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

Abstract

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 FE_C1 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.