Tailoring CO₂ Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.

Язык: Английский

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Recent strategies to improve the electroactivity of metal–organic frameworks for advanced electrocatalysis

Deleted Journal, Год журнала: 2024, Номер 1(2), С. 181 - 206

Опубликована: Авг. 4, 2024

Abstract Metal–organic frameworks (MOFs) have emerged as promising materials in the realm of electrocatalysis due to their high surface area, tunable porosity, and versatile chemical functionality. However, practical application has been hampered by inherent limitations such low electrical conductivity a limited number active metal sites. Researchers addressed these challenges through various strategies, including enhancing incorporating conductive nanoparticles, modifying structure composition MOFs replacing nodes functionalizing linkers, preparing catalysts thermal processes decarburization conversion into oxides, phosphides (MPs), sulfides (MSs). This review provided comprehensive summary strategies that were employed enhance electroactivity for improved electrocatalytic performance recent years. It also explored future directions potential innovations design synthesis MOF‐based electrocatalysts, offering valuable insights advancing sustainable energy technologies.

Язык: Английский

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Bamboo-like amorphous Ni(OH)2 nanotubes wrapped Cu nanoparticles with a confined geometry for CO2 electroreduction to ethane in a flow cell

Science China Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Язык: Английский

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Highly Selective CO2 Electroreduction to Multi‐carbon Alcohols via Amine Modified Copper Nanoparticles at Acidic Conditions

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(49)

Опубликована: Авг. 13, 2024

Abstract Electroreduction of CO 2 into multi‐carbon (C2+) products (e.g. C2+ alcohols) offers a promising way for utilization. Use strong alkaline electrolytes is favorable to producing products. However, can react with hydroxide form carbonate/bicarbonate, which results in low carbon utilization efficiency and poor stability. Using acidic electrolyte an efficient solve the problems, but it challenge achieve high selectivity Here we report that amine modified copper nanoparticles exhibit at condition. The Faradaic (FE) reach up 81.8 % media (pH=2) total current density 410 mA cm −2 over n‐butylamine Cu. Especially FE alcohols 52.6 %, higher than those reported electroreduction In addition, single‐pass towards production 60 %. Detailed studies demonstrate molecule on surface Cu cannot only enhance formation, adsorption coverage *CO, also provide hydrophobic environment, result

Язык: Английский

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Accelerated Solar-Driven Polyolefin Degradation via Self-Activated Hydroxy-Rich ZnIn₂S₄

Nano Letters, Год журнала: 2024, Номер 24(37), С. 11624 - 11631

Опубликована: Сен. 3, 2024

Degradation of polyolefin (PE) plastic by a traditional chemical method requires high pressure and temperature but generates complex products. Here, sulfur vacancy-rich ZnIn

Язык: Английский

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Solid Electrolytes for Low-Temperature Carbon Dioxide Valorization: A Review

Environmental Science & Technology, Год журнала: 2024, Номер 58(25), С. 10881 - 10896

Опубликована: Июнь 11, 2024

One of the most promising approaches to address global challenge climate change is electrochemical carbon capture and utilization. Solid electrolytes can play a crucial role in establishing chemical-free pathway for CO2. Furthermore, they be applied electrocatalytic CO2 reduction reactions (CO2RR) increase utilization, produce high-purity liquid chemicals, advance hybrid electro-biosystems. This review article begins by covering fundamentals processes capture, emphasizing advantages utilizing solid electrolytes. Additionally, it highlights recent advancements use polymer electrolyte or layer CO2RR with multiple functions. The also explores avenues future research fully harness potential electrolytes, including integration performance assessment under realistic conditions. Finally, this discusses opportunities challenges, aiming contribute establishment green sustainable society through valorization.

Язык: Английский

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Adjustable Selectivity for CO₂ Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 10, 2025

Abstract Enhancing the selectivity of C 2 products and revealing reaction mechanisms in CO electroreduction (CO RR) remain challenging. Regulating interphases catalysts is one most promising pathways. Herein, between copper (Cu) tin (Sn) oxides are regulated by controlling degree reduction during self‐assembly process, which exhibits obvious different to ethylene ethanol, respectively. The interphase Cu‐SnO ethanol as high 74.6%, while Cu O‐SnO shows 71.4% at –0.6 V versus RHE. In situ Fourier‐transform infrared spectroscopy measurements density functional theory calculations demonstrate that strong electron interaction, preferentially forming key *COH intermediates for asymmetrical C─C coupling produce ethanol. contrast, possesses oxygen vacancies both sites, thus enriching *CO symmetrical interphase. findings this work offer an advanced strategy regulating adjust RR.

Язык: Английский

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Progress in Cu‐Based Catalyst Design for Sustained Electrocatalytic CO₂ to C₂₊ Conversion

Advanced Science, Год журнала: 2025, Номер unknown

Опубликована: Фев. 27, 2025

Abstract The electrocatalytic conversion of CO 2 into valuable multi‐carbon (C 2+ ) products using Cu‐based catalysts has attracted significant attention. This review provides a comprehensive overview recent advances in catalyst design to improve C selectivity and operational stability. It begins with an analysis the fundamental reaction pathways for formation, encompassing both established emerging mechanisms, which offer critical insights design. In situ techniques, essential validating these by real‐time observation intermediates material evolution, are also introduced. A key focus this is placed on how enhance through manipulation, particularly emphasizing catalytic site construction promote C─C coupling via increasing * coverage optimizing protonation. Additionally, challenge maintaining activity under conditions discussed, highlighting reduction active charged Cu species materials reconstruction as major obstacles. To address these, describes strategies preserve sites control including novel utilization mitigation reconstruction. By presenting developments challenges ahead, aims guide future conversion.

Язык: Английский

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Tandem design on electrocatalysts and reactors for electrochemical CO2 reduction

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2025, Номер 69, С. 1 - 16

Опубликована: Фев. 1, 2025

Язык: Английский

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Selective Electrochemical Reduction of CO₂ to Ethanol on a Heteroatom-Coordinated Dual-Atom Catalyst of Fe/Cu-NC

Chemistry of Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 19, 2025

Язык: Английский

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