Mechanistic insights into selective CO2 electroreduction to methanol on cobalt tetraaminophthalocyanine DOI Creative Commons
Yun Mi Song, Yong Liu, Jianjun Su

et al.

Chem Catalysis, Journal Year: 2023, Volume and Issue: 3(12), P. 100839 - 100839

Published: Dec. 1, 2023

Language: Английский

Boosting CO2 Electroreduction over a Covalent Organic Framework in the Presence of Oxygen DOI
Hui Guo, Duan‐Hui Si,

Hong‐Jing Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(14)

Published: Feb. 7, 2024

Herein, we propose an oxygen-containing species coordination strategy to boost CO

Language: Английский

Citations

57
Backbone Engineering of Polymeric Catalysts for High‐Performance CO2 Reduction in Bipolar Membrane Zero‐Gap Electrolyzer DOI Creative Commons
Geng Li, Libei Huang,

Chengpeng Wei

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 13, 2024

Abstract Bipolar membranes (BPMs) have emerged as a promising solution for mitigating CO 2 losses, salt precipitation and high maintenance costs associated with the commonly used anion‐exchange membrane electrode assembly reduction reaction (CO RR). However, industrial implementation of BPM‐based zero‐gap electrolyzer is hampered by poor RR performance, largely attributed to local acidic environment. Here, we report backbone engineering strategy improve performance molecular catalysts in electrolyzers covalently grafting cobalt tetraaminophthalocyanine onto positively charged polyfluorene (PF‐CoTAPc). PF‐CoTAPc shows acid tolerance BPM (BPMEA), achieving FE 82.6 % at 100 mA/cm utilization efficiency 87.8 %. Notably, selectivity, carbon long‐term stability BPMEA outperform reported systems. We attribute enhancement stable cationic shield double layer suppression proton migration, ultimately inhibiting undesired hydrogen evolution improving selectivity. Techno‐economic analysis least energy consumption (957 kJ/mol) catalyst BPMEA. Our findings provide viable designing efficient environments.

Language: Английский

Citations

11
Curved strain-induced modulation of potential difference optimizes electron-mediated persulfate activation for pollutant removal DOI
Junjie Xu,

Yanchi Yao,

Chao Zhu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 357, P. 124285 - 124285

Published: June 12, 2024

Language: Английский

Citations

8
Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO2 Electroreduction DOI
Mengyang Zhang,

Dingyang Zhou,

Xueqin Mu

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: May 27, 2024

Electrocatalysis is a very attractive way to achieve sustainable carbon cycle by converting CO

Language: Английский

Citations

7
Constructing Ionic Interfaces for Stable Electrochemical CO2 Reduction DOI
Yong Liu, Yun Mi Song, Libei Huang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(22), P. 14020 - 14028

Published: May 20, 2024

The electrochemical CO2 reduction reaction (CO2RR) has emerged as a promising approach for sustainable carbon cycling and valuable chemical production. Various methods strategies have been explored to boost CO2RR performance. One of the most includes construction stable ionic interfaces on metallic or molecular catalysts using organic inorganic cations, which demonstrated significant improvement in catalytic interface is instrumental adjusting adsorption behavior, influencing reactive intermediates, facilitating mass transportation, suppressing hydrogen evolution reaction, particularly under acidic conditions. In this Perspective, we provide an overview recent advancements building electrocatalytic process discuss application strategy improve performance catalysts. We aim convey future trends opportunities creating further enhance utilization efficiency productivity products. emphasis Perspective lies pivotal role catalysis, providing reference research critical field.

Language: Английский

Citations

6
Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO2 to Methanol on Cu3P@C DOI

Haoming Yu,

Xinxin Han, Zhengyu Hua

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(17), P. 12783 - 12791

Published: Aug. 9, 2024

Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu3P@C, which has a high-electron-density layer, delivers high faradaic efficiency for methanol of 61.2% at −0.36 V versus reversible hydrogen electrode (RHE), and record partial current density 130 mA cm–2 −0.76 RHE when it is assembled gas diffusion in flow cell setup using 1 M KOH electrolyte, outperforming most state-of-the-art electrocatalysts. In contrast, Cu2Se@C Cu1.8S@C, low-electron-density layers, predominately produce formate. situ Raman spectroscopy analysis computational functional theory calculations reveal influence Cu3P electronic properties binding sites underlying mechanisms production.

Language: Английский

Citations

4
Modulating Active Center Microenvironment in Phthalocyanine‐Based Covalent Organic Frameworks for Enhanced Electrocatalytic CO2 to CH3OH DOI Open Access

Qin Wang,

Jikun Chen, Houhe Pan

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 27, 2025

Abstract Developing catalysts for electrocatalytic CO 2 to CH 3 OH still faces great challenge due the involvement of multiple proton‐coupled electron transfer (PCET) processes. Molecular phthalocyanine electrocatalysts on carbon nanotubes have achieved production methanol as sole liquid‐phase product but with activity and stability far from meeting industrial demands. Herein, phthalocyaninato cobalt is fabricated into covalent organic frameworks PE‐COF via polymerization ellagic acid. Subsequent hydrolyzation ester groups in this framework affords COOH/OH‐containing PEH‐COF, resulting successful modulation over local microenvironment Co electrochemical active center turn rendering high yield durability. Experimental theoretical investigations reveal that construction COOH group H O participated catalytic cages PEH‐COF can effectively fix hydrated potassium ions, which efficiently enhances PCET kinetics lowers energy barriers conversion OH. The partial current density ( j ) Faraday efficiency could reach 100.9 mA cm −2 38.5%, respectively. Moreover, be maintained at 100.4 after 9 h electrocatalysis, superior thus reported catalysts.

Language: Английский

Citations

0
Nuclear magnetic resonance spectroscopy: A comprehensive tool for analyzing liquid products in electrochemical CO2 reduction DOI Creative Commons
Aymen S. Abu Hatab,

Yahia H. Ahmad,

Mohamed F. Mady

et al.

Journal of Electroanalytical Chemistry, Journal Year: 2025, Volume and Issue: unknown, P. 119097 - 119097

Published: March 1, 2025

Language: Английский

Citations

0
Unlocking the Potential for Methanol Synthesis via Electrochemical CO2 Reduction Using CoPc-Based Molecular Catalysts DOI
Libo Yao, Jie Ding,

Xinhai Cai

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(33), P. 21623 - 21632

Published: Aug. 8, 2024

The electrochemical CO2 reduction reaction (CO2RR) to produce methanol (CH3OH) is an attractive yet challenging approach due a lack of selective electrocatalysts. An immobilized cobalt phthalocyanine (CoPc) molecular catalyst has emerged as promising electrocatalyst for CH3OH synthesis, demonstrating decent activity and selectivity through CO2–CO–CH3OH cascade reaction. However, CoPc's performance limited by its weak binding strength toward the CO intermediate. Recent advancements in modification aimed at enhancing intermediate have shown great promise improving CO2-to-CH3OH performance. In this Perspective, we discuss competitive mechanism between that hinders formation summarize effective strategies can enhance both conversion activity. Finally, offer future perspectives on optimization inspire further research efforts fully unlock potential synthesis via CO2RR using catalysts.

Language: Английский

Citations

3
Molecular Engineering of Poly(Ionic Liquid) for Direct and Continuous Production of Pure Formic Acid from Flue Gas DOI
Geng Li, Chengyi Zhang, Yong Liu

et al.

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

Published: Sept. 30, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) offers a promising approach to close the carbon cycle and reduce reliance on fossil fuels. However, traditional decoupled RR processes involve energy‐intensive capture, conversion, product separation, which increases operational costs. Here, we report development of bismuth‐poly(ionic liquid) (Bi‐PIL) hybrid catalyst that exhibits exceptional electrocatalytic performance for conversion formate. The Bi‐PIL achieves over 90% Faradaic efficiency formate wide potential range, even at low 15% v/v concentrations typical industrial flue gas. biphenyl in PIL backbone affords hydrophobicity while maintaining high ionic conductivity, effectively mitigating flooding issues. layer plays crucial role as concentrator co‐catalyst accelerates kinetics. Furthermore, demonstrate catalysts solid‐state electrolyte (SSE) electrolyzer continuous direct production pure formic acid solutions from Techno‐economic analysis suggests this integrated process can produce significantly reduced cost compared approaches. This work presents strategy overcome challenges associated with low‐concentration utilization streamline valuable liquid fuels chemicals .

Language: Английский

Citations

3