Molecular Dynamics Simulations Guide the Gasification Process of Carbon-Supported Nickel Catalysts in Biomass Supercritical Water

In this study, the Density Functional Theory (DFT) Calculations for Molecules and Clusters—ADF module is employed to model carbon-supported nickel catalysts and lignin monomers, integrating the ReaxFF module to simulate molecular dynamics under supercritical water conditions, with a focus on lignin decomposition reactions. Molecular dynamics models for supercritical water gasification are established under various conditions such as catalyst presence, water molecule quantities, and reaction temperature. By comparing simulation systems under different conditions, the yields of and variations in combustible gases (hydrogen and carbon monoxide) are summarized. Introducing heteroatoms into the lattice of the carbon support can alter the electronic structure within graphene, thereby influencing its electrical and electrochemical properties, increasing the number of active sites, and significantly enhancing electrocatalytic activity. Simulation results indicate that carbon-supported nickel metal catalysts can promote the cleavage of C–C bonds in lignin monomers, thereby increasing the rate of water–gas shift reactions and boosting hydrogen production in the system by 105%. Increasing water molecule quantities favored water–gas shift reactions and hydrogen generation while lowering carbon monoxide formation. Moreover, elevating reaction temperatures led to increased hydrogen and carbon monoxide production rates, which were particularly pronounced between 2500 K and 3500 K. These findings offer crucial theoretical insights for advancing efficient hydrogen production through biomass supercritical water gasification.