Co‐O‐Zn interface engineering for boosting <scp> CO ₂ </scp> hydrogenation to light olefins

Abstract The carbon dioxide (CO 2 ) hydrogenation to light olefins (CO 2 ‐to‐C 2 ‐C 4 = ) represents a promising approach for its high‐value utilization but faces the crucial challenges of low CO 2 conversion efficiency and olefin selectivity. Herein, we develop an oxide–oxide interface engineering strategy to boost CO 2 ‐to‐C 2 ‐C 4 = . A high CO 2 conversion efficiency of 27.4% and C 2 ‐C 4 = yield of 15.3% with excellent stability for 200 h are achieved on optimized CoO x /ZnGa 2 O 4 –2.5/SAPO‐34 through the oxide–zeolite (OX‐ZEO) bifunctional tandem route. The well‐controlled Co‐O‐Zn oxide–oxide interface in CoO x /ZnGa 2 O 4 facilitates the bidentate adsorption of CO 2 , enabling the exposed C atom to be attracted by spilled‐over H* from the heterolytic cleavage on adjacent Zn‐O. Accordingly, the preferentially produced HCOO* leads to effective CO 2 conversion and selective generation of methanol precursor. Therefore, this oxide–oxide interfacial engineering offers a promising strategy for achieving highly efficient CO 2 ‐to‐C 2 ‐C 4 = through OX‐ZEO route.