Abstract
The unique molecular trapdoor mechanism of chabazite zeolites provides an ideal platform for CO2 integrative adsorption and conversion. Herein, a mesoporous In-SSZ-13_((MP))) catalyst was successfully synthesized through desiliconization combined with anchoring uniformly dispersed indium (In) active sites, which achieved the highest formate Faraday efficiency (FE_(HCOO~-)) of 92.0 % and a formate partial current density (jhcoo-) of 133.3 mA cm~(-2) for electrochemical CO2 reduction reaction (CO2RR) at a moderate overpotential of 0.8 V. Experimental results combined with DFT calculations reveal the reaction mechanism of In-SSZ-13_((MP)) electrocatalytic reduction of CO2: as the only channel into the In-SSZ-13_((MP)) crystal, the gatekeeper (cation, In~(3+)) in eight-membered ring (8MR) deviates from its original position induced by CO2 molecule, then CO2 poured into CHA cage and fully reacted with uniformly distributed indium active sites.
NSTL