Selective Electrochemical Reduction of CO<sub>2</sub> to Ethanol on a Heteroatom-Coordinated Dual-Atom Catalyst of Fe/Cu-NC
Fikiru Temesgen Angerasa, Endalkachew Asefa Moges, Chia-Yu Chang, Keseven Lakshmanan, Tesfaye Alamirew Dessie, Wei‐Hsiang Huang, Habib Gemechu Edao, Woldesenbet Bafe Dilebo, Chemeda Barasa Guta, Chun‐Chi Chang, Weisheng Liao, Jung Shen, Nigus Gabbiye Habtu, Meng‐Che Tsai, Wei‐Nien Su, Bing‐Joe Hwang
Abstract
High Resolution Image Download MS PowerPoint Slide Rising CO 2 emissions, particularly from industrial sectors, are driving climate change and causing severe environmental and energy crises that demand immediate action. The electrochemical CO 2 reduction reaction (eCO 2 RR) provides a sustainable approach by converting waste CO 2 into value-added products. However, achieving a high selectivity for multicarbon products in the eCO 2 RR requires advanced catalysts with large surface areas, accessible active sites, and strong synergistic interactions. Here, we introduce a dual-atom Fe/Cu-NC catalyst synthesized through a metal–organic framework (MOF)-derived method where Fe and Cu atoms are uniformly dispersed on a porous nitrogen-doped carbon matrix, forming dual heteroactive Fe–N 4 and Cu–N 3 sites. The strategic combination of these active sites significantly enhances catalytic performance, achieving a 67.4% Faradaic efficiency (FE) for ethanol at −0.8 V vs RHE in CO 2 -saturated 0.5 M KHCO 3 . In situ spectroscopic analysis confirms the formation of major *CO and *CHO intermediates during CO 2 electrolysis on the Fe/Cu-NC electrode, which are crucial for C–C coupling and ethanol production. DFT studies reveal that Fe–N 4 and Cu–N 3 sites synergistically lower the *CO intermediate energy barriers. Fe–N 4 enriches the local CO concentration, which migrates to Cu–N 3, enhancing ethanol production. This highlights MOF-derived dual-atom catalysts as a promising strategy for efficient CO 2 conversion into ecofriendly products with zero emissions.