Electronic Structure Tuning in Cu–Co Dual Single Atom Catalysts for Enhanced COOH* Spillover and Electrocalytic CO2 Reduction Activity

Authors:
Top Cited Papers
Publisher website
Google Scholar
Abstract
The development of efficient electrocatalysts for CO2 reduction to CO is challenging due to competing hydrogen evolution and intermediate over‐stabilization. In this study, a Cu–Co dual single‐atom catalyst (CuCo‐DSAC) anchored on carbon black was synthesized via scalable pyrolysis. The catalyst achieves 98.5% CO Faradaic efficiency at 500 mA cm−2, maintaining > 95% selectivity across a 400 mV window with < 6% decay over 48 h, which is superior to the corresponding single‐atom control samples. In situ spectroscopy and DFT calculations reveal a synergistic mechanism: Co sites activate CO2 and stabilize *COOH intermediates, while adjacent Cu sites facilitate CO desorption by lowering the energy barrier through charge redistribution. This dynamic buffer system mitigates active‐site blocking and suppresses HER by weakening H adsorption. The electronic interplay between Cu and Co optimizes intermediate energetics, enabling industrial‐level performance. This work demonstrates the potential of tailored dual‐site architectures for complex electrocatalytic processes, offering a promising approach to overcoming traditional limitations.

This publication has 34 references indexed in Scilit: