Strain-Triggered Distinct Oxygen Evolution Reaction Pathway in Two-Dimensional Metastable Phase IrO₂ via CeO₂ Loading

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(29), P. 20251 - 20262

Published: July 12, 2024

A strain engineering strategy is crucial for designing a high-performance catalyst. However, how to control the in metastable phase two-dimensional (2D) materials technically challenging due their nanoscale sizes. Here, we report that cerium dioxide (CeO

Language: Английский

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Pyrrole-type TM-N3 sites as high-efficient bifunctional oxygen reactions electrocatalysts: From theoretical prediction to experimental validation

Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

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Graphitic Carbon Nitride-Supported Layered Double Hydroxides (GCN@FeMg-LDH) for Efficient Water Splitting and Energy Harvesting

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

The advancement of highly efficient and cost-effective electrocatalysts for electrochemical water splitting, along with the development triboelectric nanogenerators (TENGs), is crucial sustainable energy generation harvesting. In this study, a novel hybrid composite by integrating graphitic carbon nitride (GCN) an earth-abundant FeMg-layered double hydroxide (LDH) (GCN@FeMg-LDH) was synthesized hydrothermal approach. Under controlled conditions, optimized concentrations metal ions GCN, fabricated electrode, GCN@FeMg-LDH demonstrated remarkably low overpotentials 0.018 0.284 V 0.101 0.365 at 10 600 mA/cm2 toward hydrogen evolution (HER) oxygen (OER) reactions, respectively, in 1.0 M KOH. Furthermore, we leveraged potential to develop high-performance TENG suitable practical electronic applications. resulting GCN@FeMg-LDH-based device, sized 3 × 4 cm2, substantial current output 52 μA voltage 771 V. Notably, device exhibited instantaneous power 5780 μW exceptional stability, enduring over 15 000 cycles. Thus, study concludes that emerges as superior candidate applications splitting TENGs, exhibiting significant promise advancing clean technologies, addition lowering greenhouse gas emissions.

Language: Английский

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Boosting Oxygen Reduction Reaction Performance of Fe Single‐Atom Catalysts Via Precise Control of the Coordination Environment

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 3, 2025

Abstract Fe single‐atom on N‐doped carbon (FeN‐C) catalysts emerge as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Heterogeneous atom doping is proposed be effective modulating catalyst performance. Despite this, relationship between fine coordination structure of doped atoms and catalytic activity central metal site remains poorly understood. Herein, with S in either first shell (FeSN–C) or second (FeN–SC) active are synthesized compare effects different structure. FeN–SC exhibits prominent performance a half‐wave potential 0.92 V rotating disk electrode peak power density 251 mW cm −2 zinc–air battery. Theoretical studies reveal that effectively modulates electronic charge transfer at center. Compared directly coordinated within shell, located more optimizing adsorption desorption energy barriers oxygen‐containing intermediates sites. This study provides new strategy adjust by engineering multilayer center catalyst.

Language: Английский

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Manipulating the Electronic Properties of an Fe Single Atom Catalyst via Secondary Coordination Sphere Engineering to Provide Enhanced Oxygen Electrocatalytic Activity in Zinc‐Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(44)

Published: Sept. 16, 2024

Abstract Oxygen reduction and evolution reactions are two key processes in electrochemical energy conversion technologies. Synthesis of nonprecious metal, carbon‐based electrocatalysts with high oxygen bifunctional activity stability is a crucial, yet challenging step to achieving conversion. Here, an approach address this issue: synthesis atomically dispersed Fe electrocatalyst (Fe 1 /NCP) over porous, defect‐containing nitrogen‐doped carbon support, described. Through incorporation phosphorus atom into the second coordination sphere iron, durability boundaries catalyst pushed unprecedented level alkaline environments, such as those found zinc‐air battery. The rationale delicately incorporate P heteroatoms defects close central metal sites (FeN 4 ‐OH) order break local symmetry electronic distribution. This enables suitable binding strength oxygenated intermediates. In situ characterizations theoretical studies demonstrate that these synergetic interactions responsible for stability. These intrinsic advantages /NCP enable potential gap mere 0.65 V power density 263.8 mW cm −2 when incorporated findings underscore importance design principles access high‐performance green

Language: Английский

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Diatomic Catalysts for Aqueous Zinc‐Iodine Batteries: Mechanistic Insights and Design Strategies

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(49)

Published: Sept. 13, 2024

Abstract There has been a growing interest in developing catalysts to enable the reversible iodine conversion reaction for high‐performance aqueous zinc‐iodine batteries (AZIBs). While diatomic (DACs) have demonstrated superior performance various catalytic reactions due their ability facilitate synergistic charge interactions, application AZIBs remains unexplored. Herein, we present, first time, DAC comprising Mn−Zn dual atoms anchored on nitrogen‐doped carbon matrix (MnZn−NC) loading, resulting AZIB with capacity of 224 mAh g −1 at 1 A and remarkable cycling stability over 320,000 cycles. The electron hopping along Mn−N−Zn bridge is stimulated via spin exchange mechanism. This process broadens Mn 3d xy band width enhances metallic character catalyst, thus facilitating transfer between intermediates. Additionally, increased occupancy within d‐orbital Zn elevates Zn's d‐band center, thereby enhancing chemical interactions MnZn−NC I‐based species. Furthermore, our mechanism demonstrates potential applicability other Metal‐Zn−NC DACs spin‐polarized atoms. Our work elucidates clear mechanistic understanding provides new insights into catalyst design AZIBs.

Language: Английский

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Porous LaMO3 (M = Co, Mn, Fe) perovskite oxides derived from MOFs as efficient catalysts for toluene oxidation

Journal of Alloys and Compounds, Journal Year: 2025, Volume and Issue: unknown, P. 178617 - 178617

Published: Jan. 1, 2025

Language: Английский

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Pyridinic‐N Seized Co in Biphasic Nanoarchitecture for Reversible Oxygen Electrocatalysis Enabling Longevous (>1200 h) Aqueous and Dual‐Anion Kosmotropic Electrolyte Stabilized High Power Quasisolid‐State Zn–Air Battery

Small Methods, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 19, 2025

Abstract Integration of different active sites by heterostructure engineering is pivotal to optimize the intrinsic activities an oxygen electrocatalyst and much needed enhance performance rechargeable Zn–air batteries (ZABs). Herein, a biphasic nanoarchitecture encased in situ grown N‐doped graphitic carbon (MnO/Co‐NGC) with heterointerfacial are constructed. The density functional theory model reveals formation lattice bridged pyridinic nitrogen atoms anchored Co species, which facilitate adsorption intermediates. Consequently, well‐designed catalyst accessible sites, abundant vacant coupling effects, simultaneously accelerate electron/mass transfer thus promotes trifunctional electrocatalysis. assembled aqueous ZAB delivers maximum power ≈268 mW cm −2 specific capacity 797.8 mAh g zn −1 along excellent rechargeability extremely small voltage gap decay rate 0.0007 V h . Further, fabricated quasisolid‐state owns remarkable 163 long cycle life, outperforming benchmark air‐electrode many recent reports, underlining its robustness suitability for practical utilization diverse portable applications.

Language: Английский

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Utilizing Molybdenum to Tailor the Electronic Structure of Iron Through Electron Complementary Effect for Promoting Oxygen Reduction Activity

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

Abstract Tailoring the electronic structure of later transition metal‐based electrocatalysts by incorporating early metal based on complementary effect is anticipated to enhance electrocatalytic activity. Herein, modulation Fe 3 C through utilization Mo 2 promote oxygen reduction reaction (ORR) activity reported. In situ characterizations combined with theoretical calculations reveal that electron‐donating capability molybdenum in active center iron optimizes adsorption and activation oxygen. Concurrently, d‐band much closer Fermi level, which reduces energy barrier for rate‐determining step ( * OOH → O), thereby enhancing ORR alkaline media, catalyst delivers a half‐wave potential E 1/2 ) 0.89 V maintains its efficiency mere 8 mV decay after 10 000 cycles, surpassing Pt/C. Moreover, it can serve as an air cathode both liquid‐state all‐solid‐state zinc‐air batteries (ZABs) shows promising applications portable devices. This work brings innovative design concept highly efficient suitable advanced

Language: Английский

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Heteroatom Immobilization Engineering toward High-Performance Metal Anodes

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 11, 2024

Heteroatom immobilization engineering (HAIE) is becoming a forefront approach in materials science and engineering, focusing on the precise control manipulation of atomic-level interactions within heterogeneous systems. HAIE has emerged as an efficient strategy to fabricate single-atom sites for enhancing performance metal-based batteries. Despite significant progress achieved through metal anodes batteries, several critical challenges such dendrites, side reactions, sluggish reaction kinetics are still present. In this review, we delve into fundamental principles underlying heteroatom anodes, aiming elucidate its role electrochemical We systematically investigate how facilitates uniform nucleation inhibits reactions at anode-electrolyte interface, promoting desolvation ions accelerating Finally, discuss various strategies implementing electrode materials, high-temperature pyrolysis, vacancy reduction, molten-salt etching anchoring. These include selecting appropriate heteroatoms, optimizing methods, constructing material architectures. They can be utilized further refine enhance capabilities facilitate widespread application next-generation battery technologies.

Language: Английский

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