Atomically Dispersed Cu Active Centers: Local Structure and Mechanism Modulation for Carbon Dioxide Reduction

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

Published: Jan. 10, 2025

Abstract Reducing carbon dioxide （CO 2 ）to high‐value products using green renewable energy is a promising approach for addressing and greenhouse effect issues. Consequently, electrocatalytic CO reduction reaction (CO RR) technology has become current research hotspot. Since the discovery of high activity selectivity copper in RR, atomically dispersed Cu catalysts have garnered widespread attention due to their efficient atom utilization, unique electronic structure, outstanding catalytic performance. However, great challenge remains providing rational catalyst design principles achieve regulation product distribution. A clear understanding materials an in‐depth interpretation mechanism as well elucidation strategy progress toward different are keys building solving above problem. Therefore, this review starts with introduction advanced characterization techniques reveal structure mechanisms. Then, various optimization strategies applications producing targeted summarized discussed. Finally, perspectives on RR field future development offered.

Language: Английский

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Tunable CO₂ Electroreduction to CO with a Controllable Interfacial Microenvironment

Energy & Fuels, Journal Year: 2025, Volume and Issue: 39(6), P. 3169 - 3175

Published: Jan. 31, 2025

The electrochemical reduction of carbon dioxide to value-added chemicals using renewable energy sources represents a promising approach for implementing an artificial cycle. However, with the advancement high-performance catalysts, reaction microenvironment gas diffusion electrodes (GDEs) has become critical factor affecting performance CO2 CO. It is essential understand and control surrounding catalytic sites as it can mediate transport reactants influence pathways. This paper describes design realization controllable interfacial GDEs by spraying Ag nanoparticles hydrophobic polytetrafluoroethylene (PTFE) nanoparticle mixture onto paper. Experimental characterization results reveal that mass H2O related wettability, which be regulated PTFE. Through modulating property interface, hydrogen evolution was effectively inhibited, Faradaic efficiencies (FEs) partial current densities CO were significantly improved. A FE 98% achieved high density 450 mA/cm2, shows potential industrial application.

Language: Английский

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Reconstructed rich oxygen defects and Ag0 on Pr6O11 surface through interface-defect engineering for enhanced electrochemical carbon dioxide reduction

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown, P. 137368 - 137368

Published: March 1, 2025

Language: Английский

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Theoretical simulations inspired the design of Ni nanoparticles-NiN4 single atom composites for efficient CO2 electro-reduction at ultralow overpotential

Molecular Catalysis, Journal Year: 2025, Volume and Issue: 580, P. 115125 - 115125

Published: April 19, 2025

Language: Английский

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Enhanced CO₂ Electroreduction by Stabilizing ^*COOH on Ni Single Atoms via Short‐ and Long‐Range Electronic Modulation

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

Published: April 24, 2025

Abstract Ni single‐atoms (SAs) are active for electrocatalytic CO 2 reduction reaction (CO RR) to CO, but their performance still needs be further improved practical implementation. Herein, a strategy of “short‐ and long‐range modulation” is reported synergistically modulate the electronic structure SAs by constructing nanoparticles (NPs) integrated with N, P‐coordinated on N‐doped carbon supports (Ni‐P 1 N 3 /Ni NPs @NC). Experiments theoretical calculations reveal that both short‐range modulation involving Ni–P coordination collectively enhance electron localization around SAs, thus increasing binding strength key * COOH intermediate. This results in an RR lowering energy barrier. Ni‐P @NC exhibits Faradaic efficiency exceeding 99.0% across wide potential range from −0.5 −1.1 V versus reversible hydrogen electrode (vs RHE), highest partial current density −544 mA cm −2 at vs RHE.

Language: Английский

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Continuous Coordination Modulation with Differing Heteroatoms Unveils Favorable Single-atom Ni Sites for Near-unity CO Selectivity in CO2 Electroreduction

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

Published: Jan. 1, 2025

This work explores how heteroatom substitution (C, N, and O) affects the catalytic performance of Ni-based single-atom catalysts for CO 2 electroreduction, attributing observed variations to differing competition between eCO RR HER.

Language: Английский

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Stabilizing *COOH on Ni Single-Atom Sites by Dual-Phase Ni₃ZnC_0.7 and Ni for Enhanced Electrocatalytic CO₂ Reduction

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

Published: May 9, 2025

Metal-based nanoparticle-modulated single-atom catalysts have garnered significant attention in the field of electrocatalytic CO2 reduction reaction. However, scaling relationships between intermediates and their binding energies lead to unsatisfactory selectivity for specific products. Herein, Ni3ZnC0.7-Ni nanoparticles (NPs)-modulated Ni single-atoms (SAs) supported on N-doped carbon (NiSAs/Ni3ZnC0.7-NiNPs@NC) were constructed using a metal-organic framework as template. Experiments theoretical calculations reveal that charge transfer from Ni3ZnC0.7 NPs SAs results formation electron-enriched sites, which is conducive stabilize key *COOH intermediate. The catalyst shows partial current density CO -345 mA cm-2 Faradaic efficiency (FECO) 99.3% at -0.8 V versus reversible hydrogen electrode flow cell. Furthermore, maintains FECO above 94% after continuous electrolysis 18 h, showcasing its remarkable long-term stability.

Language: Английский

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Surmounting scaling relationship on Cu-base diatomic catalysts by geminal-site-induced synergistic effect for high-selectivity CO2 electrochemical reduction to CO

Materials Today Energy, Journal Year: 2024, Volume and Issue: 46, P. 101731 - 101731

Published: Nov. 1, 2024

Language: Английский

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Coupling In nanoclusters and Bi nanoparticles in nitrogen-doped carbon for enhanced CO2 electroreduction to HCOOH

Journal of Electroanalytical Chemistry, Journal Year: 2024, Volume and Issue: 974, P. 118711 - 118711

Published: Oct. 11, 2024

Language: Английский

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