Affiliation:
1. Department of Mechanical and Mechatronics Engineering Waterloo Institute for Nanotechnology Materials Interfaces Foundry University of Waterloo Waterloo Ontario N2L 3G1 Canada
2. Institute of Materials Science TU Darmstadt 64287 Darmstadt Germany
3. Joint Laboratory for Extreme Conditions Matter Properties Southwest University of Science and Technology Mianyang 621010 China
4. College of Optoelectronics Technology Chengdu University of Information Technology Chengdu 610225 China
5. Laboratory of New Energy and Materials Xinjiang Institute of Engineering Urumqi 830091 China
6. Institute of Physics and Electronic Information Yunnan Normal University Kunming 650500 China
Abstract
AbstractAmine‐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 Mo2B2 MBene nanosheets using a density functional theory comprehensive study. HMF and methylamine (CH3CH2) 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 Mo2B2@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 Mo2B2 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 (εd), and material property (φ) descriptors are applied to establish a linear correlation to determine promising candidate catalysts for reductive amination of HMF. The candidates Mo2B2@Cr, Mo2B2@Zr, Mo2B2@Nb, Mo2B2@Ru, Mo2B2@Rh, and Mo2B2@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.
Funder
Natural Sciences and Engineering Research Council of Canada
National Natural Science Foundation of China
Subject
Biomaterials,Biotechnology,General Materials Science,General Chemistry
Cited by
6 articles.
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