Challenges and Opportunities for Single‐Atom Electrocatalysts: From Lab‐Scale Research to Potential Industry‐Level Applications

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 13, 2024

Single-atom electrocatalysts (SACs) are a class of promising materials for driving electrochemical energy conversion reactions due to their intrinsic advantages, including maximum metal utilization, well-defined active structures, and strong interface effects. However, SACs have not reached full commercialization broad industrial applications. This review summarizes recent research achievements in the design crucial electrocatalytic on sites, coordination, substrates, as well synthesis methods. The key challenges facing activity, selectivity, stability, scalability, highlighted. Furthermore, it is pointed out new strategies address these increasing activity enhancing utilization improving optimizing local environment, developing fabrication techniques, leveraging insights from theoretical studies, expanding potential Finally, views offered future direction single-atom electrocatalysis toward commercialization.

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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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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An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Авг. 16, 2024

Industrial 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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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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Sub‐Nanometer Mono‐Layered Metal–Organic Frameworks Nanosheets for Simulated Flue Gas Photoreduction

Advanced Materials, Год журнала: 2024, Номер 36(27)

Опубликована: Апрель 18, 2024

Abstract The dilemma between the thickness and accessible active site triggers design of porous crystalline materials with mono‐layered structure for advanced photo‐catalysis applications. Here, a kind sub‐nanometer nanosheets (Co‐MOF MNSs) through exfoliation specifically designed Co 3 cluster‐based metal–organic frameworks (MOFs) is reported. inherent light‐sensitivity endow Co‐MOF MNSs fully exposed Janus sites that can selectively photo‐reduce CO 2 into formic acid under simulated flue gas. Notably, production efficiency by (0.85 mmol g −1 h ) ≈13 times higher than bulk counterpart (0.065 gas atmosphere, which highest in reported works up to date. Theoretical calculations prove simultaneously available possess activity when compared single site, validating importance nanosheet morphology. These results may facilitate development functional photo‐reduction potential treatment.

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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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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Tailoring microenvironment for efficient CO2 electroreduction through nanoconfinement strategy

Nano Research, Год журнала: 2024, Номер 17(9), С. 7880 - 7899

Опубликована: Авг. 7, 2024

Язык: Английский

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