Spatially‐Directed C─C Coupling inside Three‐dimensional Metal‐organic Frameworks for CO
<sub>2</sub>
Electroreduction to C
<sub>2</sub>
Products
Youxuan Ni, Weiwei Xie, Zhenhua Yan, Fangyi Cheng, Jun Chen
Angewandte Chemie International Edition10/23/2025·DOI·Read paper
Abstract
<jats:title>Abstract</jats:title>
<jats:p>
The CO
<jats:sub>2</jats:sub>
electroreduction reaction to fuels and chemicals is a promising strategy for storing intermittent energy (such as sunlight and wind power) and closing the carbon cycle. Producing multi‐carbon oxygenates and hydrocarbons (C
<jats:sub>2+</jats:sub>
) with broader applicability is highly desirable. However, the difficulty of the C─C coupling reaction hinders the conversion of CO
<jats:sub>2</jats:sub>
to C
<jats:sub>2+</jats:sub>
products with high energy input, low reaction rate, and poor selectivity. Here, we construct a three‐dimensional (3D) Fe‐quinoxalinedithiol (Fe‐QDT)‐based metal‐organic framework (MOF) featuring dual Fe sites within its ordered channel walls, enabling efficient interwall electrocatalysis for C
<jats:sub>2</jats:sub>
coupling reactions. We found that dual Fe sites can co‐catalyze the dimerization of *OCH
<jats:sub>2</jats:sub>
to *OCH
<jats:sub>2</jats:sub>
CH
<jats:sub>2</jats:sub>
O*, thus facilitating the generation of C
<jats:sub>2</jats:sub>
products. The free energy changes for the potential‐limiting steps in the electroreduction of C
<jats:sub>2</jats:sub>
species are −0.010 and 0.045 eV for CH
<jats:sub>3</jats:sub>
CH
<jats:sub>2</jats:sub>
OH and C
<jats:sub>2</jats:sub>
H
<jats:sub>4</jats:sub>
, respectively, which are significantly lower than those for other C
<jats:sub>2</jats:sub>
products. Consequently, the Fe‐QDT MOFs demonstrate high activity and selectivity in converting CO
<jats:sub>2</jats:sub>
to CH
<jats:sub>3</jats:sub>
CH
<jats:sub>2</jats:sub>
OH and C
<jats:sub>2</jats:sub>
H
<jats:sub>4</jats:sub>
. This work designs a novel and efficient active site for C─C coupling and provides valuable insights into the design principles of electrocatalysts for C
<jats:sub>2</jats:sub>
products.
</jats:p>
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