Efficient Electroconversion of Carbon Dioxide to Formate by a Reconstructed Amino-Functionalized Indium-Organic Framework Electrocatalyst

We report an amino-functionalized indium-organic framework for efficient CO₂ reduction to formate. The immobilized amino groups strengthen the absorption and activation of CO₂ and stabilize the active intermediates, which endow an enhanced catalytic conversion to formate despite the inevitable reduction and reconstruction of the functionalized indium-based catalyst during electrocatalysis. The reconstructed amino-functionalized indium-based catalyst demonstrates a high Faradaic efficiency of 94.4 % and a partial current density of 108 mA cm^-2 at -1.1 V vs. RHE in a liquid-phase flow cell, and also delivers an enhanced current density of ca. 800 mA cm^-2 at 3.4 V for the formate production in a gas-phase flow cell configuration. This work not only provides a molecular functionalization and assembling concept of hybrid electrocatalysts but also offers valuable understandings in electrocatalyst evolution and reactor optimization for CO₂ electrocatalysis and beyond.