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Reconstructed Bi-Sn Interfacial Sites Coupled with a Supramolecular Cation Cage Enable Low K+ Acidic CO2 Electroreduction to Formate
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DOI：10.1002/aenm.71428.png)
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Abstract
En 中文
Here, we demonstrate selective carbon dioxide reduction reaction (CO2RR) to formic acid (HCOOH) conversion under highly acidic conditions and low K+ concentration using a carbon-supported Bi-Sn bimetallic electrocatalyst (Bi-Sn/C) in combination with 2.2.2-cryptand for cation regulation. Thermal reduction of a Bi2Sn2O7 precursor yields an interface-rich Bi-Sn architecture with strong electronic coupling between Bi and Sn domains. Density Functional Theory (DFT) calculations reveal that the Bi−Sn synergy arises from a bidirectional electronic interplay: Sn enhances the activity of Bi for *OCHO generation, while Bi regulates Sn for the conversion of *OCHO to *HCOOH. This cooperative mechanism enables CO2RR to outcompete the hydrogen evolution reaction under highly acidic conditions. We further introduce supramolecular cation regulation as a complementary strategy to enhance interfacial alkali-metal ion effects. DFT calculations reveal that molecular cages such as 2.2.2. cryptand and 18-crown ether-6 selectively bind K+ ions at the catalyst-electrolyte interface, stabilizing CO2-derived intermediates while suppressing proton adsorption. As a result, cryptand-modified Bi-Sn/C achieves a HCOOH faradaic efficiency of 94% at pH = 1, with only 50 mM K2SO4 concentration. Response surface methodology further identifies cryptand loading as the dominant parameter governing selectivity, with a greater influence than applied potential and pH.
Keywords:
bimetallic catalysts
DFT
electrocatalysis
pyrochlore-derived materials
response surface methodology
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