Enhancing H₂O₂ Electrosynthesis at Industrial-Relevant Current in Acidic Media on Diatomic Cobalt Sites

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(13), P. 9434 - 9443

Published: March 20, 2024

Electrocatalytic synthesis of hydrogen peroxide (H2O2) in acidic media is an efficient and eco-friendly approach to produce inherently stable H2O2, but limited by the lack selective catalysts under industrial-relevant current densities. Herein, we report a diatomic cobalt catalyst for two-electron oxygen reduction efficiently H2O2 at 50–400 mA cm–2 acid. Electrode kinetics study shows >95% selectivity on sites. In flow cell device, record-high production rate 11.72 mol gcat–1 h–1 exceptional long-term stability (100 h) are realized high situ spectroscopic studies theoretical calculations reveal that introducing second metal into coordination sphere site can optimize binding strength key intermediates due downshifted d-band center cobalt. We also demonstrate feasibility processing municipal plastic wastes through decentralized production.

Language: Английский

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Grain boundary engineering: An emerging pathway toward efficient electrocatalysis

InfoMat, Journal Year: 2024, Volume and Issue: 6(8)

Published: July 16, 2024

Abstract Electrochemical transformation processes involving carbon, hydrogen, oxygen, nitrogen, and small‐molecule chemistries represent a promising means to store renewable energy sources in the form of chemical energy. However, their widespread deployment is hindered by lack efficient, selective, durable, affordable electrocatalysts. Recently, grain boundary (GB) engineering as one category defect engineering, has emerged viable powerful pathway achieve improved electrocatalytic performances. This review presents timely comprehensive overview recent advances GB for efficient electrocatalysis. The beneficial effects introducing GBs into electrocatalysts are discussed, followed an synthesis characterization GB‐enriched Importantly, latest developments leveraging enhanced electrocatalysis thoroughly examined, focusing on electrochemical utilization cycles nitrogen. Future research directions proposed further advance understanding application image

Language: Английский

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Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

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Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis

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

Published: Aug. 21, 2024

The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption near-site compensation" strategy to reform the bonding network via deliberate cation penetration catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic high-curvature carbon nanocages (RuNi/NC). Theoretical simulations suggest that tip-induced localized concentration hydrated K+ facilitates optimization dynamics intermediate adsorption. In situ synchrotron X-ray spectroscopy endorses H* spillover-bridged Volmer‒Tafel mechanism synergistically relayed between Ru Ni. Consequently, RuNi/NC exhibits low overpotential 12 mV high durability 1600 h at 10 mA cm‒2 HER, demonstrates performance in both electrolysis chlor-alkali electrolysis. offers microscopic perspective design manipulation local structure toward enhanced HER kinetics. A with optimized H2 reported. designed shows catalytic by achieving 13.6-fold higher mass than Pt/C.

Language: Английский

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Anode‐Electrolyte Interfacial Acidity Regulation Enhances Electrocatalytic Performances of Alcohol Oxidations

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: July 8, 2024

The local acidity at the anode surface during electrolysis is apparently stronger than that in bulk electrolyte due to deprotonation from reactant, which leads deteriorated electrocatalytic performances and product distributions. Here, an anode-electrolyte interfacial regulation strategy has been proposed inhibit acidification of enhance activity selectivity anodic reactions. As a proof concept, CeO

Language: Английский

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Rational design of local microenvironment for electrocatalytic water splitting

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(14), P. 4080 - 4106

Published: Jan. 1, 2024

This summary describes the effects of wettability, local pH, interfacial water structure, and electrolyte composition on interface reactant compositions, key intermediate adsorption, reaction kinetics.

Language: Английский

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Insights into the pH effect on hydrogen electrocatalysis

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This review systematically provides various insights into the pH effect on hydrogen electrocatalysis, and thus providing a reference for future development of electrocatalysis based these insights.

Language: Английский

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Structural Engineering and Operando Characterization of Advanced Catalysts for Electrochemical Nitrogen Reduction Reaction

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110693 - 110693

Published: Jan. 1, 2025

Language: Английский

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The breakthrough of oxide pathway mechanism in stability and scaling relationship for water oxidation

National Science Review, Journal Year: 2024, Volume and Issue: 11(11)

Published: Oct. 15, 2024

ABSTRACT An in-depth understanding of electrocatalytic mechanisms is essential for advancing electrocatalysts the oxygen evolution reaction (OER). The emerging oxide pathway mechanism (OPM) streamlines direct O–O radical coupling, circumventing formation vacancy defects featured in lattice (LOM) and bypassing additional intermediates (*OOH) inherent to adsorbate (AEM). With only *O *OH as intermediates, OPM-driven stand out their ability disrupt traditional scaling relationships while ensuring stability. This review compiles latest significant advances OPM-based electrocatalysis, detailing design principles, synthetic methods, sophisticated techniques identify active sites pathways. We conclude with prospective challenges opportunities electrocatalysts, aiming advance field into a new era by overcoming constraints.

Language: Английский

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Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(20), P. 11348 - 11434

Published: Oct. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Language: Английский

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