Commercializing Ni-catalyst for dry reforming of methane (DRM) has yet to be realized due to two known issues: catalyst sintering and carbon deposition. Significantly, our developed tremella-like Ni/SiO2 has previously demonstrated outstanding resilience against sintering under prolonged heat exposure. The carry-on investigation herein further showcases its interesting self-regenerative behavior, which enables carbon removal and full activity restoration under inert N2-blanket. Better still, the resultant N2-regenerated Ni/SiO2 can immediately re-apply to DRM, contrasted to the traditional oxidative-regenerated counterpart that mandated intermediate reduction process for catalyst re-activation. Characterization results indicate that an appreciable portion (32.05 %) of deposited Ni (7.3 wt%) is reducible into active metallic phase; however, only 1.233 % of them are resided on the surface of Ni/SiO2 and involved in DRM. Despite such low involvement rate, >90 % CO2 and CH4 conversion could still be attained initially, reasonably due to the morphological prominence of the catalyst. Longevity experiment confirmed the adequacy of intermittent N2-regeneration in removing deposited carbonaceous, mechanistically assisted by the labile O-atom migrated from SiO2 support. Upon 4 h N2-regeneration, thorough activity restoration of Ni/SiO2 can be facilely realized, thereafter sustaining DRM for 1000 h with CO2 conversion controlled at > 78 %. The results herein provide important insights to DRM community, where the demonstrated N2-self-regeneration process promises a reduction-free, time- and cost-saving solution to DRM catalysts beyond Ni/SiO2.
Read full abstract