Constructing an Active Sulfur‐Vacancy‐Rich Surface for Selective *CH3‐CH3 Coupling in CO2‐to‐C2H6 Conversion With 92% Selectivity DOI Open Access

Xiaonan Yang,

Liteng Ren,

Zhiheng Chen

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 6, 2024

Abstract To achieve high selectivity in photocatalytic CO 2 reduction to C 2+ products, increasing the number of adsorption sites and lowering energy barriers for key intermediates are critical. A ZnIn S 4 (ZIS)/MoO 3‐x (Z‐M) photocatalyst is presented, which plasmonic MoO generates hot electrons, creating a multielectron environment ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal reduces formation sulfur vacancies (S V ) ZIS, thereby enhancing activation. The ‐rich surface lowers barrier forming HCOO * −0.33 eV whereas COOH 0.77 eV. Successive hydrogenation leads CH , converts 3 with an −0.63 ‐CH 0.54 eV, lower than 0.73 form H . Thus, Z‐M preferentially produces 6 over Under visible light, achieves ‐to‐C conversion rate 467.3 µmol g −1 h 92.0% selectivity. This work highlights dual role photocatalysts improving production reduction.

Language: Английский

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO2 Reduction DOI
Hesamoddin Rabiee,

Beibei Ma,

Yang Yu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 26, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) coupled with renewable electricity holds promises for efficient mitigation of carbon emission impacts on the environment and turning into valuable chemicals. One important task in RR development is design fabrication electrodes stable operation long term. Gas‐diffusion (GDEs) have been employed to continuously feed electrolyzers. Despite significant advances GDE tailoring properties, present GDEs often suffer from critical issue flooding due electrowetting carbon‐based substrates, which hinders transition industrial application. To address flooding, intrinsically hydrophobic polymeric substrates recently fabricated shown promising performances. Herein, challenges associated carbon‐free are reviewed RR. This review first briefly outlines electrolyzers basics. Through discussion around shortcomings conventional GDEs, most recent efforts resolve summarized. Subsequently, advances, advantages, elaborated. Finally, priorities future studies suggested, aim support advancement scale‐up extend them other electrochemical systems where gas electrolyte contact.

Language: Английский

Citations

5
Unraveling the Cooperative Mechanisms in Ultralow Copper-Loaded WC@NGC for Enhanced CO2 Electroreduction to Acetic Acid DOI
Debabrata Bagchi, Mohd Riyaz, Jithu Raj

et al.

Chemistry of Materials, Journal Year: 2024, Volume and Issue: 36(7), P. 3464 - 3476

Published: March 27, 2024

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

Language: Английский

Citations

4
Operando Investigation of the Origin of C─C Coupling in Electrochemical CO2 Reduction Upon Releasing Bonding Strength, Structural Ordering in Pd─Cu Catalyst DOI
Debabrata Bagchi, Mohd Riyaz, N. C. Dutta

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 7, 2024

Abstract It is widely established that the electroreduction of carbon dioxide on a copper surface yields spectrum alcohols and hydrocarbons. But selectivity Cu toward certain product extremely poor as it forms variety reduced products concurrently. Controlling overall performance depends modification site local environment. This study depicts how can be switched from C1 to C2 multicarbon by systematic incorporation secondary metal (Pd) into lattice. Upon releasing structural ordering intermetallic alloy then bimetallic, enhancement formation CO 2 has been observed. Real‐time in situ X‐ray absorption spectroscopy (XAS) showed potential dependent evolution Pd─Cu Cu─Cu bonds different Pd‐Cu‐based catalysts. The detailed analysis IR Raman also determined adsorbed intermediate species helped identify mechanism. Computational studies show feasibility bimetallic catalysts compared current density activity have enhanced utilization flow cell gas diffusion electrode configuration.

Language: Английский

Citations

4
Scalable Low-Temperature CO2 Electrolysis: Current Status and Outlook DOI Creative Commons
Hojeong Lee,

Seontaek Kwon,

Namgyoo Park

et al.

JACS Au, Journal Year: 2024, Volume and Issue: 4(9), P. 3383 - 3399

Published: Aug. 24, 2024

The electrochemical CO2 reduction (eCO2R) in membrane electrode assemblies (MEAs) has brought e-chemical production one step closer to commercialization because of its advantages minimized ohmic resistance and stackability. However, the current performance reported eCO2R MEAs is still far below threshold for economic feasibility where low overall cell voltage (<2 V) extensive stability (>5 years) are required. Furthermore, while cost e-chemicals heavily relies on carbon capture product separation processes, these areas have received much less attention compared electrolysis, itself. In this perspective, we examine status technologies from both academic industrial points view. We highlight gap between capabilities standards offer future research directions with hope achieving industrially viable production.

Language: Английский

Citations

4
Constructing an Active Sulfur‐Vacancy‐Rich Surface for Selective *CH3‐CH3 Coupling in CO2‐to‐C2H6 Conversion With 92% Selectivity DOI Open Access

Xiaonan Yang,

Liteng Ren,

Zhiheng Chen

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 6, 2024

Abstract To achieve high selectivity in photocatalytic CO 2 reduction to C 2+ products, increasing the number of adsorption sites and lowering energy barriers for key intermediates are critical. A ZnIn S 4 (ZIS)/MoO 3‐x (Z‐M) photocatalyst is presented, which plasmonic MoO generates hot electrons, creating a multielectron environment ZIS that facilitates efficient C─C coupling reactions. Density functional theory (DFT) calculations reveal reduces formation sulfur vacancies (S V ) ZIS, thereby enhancing activation. The ‐rich surface lowers barrier forming HCOO * −0.33 eV whereas COOH 0.77 eV. Successive hydrogenation leads CH , converts 3 with an −0.63 ‐CH 0.54 eV, lower than 0.73 form H . Thus, Z‐M preferentially produces 6 over Under visible light, achieves ‐to‐C conversion rate 467.3 µmol g −1 h 92.0% selectivity. This work highlights dual role photocatalysts improving production reduction.

Language: Английский

Citations

4