Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8889 - 8898

Published: May 24, 2024

The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single–atom (SACs) more efficient conversion CO2 to valuable chemicals. However, ligands introduced into dual-atomic sites are expected but still under-explored. In this study, a Fe–Ni pair electrocatalyst with N– and S–coordination in porous carbon nanosheets was conceptually predicted electrocatalytic reduction CO (CO2RR). contrast SACs traditional diatomic (DACs), joined can balance cooperative activities Fe Ni sites, making adsorption configuration bidentate at both sites. This regulation leads substantial change CO* from facilitating desorption boosting CO2RR. Experimental results demonstrate that obtained FeNi–NSC catalyst achieves high selectivity Faradaic efficiencies 96.1%, remarkable activity turnover frequency 6526.9 h–1 −1.0 V, which were over 4.5 2.5 times those single work gives us insight designing highly effective guided by theoretical calculation.

Language: Английский

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Isolated FeN₃ sites anchored hierarchical porous carbon nanoboxes for hydrazine‐assisted rechargeable Zn‐CO₂ batteries with ultralow charge voltage

Carbon Energy, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 8, 2024

Abstract Zn‐CO 2 batteries (ZCBs) are promising for CO conversion and electric energy release. However, the ZCBs couple electrochemical reduction (ECO R) with oxygen evolution reaction competitive hydrogen reaction, which normally causes ultrahigh charge voltage efficiency attenuation, thereby resulting in ~90% total power consumption. Herein, isolated FeN 3 sites encapsulated hierarchical porous carbon nanoboxes (Fe‐HPCN, derived from thermal activation process of ferrocene polydopamine‐coated cubic ZIF‐8) were proposed hydrazine‐assisted rechargeable based on ECO R (discharging process: + 2H → H O) hydrazine oxidation (HzOR, charging N 4 4OH − 4H O 4e ). The endows HzOR a lower overpotential boosts 96% Faraday (FE Benefitting bifunctional catalytic activities, homemade assembled Fe‐HPCN air cathode exhibited an ultralow (decreasing by ~1.84 V), excellent selectivity close to 100%), high 89% efficiency. In situ infrared spectroscopy confirmed that can generate rate‐determining *N *CO intermediates during R. This paper proposes centers R/HzOR performance further presents pioneering achievements ZCBs.

Language: Английский

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A polymerization-mediated confinement strategy to fabricate Fenton-like catalysts with high H2O2 utilization for water decontamination

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: 13(1), P. 115325 - 115325

Published: Jan. 5, 2025

Language: Английский

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Metal–organic frameworks and their derivatives for the electrochemical CO₂ reduction reaction: insights from molecular engineering

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(32), P. 20578 - 20605

Published: Jan. 1, 2024

Molecular engineering of MOF-based electrocatalysts for the CO 2 RR, computational simulations, and advanced characterization studies are discussed summarized to illustrate correlation between their structure performance.

Language: Английский

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Optimization of electronic structure by defect engineering for electrocatalytic carbon dioxide reduction reaction

Inorganic Chemistry Frontiers, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This paper reviews the progress of defective Cu-based materials for eCO 2 RR, highlights design strategy defect structure and emphasizes mechanism site on catalytic behaviors.

Language: Английский

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Bowtie-Shaped Bio-Based Zwitterionic Polymer-Catalyzed Chemical Fixation of Carbon Dioxide

ACS Applied Polymer Materials, Journal Year: 2024, Volume and Issue: 6(17), P. 10906 - 10915

Published: Aug. 21, 2024

Developing green and low-cost catalytic systems is highly desired in the chemical conversion of carbon dioxide into value-added products. A zwitterionic polymer, with a bowknot-like morphology consisting uniform nanosheets, synthesized from biomass-derived cinnamic acid via simple copolymerization strategy. The as-prepared polymer (PEMP) has been employed to catalyze cycloaddition reaction epoxides atmospheric CO2, affording 9 cyclic carbonates good excellent yields under metal-free/solvent-free/cocatalyst-free conditions. PEMP outstanding stability can be reused 5 times at least without an obvious loss activity. mechanism was elaborately investigated by situ Fourier transform infrared spectra tests, control experiments, density functional theory calculations, demonstrating that CO2 over occurs through preactivation epichlorohydrin. Moreover, it illustrated synergistic effect between carbonate anion quaternary ammonium cation on played crucial role promoting activation CO2.

Language: Английский

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