Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Cation Modifies Interfacial Water Structures on Platinum during Alkaline Hydrogen Electrocatalysis

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(4), С. 2426 - 2434

Опубликована: Янв. 16, 2024

The molecular details of an electrocatalytic interface play essential role in the production sustainable fuels and value-added chemicals. Many electrochemical reactions exhibit strong cation-dependent activities, but how cations affect reaction kinetics is still elusive. We report effect (K+, Li+, Ba2+) on interfacial water structure using second-harmonic generation (SHG) classical dynamics (MD) simulation. second- (χH2O(2)) third-order (χH2O(3)) optical susceptibilities Pt are smaller presence Ba2+ compared to those K+, suggesting that can orientation. MD simulation reproduces experimental SHG observations further shows competition between cation hydration alignment governs net impact supports a hydration-mediated mechanism for hydrogen electrocatalysis; i.e., occurs via dissociation followed by cation-assisted hydroxide/water exchange Pt. Our study highlights electrocatalysis innocent additives (such as cations) local environment.

Язык: Английский

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Emerging Atomistic Modeling Methods for Heterogeneous Electrocatalysis

Chemical Reviews, Год журнала: 2024, Номер 124(14), С. 8620 - 8656

Опубликована: Июль 11, 2024

Heterogeneous electrocatalysis lies at the center of various technologies that could help enable a sustainable future. However, its complexity makes it challenging to accurately and efficiently model an atomic level. Here, we review emerging atomistic methods simulate electrocatalytic interface with special attention devoted components/effects have been model, such as solvation, electrolyte ions, electrode potential, reaction kinetics, pH. Additionally, relevant computational spectroscopy methods. Then, showcase several examples applying these understand design catalysts green hydrogen. We also offer experimental views on how bridge gap between theory experiments. Finally, provide some perspectives opportunities advance field.

Язык: Английский

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Gold Nanoparticles for CO₂ Electroreduction: An Optimum Defined by Size and Shape

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(3), С. 2015 - 2023

Опубликована: Янв. 9, 2024

Understanding the size-dependent behavior of nanoparticles is crucial for optimizing catalytic performance. We investigate differences in selectivity size-selected gold CO2 electroreduction with sizes ranging from 1.5 to 6.5 nm. Our findings reveal an optimal size approximately 3 nm that maximizes toward CO, exhibiting up 60% Faradaic efficiency at low potentials. High-resolution transmission electron microscopy reveals different shapes particles and suggests multiply twinned are favorable reduction CO. analysis shows twin boundaries pin 8-fold coordinated surface sites turn a variation shape optimize abundance viable path electrocatalytic This work contributes advancement nanocatalyst design achieving tunable conversion into valuable products.

Язык: Английский

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Addressing the Carbonate Issue: Electrocatalysts for Acidic CO₂ Reduction Reaction

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Май 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Язык: Английский

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