Engineering Catalyst-Support Interactions in Cobalt Phthalocyanine for Enhanced Electrocatalytic CO2 Reduction: The Role of Graphene-Skinned Al2O3 DOI Creative Commons
Qianqian Bai,

Bingyun Ma,

Le Wei

et al.

Chemical Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Electrocatalytic CO2 reduction (eCO2R) driven by renewable electricity holds great promise to mitigate anthropogenic emissions. In this study, we engineer cobalt phthalocyanine (CoPc) supported on graphene-skinned Al2O3 nanosheets (CoPc/Al2O3@C) enhance CO2-to-CO conversion. The strong π-π stacking between the CoPc macrocycle and interlayer graphene, coupled with electronic repulsion Co2+ center Al2O3, induces a structural distortion in CoPc, raising energy level of d z2 orbital. This perturbation facilitates activation, shifts rate-determining step, thereby substantially accelerates overall eCO2R kinetics. optimal catalyst demonstrates near-unity CO faradaic efficiency (FECO) across wide current range, achieving high partial density 388 mA cm-2 an exceptional turnover frequency (TOF) 43 s-1, addition prolonged operational stability membrane electrode assembly (MEA). work, leveraging vectorial interactions molecular moieties substrate reshape macrocyclic structure realign orbital energies offers new insights into design efficient electrocatalysts for eCO2R.

Language: Английский

Dual Effect of Oxygen Vacancy‐Enriched TiO2 Interlayer in Si Photocathode for Enhanced Photoelectrochemical CO2 Reduction to HCOOH DOI Open Access
Jun Xing, Junxia Shen,

Zhihe Wei

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 6, 2025

Integrating nanostructured catalysts with semiconductors is a prevalent strategy for the design of photoelectrochemical (PEC) photocathodes toward CO2 reduction reaction (CO2RR). However, it still challenge to achieve high efficiency and selectivity due incompatible catalyst/semiconductor heterogeneous interface. Here, proposed that engineering oxygen vacancy in TiO2 interlayer plays multifunctional role boosting PEC activity CO2RR on Bi catalyst modified Si photocathode (denoted as Si/dT/Bi). It discovered accelerates carrier transport. These vacancies also promote growth Bi-based sponge-like nanostructures during photoelectro-deposition process. Numerous experimental results combined situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal these nano-catalysts Si/dT/Bi provide density active sites adsorption kinetics HCOOH production by accelerating formation key intermediate *OCHO. This provides unique route future advancements technologies.

Language: Английский

Citations

1
Electrolytic CO2 reduction in membrane electrode assembly: Challenges in (Bi)carbonate, crossover, and stability DOI Creative Commons
Minqiu Lan, Wenhao Ren

Next Materials, Journal Year: 2025, Volume and Issue: 6, P. 100506 - 100506

Published: Jan. 1, 2025

Language: Английский

Citations

0
Redox‐Mediated CO2 Electrolysis for Recovering Transmembrane Carbon Loss DOI Open Access
Xinhui Yu, Liwei Xue, Yi Liao

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 9, 2025

CO2 electrolysis in alkaline media presents advantages by suppressing the competitive hydrogen evolution reaction (HER) and enhancing reduction selectivity. However, it suffers from carbonation issue, leading to substantial carbon loss due transmembrane transport. To tackle this we here put forward a redox mediator (RM)-coupled strategy. By integrating highly reversible couple, approach spatially separates cathodic anodic oxygen reactions (OERs) into two electrolyzers, thereby enabling recovery reuse of CO2. Anthraquinone-2,7-disulfonic acid (AQDS) was chosen as owing its suitable potential, excellent electrochemical reversibility, high solubility, nontransmembrane shuttling characteristics. It allowed RM-coupled system operate continuously at 100 mA/cm2, maintaining Faradaic efficiency (FE) for CO2-to-CO conversion consistently around 90%, while effectively capturing This proof-of-concept demonstration validates feasibility highlights significant potential advance practical application electrolysis.

Language: Английский

Citations

0
Redox‐Mediated CO2 Electrolysis for Recovering Transmembrane Carbon Loss DOI Open Access
Xinhui Yu, Liwei Xue, Yi Liao

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 9, 2025

Abstract CO 2 electrolysis in alkaline media presents advantages by suppressing the competitive hydrogen evolution reaction (HER) and enhancing reduction selectivity. However, it suffers from carbonation issue, leading to substantial carbon loss due transmembrane transport. To tackle this we here put forward a redox mediator (RM)‐coupled strategy. By integrating highly reversible couple, approach spatially separates cathodic anodic oxygen reactions (OERs) into two electrolyzers, thereby enabling recovery reuse of . Anthraquinone‐2,7‐disulfonic acid (AQDS) was chosen as owing its suitable potential, excellent electrochemical reversibility, high solubility, nontransmembrane shuttling characteristics. It allowed RM‐coupled system operate continuously at 100 mA/cm , maintaining Faradaic efficiency (FE) for ‐to‐CO conversion consistently around 90%, while effectively capturing This proof‐of‐concept demonstration validates feasibility highlights significant potential advance practical application electrolysis.

Language: Английский

Citations

0
Microenvironment modulation induced by ethylene-glycol modification enables high activity in selective CO2 electroreduction over lead-based catalysts DOI

Yingying Shu,

Zhihao Wang, Zichen Song

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161963 - 161963

Published: April 1, 2025

Language: Английский

Citations

0
Environmentally Friendly and Earth-Abundant Self-Healing Electrocatalyst Systems for Durable and Efficient Acidic Water Splitting DOI
Xuan Minh Chau Ta, Thành Trần‐Phú, Thi Kim Anh Nguyen

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: April 21, 2025

Electrochemical water splitting under acidic conditions is an efficient route for green hydrogen production from renewable electricity. Its implementation on a globally relevant scale hindered by the lack of abundant and low-cost electrocatalysts oxygen evolution reaction that can operate stably efficiently highly anodic conditions. Here, we report design stable OER consisting self-healing bismuth (Bi)-based matrix hosting transition metal active sites. Comprehensive structural performance investigation Co- Ni-BiOx electrodes provides insights into role electrolyte composition pH in mechanism Our best-performing [Co-Bi]Ox [Ni-Bi]Ox anodes achieve over 200 h continuous electrolysis at catalytic current 10 mA cm-2 with overpotential 590 670 mV 1 0.1 M H2SO4 electrolyte. Notably, while [Bi]Ox did not contribute to activity, it was essential stabilize Co Ni sites during OER. findings provide promising strategy engineering earth-abundant materials splitting, as alternative use poorly scalable expensive noble catalysts.

Language: Английский

Citations

0
Reactor operating parameters and their effects on the local reaction environment of CO(2) electroreduction DOI Creative Commons
Xiao Kun Lu, Linsey C. Seitz

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review traces the intricate connections of operational parameters and local reaction environment effects aqueous electrochemical CO (2) reduction.

Language: Английский

Citations

0
Engineering Catalyst-Support Interactions in Cobalt Phthalocyanine for Enhanced Electrocatalytic CO2 Reduction: The Role of Graphene-Skinned Al2O3 DOI Creative Commons
Qianqian Bai,

Bingyun Ma,

Le Wei

et al.

Chemical Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Electrocatalytic CO2 reduction (eCO2R) driven by renewable electricity holds great promise to mitigate anthropogenic emissions. In this study, we engineer cobalt phthalocyanine (CoPc) supported on graphene-skinned Al2O3 nanosheets (CoPc/Al2O3@C) enhance CO2-to-CO conversion. The strong π-π stacking between the CoPc macrocycle and interlayer graphene, coupled with electronic repulsion Co2+ center Al2O3, induces a structural distortion in CoPc, raising energy level of d z2 orbital. This perturbation facilitates activation, shifts rate-determining step, thereby substantially accelerates overall eCO2R kinetics. optimal catalyst demonstrates near-unity CO faradaic efficiency (FECO) across wide current range, achieving high partial density 388 mA cm-2 an exceptional turnover frequency (TOF) 43 s-1, addition prolonged operational stability membrane electrode assembly (MEA). work, leveraging vectorial interactions molecular moieties substrate reshape macrocyclic structure realign orbital energies offers new insights into design efficient electrocatalysts for eCO2R.

Language: Английский

Citations

0