Interface Engineering-Modulated Nanoscale Bimetallic CoFe-MIL-88A In-Situ-Grown on 2D V2CTx MXene for Electrocatalytic Nitrogen Reduction.

Abstract

The electrochemical nitrogen reduction reaction (eNRR) provides a sustainable green development route for the nitrogen-neutral cycle. In this work, bimetallic CoFe-MIL-88A with two active sites (Fe, Co) were immobilized on a 2D V2CTx MXene surface by in situ growth method to achieve the purpose of the control interface. A large number of heterostructures are formed between small CoFe-MIL-88A and V2CTx, which regulate the electron transfer between the catalyst interfaces. The adsorption and activation of nitrogen on the active sites were enhanced, and the NRR reaction kinetics was accelerated. CoFe-MIL-88A is tightly arranged on V2CTx, which makes CoFe-MIL-88A/V2CTx have better hydrophobicity and can significantly inhibit the hydrogen evolution reaction. The synergistic effect of multicatalytic active sites and multi-interface structure of CoFe-MIL-88A/V2CTx MXene is propitious to nitrogen efficiently and stably to convert into ammonia under environmental conditions with superior selectivity and good catalytic activity. The NH3 yield rate is 29.47 μg h-1 mgcat-1 at -0.3 V vs RHE, and the Faradaic efficiency (FE) is 28.86% at -0.1 V vs RHE. The catalytic mechanism was verified to conform to the distal pathway. This work will provide a new way to develop an MXene-based electrocatalyst for eNRR.