Exogenous addition of H₂ for an in situ biogas upgrading through biological reduction of carbon dioxide into methane

Biological reduction of CO₂ into CH₄ by exogenous addition of H₂ is a promising technology for upgrading biogas into higher CH₄ content. The aim of this work was to study the feasibility of exogenous H₂ addition for an in situ biogas upgrading through biological conversion of the biogas CO₂ into CH_4. Moreover, this study employed systematic study with isotope analysis for providing comprehensive evidence on the underlying pathways of CH₄ production and upstream processes. Batch reactors were inoculated with digestate originating from a full-scale biogas plant and fed once with maize leaf substrate. Periodic addition of H₂ into the headspace resulted in a completely consumption of CO₂ and a concomitant increase in CH₄ content up to 89%. The microbial community and isotope analysis shows an enrichment of hydrogenotrophic Methanobacterium and the key role of hydrogenotrophic methanogenesis for biogas upgrading to higher CH₄ content. Excess H₂ was also supplied to evaluate its effect on overall process performance. The results show that excess H₂ addition resulted in accumulation of H₂, depletion of CO₂ and inhibition of the degradation of acetate and other volatile fatty acids (VFA). A systematic isotope analysis revealed that excess H₂ supply led to an increase in dissolved H₂ to the level that thermodynamically inhibit the degradation of VFA and stimulate homo-acetogens for production of acetate from CO₂ and H₂. The inhibition was a temporary effect and acetate degradation resumed when the excess H₂ was removed as well as in the presence of stoichiometric amount of H₂ and CO₂. This inhibition mechanism underlines the importance of carefully regulating the H₂ addition rate and gas retention time to the CO₂ production rate, H₂-uptake rate and growth of hydrogenotrophic methanogens in order to achieve higher CH₄ content without the accumulation of acetate and other VFA.