Multi-enzyme reaction inspired cascade photocatalysis for solar-driven CO2 reduction to ethane DOI Creative Commons
Jianji Wang, Huiyong Wang, Zhimin Liu

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 24, 2024

Abstract Solar-driven photocatalytic CO2 conversion into value-added chemicals and fuels is an emerging solution to the challenges of traditional energy environmental/climate concerns. However, synthesis two-carbon (C2) compounds quite challenging due high activation barrier C-C coupling reaction low content intermediates. Herein, inspired by tandem in multi-enzyme reactions, Cu-N4 Mo-N4 active sites have been designed integrated CuPor-POP-Mo as cascade dual metal for efficient reduction ethane (C2H6) first time. Significantly, excel-lent C2H6 production rate 472.5 µmol g− 1 h− a product selectivity 87.5% (electron ~ 97.5%) achieved, which are record values using porous polymer catalysts. In-situ spectral characterizations DFT calculations indicate that unlike electrocatalytic C2 products reported previously, Cu site mainly catalyzes *CO production, Mo triggers between intermediates, thus synergistically boost photoreduction C2H6. Our work provides new insights rational design photocatalysts effective C2+ from CO2.

Language: Английский

Recent progress in electrocatalytic C-N coupling of CO2 and inorganic N-containing small molecules DOI
Huijuan Jing, Jun Long, Dunfeng Gao

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Language: Английский

Citations

0
A Pulsed Tandem Electrocatalysis Strategy for CO2 Reduction DOI
Hao Sun, Jing‐yao Liu

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 18, 2025

Electroreduction of CO2 to value-added C2 products remains hindered by sluggish C-C coupling kinetics and competing side reactions. Inspired the tandem catalytic mechanisms multienzyme systems, we designed a dual-site single-atom nanozyme (DSAN) comprising FeN4 FeO4 sites (FeN4-FeO4). Density functional theory (DFT) calculations under constant potential reveal that site functions as CO generator, while facilitates migration, coupling, subsequent product formation. To further optimize efficiency, introduced pulsed electrocatalysis strategy alternating between zero -0.7 V. This approach dynamically modulates active-site functions: at -0.70 V, adsorption *CH3CH2OH formation are facilitated, 0 migration enhanced due spin-state transitions during switching. Additionally, suppresses excessive hydrogenation key intermediates, thereby improving CH3CH2OH selectivity. These findings highlight synergistic integrating catalysis control, offering novel effective for CO2-to-C2 conversion using SAN catalysts.

Language: Английский

Citations

0
Multi-enzyme reaction inspired cascade photocatalysis for solar-driven CO2 reduction to ethane DOI Creative Commons
Jianji Wang, Huiyong Wang, Zhimin Liu

et al.

Research Square (Research Square), Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 24, 2024

Abstract Solar-driven photocatalytic CO2 conversion into value-added chemicals and fuels is an emerging solution to the challenges of traditional energy environmental/climate concerns. However, synthesis two-carbon (C2) compounds quite challenging due high activation barrier C-C coupling reaction low content intermediates. Herein, inspired by tandem in multi-enzyme reactions, Cu-N4 Mo-N4 active sites have been designed integrated CuPor-POP-Mo as cascade dual metal for efficient reduction ethane (C2H6) first time. Significantly, excel-lent C2H6 production rate 472.5 µmol g− 1 h− a product selectivity 87.5% (electron ~ 97.5%) achieved, which are record values using porous polymer catalysts. In-situ spectral characterizations DFT calculations indicate that unlike electrocatalytic C2 products reported previously, Cu site mainly catalyzes *CO production, Mo triggers between intermediates, thus synergistically boost photoreduction C2H6. Our work provides new insights rational design photocatalysts effective C2+ from CO2.

Language: Английский

Citations

0