Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO2 Electroreduction to Acetic Acid

• DOI: 10.1021/acs.chemmater.4c00405
• Publication Date: 2024-03-27T10:42:15Z
• Authors: Debabrata Bagchi; Mohd Riyaz; Jithu Raj; Soumyabrata Roy; Ashutosh Kumar Singh; Arjun Cherevotan; Chathakudath P. V...; Sebastian C. Peter

Electrochemical CO2 reduction reaction (eCO2RR) has been explored on tungsten carbide (WC) nanoparticles embedded N-doped graphitic carbon (NGC), demonstrating excellent activity toward the formation of acetic acid at an extremely lower potential. The further enhanced by loading ultralow copper sites into catalyst system, exhibiting 80.02% Faradaic efficiency (FE) applied potential −0.3 V (vs RHE). Potential-dependent in situ infrared (IR), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, ex extended absorption fine structure (EXAFS) studies, and computational analysis confirm that synergy between uniformly dispersed Cu atoms WC lattice plays a crucial role with high FE It observed W atom strongly chemisorbs significant change C–O bond length O–C–O angle, contrast to weaker adsorption Cu-based surfaces. presence site enhances CO2, thereby increasing possibility C–C coupling kinetically. Most importantly, hydrogen evolution predominates catalyst's surface higher potentials (−0.5 −1.1 vs RHE), elucidating mechanism underlying charge transfer WC, phenomenon ascertained through IR XPS