Toward Electrocatalytic Methanol Oxidation Reaction: Longstanding Debates and Emerging Catalysts

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: Jan. 27, 2023

The study of direct methanol fuel cells (DMFCs) has lasted around 70 years, since the first investigation in early 1950s. Though enormous effort been devoted this field, it is still far from commercialization. oxidation reaction (MOR), as a semi-reaction DMFCs, bottleneck that restricts overall performance DMFCs. To date, there intense debate on complex six-electron reaction, but barely any reviews have systematically discussed topic. end, controversies and progress regarding electrocatalytic mechanisms, evaluations well design science toward MOR electrocatalysts are summarized. This review also provides comprehensive introduction recent development emerging with focus innovation alloy, core-shell structure, heterostructure, single-atom catalysts. Finally, perspectives future outlook mechanisms provided.

Language: Английский

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Co-catalytic metal–support interactions in single-atom electrocatalysts

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

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Recent progress of metal single-atom catalysts for energy applications

Nano Energy, Journal Year: 2023, Volume and Issue: 111, P. 108404 - 108404

Published: April 5, 2023

Language: Английский

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Stability Issues in Electrochemical CO₂ Reduction: Recent Advances in Fundamental Understanding and Design Strategies

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(51)

Published: Aug. 11, 2023

Electrochemical CO2 reduction reaction (CO2 RR) offers a promising approach to close the anthropogenic carbon cycle and store intermittent renewable energy in fuels or chemicals. On path commercializing this technology, achieving long-term operation stability is central requirement but still confronts challenges. This motivates organize present review systematically discuss issue of RR. starts from fundamental understanding on destabilization mechanisms RR, with focus degradation electrocatalyst change microenvironment during continuous electrolysis. Subsequently, recent efforts catalyst design stabilize active sites are summarized, where increasing atomic binding strength resist surface reconstruction highlighted. Next, optimization electrolysis system enhance by maintaining especially mitigating flooding carbonate problems demonstrated. The manipulation conditions also enables prolong RR lifespan through recovering catalytically mass transport process. finally ends up indicating challenges future opportunities.

Language: Английский

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Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

JACS Au, Journal Year: 2023, Volume and Issue: 3(3), P. 736 - 755

Published: Feb. 16, 2023

Single-atom catalysts (SACs) are emerging as the most promising for various electrochemical reactions. The isolated dispersion of metal atoms enables high density active sites, and simplified structure makes them ideal model systems to study structure–performance relationships. However, activity SACs is still insufficient, stability usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, catalytic mechanism on a single site unclear, leading development rely trial-and-error experiments. How can one break current bottleneck sites density? further increase activity/stability sites? In this Perspective, we discuss underlying reasons challenges identify precisely controlled synthesis involving designed precursors innovative heat-treatment techniques key high-performance SACs. addition, advanced operando characterizations theoretical simulations essential uncovering true electrocatalytic an site. Finally, future directions that may arise breakthroughs discussed.

Language: Английский

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Renewable energy driven electroreduction nitrate to ammonia and in-situ ammonia recovery via a flow-through coupled device

Water Research, Journal Year: 2023, Volume and Issue: 242, P. 120256 - 120256

Published: June 20, 2023

Language: Английский

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Porous Organic Polymers‐Based Single‐Atom Catalysts for Sustainable Energy‐Related Electrocatalysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(28)

Published: June 8, 2023

Abstract Single‐atom catalysts (SACs) have been emerging as attractive catalytic materials in electrocatalysis for sustainable energy storage and conversion. To realize the practical implementation of SACs, reliable support is highly imperative to stabilize atomically dispersed metals with strong metal–support interaction, tunable local electronic environment, favorable electron/mass transport. Thanks great designability tunability composition, structure, morphology, porous organic polymers (POPs) demonstrated grand promise appropriate platforms toward design SACs at molecular level fabrication a controlled manner. Herein, comprehensive overview recent advances elucidation general principles, effective synthesis approaches, fundamental mechanisms boosting development high‐performance POPs‐based electrocatalytic transformations provided. The authors first outline rationales using supports principles electrocatalysis, followed by discussing approaches utilizing POPs POPs‐derived nanocarbons host single‐atom metals. Then, state‐of‐the‐art their applications heterogeneous (ORR, OER, HER, CO 2 RR, NRR) are discussed, which focus on revealing structure–performance correlation mechanisms. Finally, challenges strategies associated rational suggested.

Language: Английский

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Efficient strategies for promoting the electrochemical reduction of CO2 to C2+ products over Cu-based catalysts

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2023, Volume and Issue: 48, P. 32 - 65

Published: May 1, 2023

Language: Английский

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Potential and electric double-layer effect in electrocatalytic urea synthesis

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 6, 2024

Abstract Electrochemical synthesis is a promising way for sustainable urea production, yet the exact mechanism has not been fully revealed. Herein, we explore of electrochemical coupling nitrite and carbon dioxide on Cu surfaces towards basis constant-potential method combined with an implicit solvent model. The working electrode potential, which normally overlooked, found influential both reaction activity. further computational study pathways reveals that *CO-NH *NH-CO-NH as key intermediates. In addition, through analysis turnover frequencies under various potentials, pressures, temperatures within microkinetic model, demonstrate activity increases temperature, Cu(100) shows highest efficiency among all three surfaces. electric double-layer capacitance also plays role in synthesis. Based these findings, propose two essential strategies to promote electrodes: increasing surface ratio elevating temperature.

Language: Английский

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Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Dec. 14, 2023

Abstract Understanding the structure-stability relationship of catalysts is imperative for development high-performance electrocatalytic devices. Herein, we utilize operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to quantitatively monitor evolution Cu single-atom (SACs) during electrochemical reduction CO 2 (CO RR). SACs are converted into 2-nm nanoparticles through a reconstruction process RR. The rate highly dependent on substrates due coordination difference. Density functional theory calculations demonstrate that stability their formation energy, which can be manipulated by controlling affinity between sites and substrates. This work highlights use ATR-SEIRAS achieve mechanistic understanding long-term applications.

Language: Английский

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