Ying Wang, Yingying Xue, Liting Yan
May 6, 2020
Citations
0
Influential Citations
27
Citations
Journal
ACS applied materials & interfaces
Abstract
As an important organic intermediate, benzonitrile (BN) is widely involved in organic synthetic chemistry, pharmaceutical and dyestuffs industry. However, the exploration of more efficient and controllable synthesis technique and corresponding greener catalysts for the synthesis of BN still keep a great challenge. Herein, with multi-metallic two-dimension conductive metal-organic frameworks (2D cMOF) as anodic electrocatalysts, we develop a green, convenient and highly-efficient electrochemical synthesis strategy for BN. Thanks to the intrinsic 2D electrically conductive structure and the optimized the multi-metallic coupling catalytic effect, the resulting multi-metallic 2D cMOFs exhibit top-level benzylamine (BA) electrooxidation performance. Specially, the trimetallic 2D cMOF (NiCoFe-CAT) requires an ultralow potential of 1.29 V vs. RHE to achieve the 10 mA∙cm-2 current density, which indicating a fastest reaction and a most favourable thermodynamic condition. A very high yield (0.058 mmol∙mg-1∙h-1) and Faradaic efficiency (~ 87 %) of benzonitrile are both achieved during the BA electrooxidation reaction at 1.45 V. The reaction mechanism investigations indicated that the various redox mediators of MII/MIII (Ni, Co, Fe) may regard as the multi-metals active species to promote BA conversion. Also, the excellent cycling durability of multi-metallic 2D cMOFs furtherly promotes their potential practical applications. These electrocatalytic performances are considered top-level and nearly surpass all other reported Ni-based inorganics or MOF-based electrocatalysts for the electrocatalytic oxidation of benzylamine.