Photocatalytic Cellulose Reforming For H-2 And Formate Production By Using Graphene Oxide-Dot Catalysts

The mechanism of photocatalytic biomass reforming for H-2 production is far from fully understood. This study uses functionalized graphene dots with Pt-cocatalyst to reform cellulose in an alkaline solution under 1 sun illumination. Reforming of cellulose is initiated with the peeling of its constituent 6-glucose units, which subsequently transform into deprotonated isosaccharinic acid (C-6). Further degradation of C-6 into molecules C-5-C-1 proceeds through successive alternation of C-eliminating hydrolysis and photocatalytic oxidation of C-6 derivatives. The C-6-C-1 species are quantitatively identified using chromatography and mass spectroscopy. The end C-containing product is predominantly HCOO- rather than HCO3- (or CO2). The photocatalytic oxidation is accompanied by the photocatalytic reduction of water to produce H-2. This reforming steadily produced H-2 for 6 days with a negligible rate decay, accomplishing 35% of the theoretical ultimate value for the reforming of cellulose. This study elucidates the detailed mechanism in the photocatalytic reforming of cellulose.