Integrated low carbon H₂ conversion with in situ carbon mineralization from aqueous biomass oxygenate precursors by tuning reactive multiphase chemical interactions

Meeting our rising demand for clean energy carriers such as H-2 from renewable biomass resources is challenged by the co-emission of CO2 and CH4. To address this challenge, we design novel reactive separation pathways that integrate multiphase chemical reactions by harnessing Ca and Mg bearing minerals as a sorbent to capture CO2 released during the hydrothermal deconstruction of aqueous biomass oxygenates to produce H-2 and solid carbonates via low temperature aqueous phase reforming and thermodynamically downhill carbon mineralization. Earth abundant catalysts such as Ni/Al2O3 are effective in producing H-2 yields as high as 79% and 74% using ethylene glycol and methanol in the presence of Ca(OH)(2) as an alkaline sorbent, without contaminating or deactivating the catalyst. H-2 yields with in situ carbon mineralization using a Ni or Pt/Al2O3 catalyst are enhanced based on the following order of reactivity: acetate < glycerol < methanol < formate < ethylene glycol. These studies demonstrate that the multiphase chemical interactions can be successfully tuned to enhance H-2 yields through the selective cleavage of C-C bonds using Ni/Al2O3 catalysts to deconstruct biomass oxygenates for producing H-2 and CO2, and in situ carbon mineralization by harnessing abundant alkaline materials, as demonstrated using ladle slag. This approach unlocks new scientific possibilities for harnessing multiple emissions including abundant organic-rich wastewater streams and alkaline industrial residues to co-produce low carbon H-2 and carbonate-bearing materials for use in construction by using renewable solar thermal energy resources.