Comprehensive Study Addressing the Challenge of Efficient Electrocatalytic Biomass Upgrading of 5‐(Hydroxymethyl)Furfural (HMF) with a CH3NH2 Ionic Liquid on Metal‐Embedded Mo2B2 MBene Nanosheets

Abstract Amine‐containing derivatives are important intermediates in drug manufacturing; sustainable synthesis of amine compounds from green carbon‐based biomass derivatives has attracted increasing attention, especially the reductive amination of biomass molecules via electrochemical upgrading. To achieve efficient reductive amination of 5‐(hydroxymethyl)furfural (HMF) via electrocatalytic biomass upgrading, this work proposes a new HMF biomass upgrading strategy based on metal supported on Mo 2 B 2 MBene nanosheets using a density functional theory comprehensive study. HMF and methylamine (CH 3 CH 2 ) can be reduced to 5‐(hydroxymethyl) aldiminefurfural (HMMAMF) via electrocatalytic biomass upgrading, which is identified as a promising technology to produce pharmaceutical intermediates. Based on the proposed reaction mechanisms of HMF reductive amination, this work performs a systematic study of HMF amination to HMMAMF using an atomic model simulation method. This study aims to design a high‐efficiency catalyst based on Mo 2 B 2 @TM nanosheets via the reductive amination of 5‐HMF and provide insights into the intrinsic relation between thermochemical and material electronic properties and the role of dopant metals. This work establishes the Gibbs free energy profiles of each reaction HMF Biomass Upgrading on Mo 2 B 2 systems and obtained the limiting potentials of the rate‐determining step, which included the kinetic stability of dopants, HMF adsorbability, and the catalytic activity and selectivity of the hydrogen evolution reaction or surface oxidation. Furthermore, charge transfer, d‐band center ( ε d ), and material property ( φ ) descriptors are applied to establish a linear correlation to determine promising candidate catalysts for reductive amination of HMF. The candidates Mo 2 B 2 @Cr, Mo 2 B 2 @Zr, Mo 2 B 2 @Nb, Mo 2 B 2 @Ru, Mo 2 B 2 @Rh, and Mo 2 B 2 @Os are suitable high‐efficiency catalysts for HMF amination. This work may contribute to the experimental application of biomass upgrading catalysts for biomass energy and guide the future development of biomass conversion strategies and utilization.