Electrochemical CO₂ Reduction in Acidic Media: A Perspective

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

Опубликована: Март 4, 2025

The electrochemical CO2 reduction reaction (eCO2RR) is a promising approach for converting to useful chemicals and, hence, achieving carbon neutrality. Though high selectivity and activity of products have been achieved recently, all are reported in neutral or alkaline electrolytes. Although these electrolyte media give activity, they face the major challenge low utilization because carbonate formation, which lowers overall efficiency process. Conducting eCO2RR acidic can help overcome issue formation hence increase efficiency. However, there many challenges associated with eCO2RR. Two concerns highly competitive hydrogen evolution salt precipitation issues. This Perspective focuses on fundamentals eCO2RR, recent catalyst development strategies, relevant problems that need be addressed future. In end, we provide future outlook will an idea about focus field

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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Revisiting Factors Controlling the Electrochemical CO₂ Reduction to CO and HCOOH on Transition Metals with Grand Canonical Density Functional Theory Calculations

ACS Catalysis, Год журнала: 2024, Номер 14(11), С. 8549 - 8560

Опубликована: Май 17, 2024

The design of highly selective catalysts to form a single product represents one the biggest challenges in electrochemical carbon dioxide reduction reactions (eCO2RR). However, controversial and simplified mechanistic studies hinder proposal effective principles guiding rational catalyst design. Herein, by using grand canonical density functional theory (GC-DFT) calculations hybrid solvent model, we revisited reaction mechanism two-electron eCO2RR on group transition metals with an emphasis illustrating why gold favors CO while Indium HCOOH. We identified potential difference (Ud) between onset for stable ∧-shaped *CO2– formation (U∧-CO2) zero charge system (UPZC–CO2) as crucial indicator HCOOH production, representing good addition criteria via binding strength comparison *COOH HCOO* species. Our results not only deepen understanding process at different potentials but also provide guidance produce selectively.

Язык: Английский

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Stabilized High‐Valent Indium for Promoted Formate Production from Electrochemical CO₂ Reduction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 5, 2024

Abstract Electrocatalysts based on high‐valent indium are promising for formate production via CO 2 electroreduction. However, reconstruction often occurs during the reaction progress, resulting in a decline catalytic performance. Here, composite of In O 3 /In S is developed, and its performance exceeds that either individual phase, particularly stability. Analysis morphology, valence state, situ Raman spectroscopy reveals well preserved reaction. Theoretical calculations suggest desorption energy lattice oxygen can be strengthened due to ‐In bonding within composite. This reinforcement facilitates formation more active sites promotes adsorption, further decreasing barrier only 0.12 eV. As result, exhibits selectivity over 95.05% at –1.13 V vs reversible hydrogen electrode accompanied by partial current density 434.4 mA cm –2 . Notably, maintains 95% even after 50 h an industrial‐level 200 , 17 times longer than phase. Furthermore, 18.33% solar‐to‐formate 19.49% solar‐to‐fuel obtained when coupled with III‐V solar cells, demonstrating feasibility.

Язык: Английский

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Boosting Formate Production in Electrocatalytic CO₂ Reduction on Bimetallic Catalysts Enriched with In–Zn Interfaces

ACS Nano, Год журнала: 2024, Номер 18(52), С. 35749 - 35757

Опубликована: Дек. 18, 2024

We present an effective strategy for developing the dispersing strong-binding metal In on surface of weak-binding Zn, which modulates binding energy reaction intermediates and further facilitates efficient conversion CO2 to formate. The In-Zn interface (In-Zn2) benefits from formation active sites through favorable orbital interactions, leading a Faradaic efficiency 82.7% formate partial current density 12.39 mA cm-2, along with stable performance over 15 h at -1.0 V versus reversible hydrogen electrode. Both in situ Fourier transform infrared spectroscopy functional theory calculations show that bimetallic catalyst can deliver superior *OCHO intermediate, thereby fundamentally accelerating addition, exposed promotes capture activation molecules dynamics within significantly reduce barrier associated generation HCOO-, thus augmenting selectivity catalytic activity generation.

Язык: Английский

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Mesostructure‐Specific Configuration of *CO Adsorption for Selective CO₂ Electroreduction to C₂₊ Products

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(1)

Опубликована: Сен. 2, 2024

The multi-carbon (C2+) alcohols produced by electrochemical CO2 reduction, such as ethanol and n-propanol, are considered indispensable liquid energy carriers. In most C-C coupling cases, however, the concomitant gaseous C2H4 product results in low selectivity of C2+ alcohols. Here, we report rational construction mesostructured CuO electrocatalysts, specifically mesoporous (m-CuO) cylindrical (c-CuO), enables selective distribution products. m-CuO c-CuO show similar towards total products (≥76 %), but corresponding predominant (55 %) (52 respectively. ordered mesostructure not only induces surface hydrophobicity, selectively tailors adsorption configuration *CO intermediate: prefers bridged adsorption, whereas favors top revealed situ spectroscopies. Computational calculations unravel that adsorbate is prone to deep protonation into *OCH3 intermediate, thus accelerating intermediates generate alcohols; contrast, apt undergo conventional process produce C2H4. This work illustrates via manipulation, paves a new path design efficient electrocatalysts with tunable key for targeted

Язык: Английский

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A review of carbon-supported single-atom catalysts for electrochemical reactions

New Carbon Materials, Год журнала: 2024, Номер 39(3), С. 407 - 438

Опубликована: Июнь 1, 2024

Язык: Английский

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Regulating p-orbital electronic configuration of In2O3 by thickness-controlled carbon layer for efficient electrocatalytic CO2 reduction to HCOOH

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер unknown, С. 124596 - 124596

Опубликована: Сен. 1, 2024

Язык: Английский

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Plasmon‐Driven Highly Selective CO2 Photoreduction to C2H4 on Ionic Liquid‐Mediated Copper Nanowires

Angewandte Chemie, Год журнала: 2024, Номер 136(42)

Опубликована: Июль 20, 2024

Abstract Selective CO 2 photoreduction to value‐added multi‐carbon (C 2+ ) feedstocks, such as C H 4 , holds great promise in direct solar‐to‐chemical conversion for a carbon‐neutral future. Nevertheless, the performance is largely inhibited by high energy barrier of C−C coupling process, thereby leading products with low selectivity. Here we report that through facile surface immobilization 1‐ethyl‐3‐methylimidazolium tetrafluoroborate (EMIM‐BF ionic liquid, plasmonic Cu nanowires could enable highly selective product. At an optimal condition, resultant photocatalyst exhibits production selectivity up 96.7 % under 450 nm monochromatic light irradiation, greatly surpassing its pristine counterpart. Combined situ spectroscopies and computational calculations unravel addition EMIM‐BF liquid modulates local electronic structure Cu, resulting enhanced adsorption strength *CO intermediate significantly reduced process. This work paves new path plasmons artificial photosynthesis targeted products.

Язык: Английский

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Rational Strategies for Preparing Highly Efficient Tin‐, Bismuth‐ or Indium Based Electrocatalysts for Electrochemical CO2 Reduction to Formic acid

ChemSusChem, Год журнала: 2024, Номер unknown

Опубликована: Окт. 8, 2024

Electrochemical carbon dioxide reduction reaction (CO

Язык: Английский

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