Issue 38, 2023

Revealing the role of aniline in assisting SnO2 electrocatalytic CO2 reduction to HCOOH: via the perspective of the reaction pathway

Abstract

Sn-based electrocatalysts are exceptionally competitive for electrochemical reduction of CO2 (CO2ER) applications. The rate-controlling step of Sn-based catalysts, extensively investigated through experiment and theoretical studies, primarily involves the electron transfer process from CO2 to form surface-adsorbed *CO2˙. In light of this, the introduction of amines to enhance guest–host interaction for CO2 adsorption and simultaneously reduce the reaction energy barrier is an innovative tactic that will make a decisive contribution to improving the CO2ER performance. Herein, an aniline modified tin oxide composite catalyst (SnO2/PDA0.5-OCNTs) was constructed and applied to electrocatalytic CO2 reduction to produce HCOOH. A thin amorphous organic aniline layer was formed on the exterior of oxidized carbon nanotubes (OCNTs), which anchors tin oxide nanoparticles (SnO2 NPs) and improves the stability of the composite electrocatalysts. Depending on the robust chemical interactions between aniline and CO2, the captured CO2 is converted into an intriguing carbamate intermediate (NHCOO*), which reduces the reaction energy barrier through a new reaction pathway and accelerates the reaction kinetics of the rate-determining step for CO2ER to generate HCOOH. Benefiting from these merits, SnO2/PDA0.5-OCNTs delivered an excellent HCOOH faradaic efficiency (FEHCOOH) of 96% at −1.43 V (vs. RHE) with a satisfactory HCOOH partial current density (jHCOOH) of 166 mA cm−2 at −1.83 V in a flow cell.

Graphical abstract: Revealing the role of aniline in assisting SnO2 electrocatalytic CO2 reduction to HCOOH: via the perspective of the reaction pathway

  • This article is part of the themed collection: #MyFirstJMCA

Supplementary files

Article information

Article type
Paper
Submitted
24 Jul 2023
Accepted
05 Seb 2023
First published
20 Seb 2023

J. Mater. Chem. A, 2023,11, 20796-20807

Revealing the role of aniline in assisting SnO2 electrocatalytic CO2 reduction to HCOOH: via the perspective of the reaction pathway

Y. Zhang, H. Jiang, K. Wang, D. Niu and X. Zhang, J. Mater. Chem. A, 2023, 11, 20796 DOI: 10.1039/D3TA04368A

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