Importing Antibonding‐Orbital Occupancy through Pd−O−Gd Bridge Promotes Electrocatalytic Oxygen Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)

Published: Nov. 9, 2023

The active-site density, intrinsic activity, and durability of Pd-based materials for oxygen reduction reaction (ORR) are critical to their application in industrial energy devices. This work constructs a series carbon-based rare-earth (RE) oxides (Gd2 O3 , Sm2 Eu2 CeO2 ) by using RE metal-organic frameworks tune the ORR performance Pd sites through Pd-REx Oy interface interaction. Taking Pd-Gd2 /C as representative, it is identified that strong coupling between Gd2 induces formation Pd-O-Gd bridge, which triggers charge redistribution . screened exhibits impressive with high onset potential (0.986 VRHE ), half-wave (0.877 excellent stability. Similar results also found Pd-Sm2 /C, Pd-Eu2 Pd-CeO2 catalysts. Theoretical analyses reveal promotes electron transfer antibonding-orbital occupancy Pd-*OH optimization *OH adsorption rate-determining step ORR. pH-dependent microkinetic modeling shows close theoretical optimal activity ORR, outperforming Pt under same conditions. By its ascendancy superior Zn-air battery an air cathode, implying practicability.

Language: Английский

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Lithium-Induced Oxygen Vacancies in MnO₂@MXene for High-Performance Zinc–Air Batteries

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(10), P. 12781 - 12792

Published: Feb. 28, 2024

The traditional methods for creating oxygen vacancies in materials present several challenges and limitations, such as high preparation temperatures, limited vacancy generation, morphological destruction, which hinder the application of transition metal oxides field zinc–air batteries (ZABs). In order to address these we have introduced a pioneering lithium reduction strategy generating δ-MnO2@MXene composite materials. This stands out its simplicity implementation, applicability at room temperature, preservation material's structural integrity. research demonstrates that aqueous Ov-MnO2@MXene-5, with vacancies, exhibits an outstanding reaction (ORR) activity ORR half-wave potential reaching 0.787 V. DFT calculations demonstrated enhanced could be attributed adjustments electronic structure alterations adsorption bond lengths. These result from introduction turn promote electron transport catalytic activity. context batteries, cells Ov-MnO2@MXene-5 air cathode exhibit performance, featuring significantly improved maximum power density (198.3 mW cm–2) long-term cycling stability. Through innovative introducing this study has successfully electrochemical performance MnO2, overcoming limitations associated vacancies. Consequently, opens up new avenues directions nonprecious catalyst ZABs.

Language: Английский

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Design Principles and Mechanistic Understandings of Non-Noble-Metal Bifunctional Electrocatalysts for Zinc–Air Batteries

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: March 26, 2024

Zinc-air batteries (ZABs) are promising energy storage systems because of high theoretical density, safety, low cost, and abundance zinc. However, the slow multi-step reaction oxygen heavy reliance on noble-metal catalysts hinder practical applications ZABs. Therefore, feasible advanced non-noble-metal electrocatalysts for air cathodes need to be identified promote catalytic reaction. In this review, we initially introduced advancement ZABs in past two decades provided an overview key developments field. Then, discussed working mechanism design bifunctional from perspective morphology design, crystal structure tuning, interface strategy, atomic engineering. We also included studies, machine learning, characterization technologies provide a comprehensive understanding structure-performance relationship pathways redox reactions. Finally, challenges prospects related designing

Language: Английский

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Inhibited Passivation by Bioinspired Cell Membrane Zn Interface for Zn–Air Batteries with Extended Temperature Adaptability

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 27, 2024

Abstract Due to the slow dynamics of mass and charge transfer at Zn|electrolyte interface, stable operation Zn–air batteries (ZABs) is challenging, especially low temperature. Herein, inspired by cell membrane, a hydrophilic‐hydrophobic dual modulated interface constructed. This amphiphilic design enables quasi‐solid‐state (QSS) ZABs display long‐term cyclability 180 h@50 mA cm −2 25 °C. Moreover, record‐long time 173 h@4 −60 °C also achieved, which almost threefolds untreated QSS ZABs. Control experiments (in situ) characterization reveal that growth insulating ZnO passivation layers largely inhibited tuned hydrophilic–hydrophobic behavior. Thus, enhanced dynamic Zn 2+ from attained. As an extension, Al‐air (AABs) with bioinspired show unprecedented discharge stability 420 h@1 ‐40 °C, about two times AABs. bioinspired‐hydrophilic‐hydrophobic modulation strategy may provide reference for energy transform storage devices broad temperature adaptability.

Language: Английский

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Engineering the Electronic Interaction Between Single Au Atoms and CoN Through Nitrogen‐Coordination Bonding as an Efficient Bifunctional Electrocatalyst for Rechargeable Zn–Air Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(27)

Published: Feb. 25, 2024

Abstract Single‐atom catalysts hold significance in the field of electrocatalysis. In this study, cobalt nitride (CoN), known for its semiconductor characteristics, is selected as substrate, on which single gold (Au) atoms are loaded, to synthesize catalyst Au SAC CoN@NF with anchored CoN and grown nickel foam. The introduction results an exceptional double‐layer capacitance (1425.7 mF cm −2 ), offers immense possibilities applications zinc–air batteries based CoN@NF. demonstrated remarkable performance metrics, including a power density 161.94 mW , specific capacity 813.80 mAh g −1 cycling stability more than 260 h at 10 mA . addition, these show outstanding round‐trip efficiency 65.1%. Density functional theory calculations reveal that can optimize adsorption energies intermediates oxygen evolution reaction promote transporting electrons OH − species Au–N active site reduction reaction. proposed electronic metal‐support interaction strategy fresh insights designing single‐atom enhance electrocatalysis efficiency, thereby expanding practical application prospects batteries.

Language: Английский

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Engineering Electronic Structure of Nitrogen‐Carbon Sites by sp³‐Hybridized Carbon and Incorporating Chlorine to Boost Oxygen Reduction Activity

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(1)

Published: Nov. 30, 2023

Development of efficient and easy-to-prepare low-cost oxygen reaction electrocatalysts is essential for widespread application rechargeable Zn-air batteries (ZABs). Herein, we mixed NaCl ZIF-8 by simple physical milling pyrolysis to obtain a metal-free porous electrocatalyst doped with Cl (mf-pClNC). The mf-pClNC exhibits good reduction (ORR) activity (E1/2 =0.91 V vs. RHE) high stability in alkaline electrolyte, exceeding most the reported transition metal carbon-based being comparable commercial Pt/C electrocatalysts. Likewise, also shows state-of-the-art ORR acidic electrolyte. From experimental theoretical calculations, better likely originated from fact that introduced promotes increase sp3 -hybridized carbon, while carbon together modify electronic structure N-adjacent carbons, as active sites, molten-salt etching provides abundant paths transport electrons/protons. Furthermore, liquid ZAB using cathode fulfilling performance peak power density 276.88 mW cm-2 . Flexible quasi-solid-state constructed an exciting both at low, room temperatures.

Language: Английский

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Sustainable Energy Resources for Driving Methane Conversion

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(36)

Published: Aug. 13, 2023

Abstract The conversion of methane to value‐added chemicals by traditional reforming processes suffers from intensive energy consumption due its particularly strong C─H bonds. Thus, it is urgent optimize the driving force structure for accelerating integration sustainable energy. In this review, advances in energy‐driven are systematically summarized provide a scientific understanding operation/storage concepts, reactor design, technological maturity, system optimization, and remaining issues. Furthermore, essence, economic evaluations, balance, social impacts driven carefully discussed, paving path future course research development. Diversifying mix can play an important role industries, being used as crucial step transition energy, especially combination solar/nuclear with fossil fuels produce chemicals. Additionally, review intends bridge studies development, ultimate goal offering robust framework understand current status guidance design solutions greener future.

Language: Английский

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Pumping Electrons from Oxygen-Bridged Cobalt for Low-Charging-Voltage Zn-Air Batteries

Nano Letters, Journal Year: 2024, Volume and Issue: 24(43), P. 13653 - 13661

Published: Oct. 21, 2024

Reducing the charging voltage is a prerequisite for improving chargeability and energy efficiency of Zn-air batteries (ZABs). Herein, Fe

Language: Английский

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Co/Ce-MOF-Derived Oxygen Electrode Bifunctional Catalyst for Rechargeable Zinc–Air Batteries

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(24), P. 11135 - 11145

Published: June 3, 2024

Improving the practicality of rechargeable zinc–air batteries relies heavily on development oxygen electrode catalysts that are low-cost, durable, and highly efficient in performing dual functions. In present study, a catalyst with atomic Ce Co distribution nitrogen-doped carbon substrate was prepared by doping rare earth elements into metal–organic framework precursor. Rare element Ce, known for its unique structure excellent affinity, utilized to regulate catalytic activity. The this study demonstrated an exceptional electrocatalytic performance. At current density 10 mA cm–2, exhibited overpotential 340 mV evolution reaction (OER), which lower than commercial IrO2 (370 mV), while achieving half-wave potential 0.79 V process reduction (ORR), exhibiting similar level effectiveness as commercially accessible Pt/C (0.8 V). catalyst's porous structure, interconnected three-dimensional network, large specific surface area factors contributing significant improvement Furthermore, comparison Pt/C+IrO2, good cycling stability high efficiency batteries.

Language: Английский

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Densely populated trimetallic single-atoms for durable low-temperature flexible zinc-air batteries

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123438 - 123438

Published: Oct. 28, 2023

Language: Английский

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