Multivariate indium–organic frameworks for highly efficient carbon dioxide capture and electrocatalytic conversion

It is crucial to design highly selective and cost-effective materials for efficient CO2 uptake and the desirable transformation of CO2 into fuels or high-value chemical products. Here, we synthesize a series of trinuclear indium cluster-based metal–organic frameworks (MOFs) for highly efficient CO2 capture and electrocatalytic conversion into C1 products. By adjusting the metal type and replacing the ligand, the mixed metal-based MOF InCo-ABDBC-HIN shows high CO2 capture performance (101.7 cm3 g−1 at 273 K under low pressure) and superior activity (a maximum FEC1 of 81.5% at −2.2 V vs. Ag/Ag+) for electrocatalytic CO2 reduction in organic electrolytes due to its modified electronic structure. Theoretical calculations suggest that the substitution of In by Co significantly modified the electronic structure of In-based clusters, which provides rich unpaired electrons for the CO2RR and enhances the charge transfer efficiency. This work provides a specially coordinated trinuclear indium cluster-based MOF and sheds new light on the precise structural design of both CO2 adsorbents and electrocatalysts for efficient CO2 reduction.