Cleavage of C-C bonds is crucial for hydrogen production via aqueous phase reforming of biomass-derived oxygenates. In this study, the hydrogen production performance and C-C bond cleavage capacity of Ni-W/AC catalysts with varying W/Ni ratios are evaluated using ethylene glycol as a model compound. A series of APR experiments conducted suggests that Ni-0.2W/AC catalyst exhibits the highest C1/C2+ratio of 15.87 and achieves a hydrogen yield of 47.76%. The enhanced Ni-W bimetallic interactions, which significantly improve the efficiency of C-C bond cleavage and increase catalyst activity by promoting active site dispersion, are confirmed by detailed characterization techniques. Further analysis of product distribution provides insights into the reaction pathways of ethylene glycol and the reaction mechanism for ethanol during aqueous phase reforming. All the results indicate that this catalytic reforming method effectively facilitates C-C bond cleavage and hydrogen production, contributing to a better understanding of APR mechanisms for biomass-derived oxygenates.
Achieving high efficiency and selectivity in cleaving aryl C–O bonds is critical for lignin valorization and the production of aromatic chemicals. A green and sustainable approach has been developed using bimetallic Ni–W catalysts, which controlled the hydrogen supply and mediated hydrogen transfer via in situ hydrogen donors. An appropriate W/Ni ratio is essential for enhancing the supply of active hydrogen, the adsorption capacity for reactive molecules, and the efficiency of hydrogen transfer, thereby optimizing the overall catalytic performance. A comprehensive investigation was conducted on the factors influencing the catalytic transfer hydrogenolysis of lignin derivatives, focusing on the reaction temperature, solvent, hydrogen source, pressure, and duration. Under optimal conditions (180 °C, 1.0 MPa N2, and <2.5 h), various lignin-derived aryl ethers achieved complete conversion with 100% monomer selectivity. This study demonstrated the excellent reusability of the Ni–W catalyst for four cycles. More significantly, the mechanisms underlying active hydrogen transfer, transfer hydrogenolysis, and bimetallic interactions were elucidated. The integration of Ni and W species significantly enhanced the synergy among active metal sites, oxygen defects, and acid sites. This synergistic mechanism enabled H• and H+ to function as the primary active hydrogen species. Furthermore, the in situ generation and targeted migration of H• radicals and H+ ions facilitated the preferential cleavage of C–O bonds over the hydrogenation of aromatic units within lignin, leading to the formation of high-value aromatic monomers.
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