Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and ***,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of ...
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Solar thermochemical CO_(2)-splitting(STCS)is a promising solution for solar energy harvesting and ***,practical solar fuel production by utilizing earth-abundant iron/iron oxides remains a great challenge because of the formation of passivation layers,resulting in slow reaction kinetics and limited CO_(2)***,we report a novel material consisting of an iron-nickel alloy embedded in a perovskite substrate for intensified CO production via a two-step STCS *** novel material achieved an unprecedented CO production rate of 381 mL g^(-1)min^(-1)with 99%CO_(2)conversion at 850℃,outperforming state-of-the-art *** situ structural analyses and density functional theory calculations show that the alloy/substrate interface is the main active site for CO_(2)*** oxidation of the FeNi alloy at the interface(as opposed to forming an FeO_(x)passivation shell encapsulating bare metallic iron)and rapid stabilization of the iron oxide species by the robust perovskite matrix significantly promoted the conversion of CO_(2)to *** regeneration of the alloy/perovskite interfaces was realized by isothermal methane reduction with simultaneous production of syngas(H_(2)/CO=2,syngas yield>96%).Overall,the novel perovskite-mediated dealloying-exsolution redox system facilitates highly efficient solar fuel production,with a theoretical solar-to-fuel efficiency of up to 58%,in the absence of any heat integration.
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