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.