Global energy-related CO2 emissions have reached 3.15 x 1011 tons at a record high in 2020. Reducing CO2 emissions requires multi-faceted negative emission technologies. Our vision is that CO2 in the air can be monetized as it can be profitable to capture the CO2 directly from the atmosphere and turn it into valuable chemical products. Here, we demonstrated H2-free CO2 valorization pathway throughout two-step tandem processes of CO2-assisted oxidative dehydrogenation of ethane (CODE) and CO-ethylene carbonylation (CEC). A binuclear single-site and noble-metal-free (ZnCr)1/SSZ-13 catalyst has been developed for highly efficient co-conversion of CO2 and ethane, surpassing existing transition metal-based catalysts. C(CO2) = 18.7%; C(C2H6) = 19.8%; S(C2H4) = 93%; CO2 utilization = 95% at 550 oC; Space-time yield (STY) of ethylene of 0.55 kg h-1 kg-1(Zn+Cr); 100% of regeneration capability within 150 h at 500 oC. Low-coordinated, low valence-state, and local atomic disordered Znδ+ account for the outstanding CODE performance to produce CO and ethylene, which will be the feedstock for the 2nd-step CEC transformation to valuable oxygen-containing polymers. Our concepts of SSCs material design and tandem process design demonstrated here will give insights into future directions of CO2 valorization and steer the relevant technology development.

CO2 fixation into polymer

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