GC-DFT-Based Dynamic Product Distribution Reveals Enhanced CO2-to-Methanol Electrocatalysis Durability by Heterogeneous CoPc DOI
Zhiyuan Xu, Chao Ma, Beibei Tang

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 16(1), P. 294 - 307

Published: Dec. 26, 2024

Heterogeneous cobalt phthalocyanine has emerged as a promising molecular catalyst for electrochemical reduction of CO2 to methanol. Boosting both electrocatalytic durability and selectivity remains great challenge, which is more difficult with unknown regulation factors the HER side reaction. Herein, discover key balancing selectivity, well regulation, we carried out GC-DFT calculations, based on dynamic product distribution modeling was conducted visually present variation within applied voltage range. The strongly electron-donating NMe2-substituted CoPc found be an excellent candidate. reveals that balance regulate potential highest methanol Faradaic efficiency corresponding energy barrier selectivity-determining step hydrogenated CoPc. pivotal factor in stems from hindered H adsorption due ligand hydrogenation, arising decreased Co-to-H charge transfer. analysis provides intuitive theoretical guidance highly selective durable electroreduction.

Language: Английский

Electrocatalytic Reduction of CO2 to Long-Chain Hydrocarbons on (FeCoNiCu)3O4 Medium Entropy Oxide Nanoparticles DOI
Ahmad Ostovari Moghaddam, Seyedsaeed Mehrabi-Kalajahi, Mohammad Moaddeli

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 4196 - 4204

Published: April 20, 2025

Electrocatalytic CO2 reduction reaction (CO2RR) to valuable multicarbon (C2+) fuels and chemicals presents a promising strategy mitigate atmospheric accumulation promote the closure of carbon cycle. However, significant challenges persist in achieving both high product selectivity sustained stability CO2RR. In this study, catalytic performance (Fe,Co,Ni,Cu)3O4 medium entropy oxide (MEO) nanoparticles anchored on reduced graphene (rGO) was evaluated for The MEO-rGO catalyst exhibited remarkable activity, cathodic current density -0.5 A cm-2 at -1.7 V, significantly outperforming bare nickel foam (-0.15 cm-2). Additionally, demonstrated total Faradaic efficiency (FE) 60.3% C2+ products, comprising 30.6% C5H12O 29.7% C5H10O. This exceptional toward long-chain hydrocarbons is attributed enhanced C-C coupling surface, facilitated by energy barriers. Density functional theory (DFT) calculations further revealed that adsorption MEO surface are energetically favorable processes.

Language: Английский

Citations

0
GC-DFT-Based Dynamic Product Distribution Reveals Enhanced CO2-to-Methanol Electrocatalysis Durability by Heterogeneous CoPc DOI
Zhiyuan Xu, Chao Ma, Beibei Tang

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 16(1), P. 294 - 307

Published: Dec. 26, 2024

Heterogeneous cobalt phthalocyanine has emerged as a promising molecular catalyst for electrochemical reduction of CO2 to methanol. Boosting both electrocatalytic durability and selectivity remains great challenge, which is more difficult with unknown regulation factors the HER side reaction. Herein, discover key balancing selectivity, well regulation, we carried out GC-DFT calculations, based on dynamic product distribution modeling was conducted visually present variation within applied voltage range. The strongly electron-donating NMe2-substituted CoPc found be an excellent candidate. reveals that balance regulate potential highest methanol Faradaic efficiency corresponding energy barrier selectivity-determining step hydrogenated CoPc. pivotal factor in stems from hindered H adsorption due ligand hydrogenation, arising decreased Co-to-H charge transfer. analysis provides intuitive theoretical guidance highly selective durable electroreduction.

Language: Английский

Citations

0