Steering the Site Distance of Atomic Cu‐Cu Pairs by First‐Shell Halogen Coordination Boosts CO2‐to‐C2 Selectivity

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(46)

Опубликована: Авг. 6, 2024

Electrocatalytic reduction of CO

Язык: Английский

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Modulating the Electronic Properties of Single Ni Atom Catalyst via First‐Shell Coordination Engineering to Boost Electrocatalytic Flue Gas CO₂ Reduction

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract Electrochemical converting CO 2 to via single atom catalyst is an effective strategy for reducing concentration in the atmosphere and achieving a carbon‐neutral cycle. However, relatively low industrial processes large energy barriers activating severely obstruct actual application. Reasonably modulating coordination shell of active center enhance activity catalysts. Herein, well‐designed single‐atom electrocatalyst Ni‐N 3 S 1 developed large‐scale synthesis strategy. The constructed S‐C exhibits superior catalytic than 4 ‐C conversion H‐type cells, industrial‐level current density with excellent durability at wide pH range can be achieved gas‐diffusion flow cells. Experimental results functional theory (DFT) calculation demonstrate that introducing electronegative significantly regulate electronic structure site, promoting adsorption capacity decreasing barrier *COOH formation, thus larger size flexibility sulfur mitigate nickel agglomeration stability catalyst. This work provides designing highly catalysts electrocatalysis reactive sites.

Язык: Английский

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Selective CO₂ Reduction over γ-Graphyne Supported Single-Atom Catalysts: Crucial Role of Strain Regulation

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(34), С. 24133 - 24140

Опубликована: Авг. 14, 2024

The two-electron CO

Язык: Английский

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Machine Learning Big Data Set Analysis Reveals C–C Electro-Coupling Mechanism

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(32), С. 22850 - 22858

Опубликована: Авг. 3, 2024

Carbon-carbon (C-C) coupling is essential in the electrocatalytic reduction of CO

Язык: Английский

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A Review on Single Site Catalysts for Electrochemical CO₂ Reduction

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 18, 2025

Abstract Single site catalysts (SSCs), characterized by high atomic utilization and well‐defined active sites, exhibit significant potential in the field of CO 2 electroreduction (CO RR). Typically, SSCs tend to a 2‐electron transfer reaction RR, there remain challenges achieving efficient conversion above 2‐electrons (methane (CH 4 ) multicarbon products(C 2+ ). Therefore, systematic review is crucial summarize recent advancements single electrocatalysts their structure‐activity relationship. The discussion begins with state‐of‐the‐art characterization techniques SSCs. Then influence central atoms, coordination environments, support metal‐support interactions on catalytic performance discussed detail. Subsequently, regulation strategies improve activity selectivity CH C products are discussed. Furthermore, dynamic evolution metal sites true nature during RR also addressed. Finally, associated for product formation analyzed.

Язык: Английский

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Switching CO-to-Acetate Electroreduction on Cu Atomic Ensembles

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Дек. 17, 2024

The electrocatalytic reaction pathway is highly dependent on the intrinsic structure of catalyst. CO2/CO electroreduction has recently emerged as a potential approach for obtaining C2+ products, but it challenging to achieve high selectivity single product. Herein, we develop Cu atomic ensemble that satisfies appropriate site distance and coordination environment required CO-to-acetate conversion, which shows outstanding overall performance with an acetate Faradaic efficiency 70.2% partial current density 225 mA cm–2 formation rate 2.1 mmol h–1 cm–2. Moreover, single-pass CO conversion 91% remarkable stability can be also obtained. Detailed experimental theoretical investigations confirm significant advantages ensembles in optimizing C–C coupling, stabilizing key ketene intermediate (*CCO), inhibiting *HOCCOH intermediate, switch reduction from ethanol/ethylene conventional metallic ensembles.

Язык: Английский

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Strategies for Improving Product Selectivity in Electrocatalytic Carbon Dioxide Reduction Using Copper‐Based Catalysts

Advanced Functional Materials, Год журнала: 2024, Номер 34(51)

Опубликована: Авг. 29, 2024

Abstract As an effective approach to converting carbon oxide (CO 2 ) into value‐added carbonaceous products, the electrochemical CO reduction reaction (ECO RR) has shown considerable potential for neutrality, addressing global pollution and climate issues. Copper (Cu)‐based electrocatalysts (CuECs) are acknowledged as important candidates ECO RR of multi‐carbon products. Nevertheless, complicated electron transfer multiple competitive pathways in production process raise challenges product selectivity. While achieving high current density structural stability, improving selectivity CuECs become crucial their practical applications. Herein, overview fundamental thermodynamic kinetic principles presented. Then, typical strategies summarized increasing CuEC formation products from , including morphological control, component design, defect interface design. The catalyst catalytic performance, mechanisms involved these reviewed. Finally, major future prospects high‐performance discussed.

Язык: Английский

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Understanding the CO₂ Reduction Selectivity toward Ethanol on Single Atom Doped Cu/Cu₂O Catalysts: Insights from Bader Charge as a Descriptor

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 963 - 968

Опубликована: Янв. 21, 2025

In the CO2 reduction reactions (CO2RR), product selectivity is strongly dependent on binding energy differences of key intermediates. Herein, we systematically evaluated CO2RR reaction pathways single transition metal atom doped catalysts TM1Cu/Cu2O by density functional theory (DFT) methods and found that *CO more likely to undergo C-O bond cleavage rather than be hydrogenated (TM = Sc, Ti, V, Cr, Mn, Fe, Co), which facilitates C2+ production with a low-energy pathway OC-C coupling, while it prefers form CHO Ni, Cu). The defects Cu in were confirmed enhance ethanol. Furthermore, established scaling relationship between free energies intermediates Bader charges active sites TM defective surfaces. This rational efficient design Cu/Cu2O-based catalysts.

Язык: Английский

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Electrochemical CO₂ Reduction on SnO: Insights into C₁ Product Dynamic Distribution and Reaction Mechanisms

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3173 - 3183

Опубликована: Фев. 6, 2025

The precise synthesis of desirable products from the electrochemical CO2 reduction reaction (CO2RR) remains challenging, primarily due to unclear structure–activity relationships under in situ conditions. Recognized by their cost-effectiveness and nontoxic nature, Sn-based materials are extensively utilized CO2RR produce valuable chemicals. Notably, our large-scale data mining experimental literature reveals a significant trend: SnO2-based electrocatalysts generate HCOOH, while SnO-based counterparts demonstrate ability both HCOOH CO comparable quantities. Furthermore, findings indicate that SnO underexplored terms its surface speciation for compared materials. Addressing these issues is crucial field electrocatalysis, as understanding them will not only clarify why uniquely influences distribution C1 but also provide insights into how precisely control electrocatalytic processes targeted product synthesis. Herein, we employed constant-potential method combined with coverage reconstruction analyses simulate energetics intermediates elucidate dynamic on resting typical Our analysis effectively identifies active involved CO2RR. comparative simulations between pristine reconstructed surfaces reveal electrochemistry-induced oxygen vacancies direct distribution. By addressing critical issues, aim advance electrocatalysis contribute chemical production CO2, stimulating future exploration conditions other systems.

Язык: Английский

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Reaction-Driven Varieties of Active Sites on Cu(100) in Electrochemical CO₂ Reduction Reaction

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 6497 - 6506

Опубликована: Апрель 6, 2025

Язык: Английский

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