Effect of H2S on biogas sorption enhanced steam reforming using a Pd/Ni-Co catalyst and dolomite as a sorbent

Abstract

To achieve net zero carbon emissions from energy systems, biogas has become an attractive renewable resource for hydrogen production. The sorption enhanced steam reforming (SESR) process is proposed to produce high-purity hydrogen from biogas, enabled by combining the catalytic reforming reaction with the simultaneous CO2 removal by sorption in a single reactor. One of the most critical challenges in using biogas in conventional reforming processes is the presence of H2S since it may deactivate the reforming catalyst. Here we experimentally study the effect of the biogas H2S concentration on the H2 production by SESR, i.e., accounting for the presence of a CaO-based solid sorbent. This work was performed in a fixed-bed reactor using a Pd/Ni-Co hydrotalcite-like material (HT) catalyst and dolomite as CO2 sorbent. Biogas (60CH4/40CO2 vol.%) with different concentrations of H2S (150, 350, 500 and 1000 ppm) was evaluated. The catalyst did not deactivate for biogas H2S concentrations of 150 and 350 ppm during five cycles of the SESR process. However, a slight decrease in the catalyst activity was detected under higher sulfur concentrations after the third SESR cycle. Sulfur was detected in the spent catalyst and sorbent materials, with a higher proportion in the sorbent for the highest H2S concentration tested (1000 ppm). H2 yield decreased by 10.8% and 4.5% points for biogas H2S concentrations of 500 and 1000 ppm after five cycles, respectively, while H2 purity decreased by only 3 vol.% and 2 vol.% points, respectively.