxidation.

Abstract

Ultrathin two-dimensional metal-organic frameworks (2D MOFs) have the potential to improve the oxidation of benzyl alcohol (BA) with a large surface area and open catalytic active sites. To achieve high-efficiency electrocatalysts for the oxidation of benzyl alcohol, a moderate solvothermal method was evolved to synthesize a series of 2D MOFs on nickel foam (Ni-MOF/NF, NiCo-61-MOF/NF, NiCo-21-MOF/NF). As the electrocatalyst used for the oxidation of benzyl alcohol, NiCo-61-MOF/NF presented a lower overpotential and superior chemical durability than other electrocatalysts; it only required a potential of ∼1.52 V (vs RHE) to reach 338.16 mA cm-2, with an oxidation efficiency of more than 86%. Besides, after continuous electrocatalysis for 20 000 s at 1.42 V (vs RHE), the current density of NiCo-61-MOF/NF nanosheets was still 38.67 mA cm-2 with 77.34% retention. This demonstrated that NiCo-61-MOF/NF nanosheet electrocatalysts had great potential for benzyl alcohol oxidation. From both the experimental and theoretical studies, it was discovered that NiCo-61-MOF/NF nanosheets have the highest electrocatalytic activity due to their distinctive ultrathin 2D structure, optimized electron structure, and more accessible active sites. This finding would pave a brand-new thought for the design of electrocatalysts with electrocatalytic activity for benzyl alcohol oxidation (EBO).