Solar-driven biomass photoreforming (PR) is a sustainable and potentially economical technology for green energy carriers such as H2 and value-added chemicals. However, most previous studies on biomass PR only focused on hydrogen evolution reaction (HER) by directly using biomass derived soluble components as sacrificial reagents to consume photogenerated holes. It will be more promising to selectively convert biomass as feedstock to value-added chemicals along with H2 generation during PR process, namely biomass photorefinery. Our research aims to produce sustainable H2 and value-added chemicals by using alternative oxidation half-reactions to selectively utilize biomass, waste polymers or chemicals. To realize this concept, biomass feedstocks pretreatment, proper catalyst, reactor design and substrate are taken into consideration.
Biomass PR always suffers slow reaction kinetics due to the complex structure and recalcitrant characteristics of substrates. Physicochemical pretreatment for lignocellulose (cellulose, hemicellulose and lignin) is usually required to firstly disrupt the highly organized cell wall structure and increase the accessibility with catalyst.
Good catalyst design should take light absorption, charge transfer, mass diffusion, surface redox reaction et al into consideration. We are constructing catalysts with a hierarchically porous structure, heterojunction structure, solid solution, plasmonics, 2D materials, quantum dots, and carbon-based nanomaterials to improve the efficiency and selectivity for biomass photorefinery.
We have designed and fabricated some free-standing reactors with circulating condensate jackets to control reaction temperature for the suspended system and photoelectrochemical system. We also construct an automatic on-line system with GC.
Considering the specificity (functional group, solubility, basic unit) of different substrates (sugars, alcohols, cellulose, lignin, hemicellulose, plastic waste et al), reaction conditions such as solvent, pH, atmosphere are systematically investigated for improving value-added chemicals selectivity.
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