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

Developing efficient electrocatalysts is pivotal for electrochemical carbon dioxide (CO2) reduction to realize the selective production of valuable chemicals and fuels. Herein, we report an amino-functionalized indium-organic framework for efficient CO2 reduction to formate. The immobilized surface 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 ~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.