Oxygen‐Vacancy‐Induced Formation of Pt‐Based Intermetallics on MXene with Strong Metal‐Support Interactions for Efficient Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2024, Номер 36(25)

Опубликована: Март 7, 2024

Abstract The Pt‐based alloys can moderate the binding energies of oxygenated species on catalytic surface, endowing superior performance towards oxygen reduction reaction (ORR). Nevertheless, it is still challenging to explore general methods synthesize structurally ordered intermetallics with uniform distributions. Herein, strong metal‐support interaction employed facilitate interdiffusion Pt/M atoms by establishing a tunnel vacancy ultrathin Ti 3 C 2 T x (MXene) sheets, synthesizing PtFe, PtCo, PtZn, PdFe, PdZn loaded onto . Furthermore, in‐situ generation Ti–O from could be bonded Pt and forming Pt–O–Ti, resulting in charge redistribution through Pt–O–Ti structure. Theoretical calculations demonstrate that valuable observed at interface extended even distance two nanometers interface, which modulate Pt–Pt distance, optimize Pt–O energy enhance intrinsic activity ORR. coupling between PtFe containing titanium oxide layer endows high stability composites. This work not only presents synthesis strategy for but also provides new insight essential structural evolution materials vacancies.

Язык: Английский

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Construction of Fe Nanoclusters/Nanoparticles to Engineer FeN₄ Sites on Multichannel Porous Carbon Fibers for Boosting Oxygen Reduction Reaction

Advanced Functional Materials, Год журнала: 2024, Номер 34(23)

Опубликована: Янв. 15, 2024

Abstract Fe–N–C catalysts are emerging as promising alternatives to Pt‐based for the oxygen reduction reaction (ORR), while they still suffer from sluggish kinetics due discontented binding affinity between Fe‐N 4 sites and oxygen‐containing intermediates, unsatisfactory stability. Herein, a flexible multichannel carbon fiber membrane immobilized with atomically dispersed neighboring Fe nanoclusters/nanoparticles (FeN ‐Fe NCP @MCF) is synthesized. The optimized geometric electronic structures of atomic brought by adjacent hierarchically porous structure matrix endow FeN @MCF outstanding ORR activity stability, considerably outperforming its counterpart only commercial Pt/C catalyst. Liquid solid‐state zinc–air batteries employing both exhibit durability. Theoretical calculation reveals that nanoclusters can trigger remarkable electron redistribution modulate hybridization central 3 d O 2 p orbitals, facilitating activation molecules optimizing adsorption capacity intermediates on sites, thus accelerating kinetic. This work offers an effective approach constructing coupling have single atoms coexisting efficient catalysis.

Язык: Английский

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Tailoring First Coordination Sphere of Dual‐Metal Atom Sites Boosts Oxygen Reduction and Evolution Activities

Advanced Functional Materials, Год журнала: 2024, Номер 34(28)

Опубликована: Фев. 24, 2024

Abstract It is important to tune the coordination configuration of dual‐atom catalyst (DAC), especially in first sphere, render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type atomically dispersed and boron‐coordinated DAC structure, namely, FeN 4 B‐NiN B dual sites, reported. In this incorporation boron into sphere /NiN atomic sites regulates its geometry electronic structure by forming “Fe‐B‐N” “Ni‐B‐N” bridges. The exhibits much enhanced ORR OER property compared ‐NiN counterparts. Density functional theory calculations reveal that boron‐induced charge transfer asymmetric distributions central Fe/Ni atoms optimize adsorption desorption behavior ORR/OER intermediates reduce activation energy potential‐determining step. Zinc‐air batteries employing cathode exhibit maximum power density (236.9 mW cm −2 ) stable cyclability up 1100 h. result illustrates pivotal role first‐coordination DACs tuning electrochemical conversion storage activities.

Язык: Английский

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Boosting ORR/OER bifunctional electrocatalysis by promoting electronic redistribution of Fe-N-C on CoFe-FeNC for ultra-long rechargeable Zn-air batteries

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 359, С. 124485 - 124485

Опубликована: Авг. 8, 2024

Язык: Английский

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Low-loaded Ru on hollow SnO₂ for enhanced electrocatalytic hydrogen evolution

Chemical Communications, Год журнала: 2024, Номер 60(20), С. 2768 - 2771

Опубликована: Янв. 1, 2024

Ru–SnO 2 with low Ru loading and a hollow structure is developed as high-performance electrocatalyst for the hydrogen evolution reaction.

Язык: Английский

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Potential-Resolved Ratiometric Aptasensor for Sensitive Acetamiprid Analysis Based on Coreactant-free Electrochemiluminescence Luminophores of Gd-MOF and “Light Switch” Molecule of [Ru(bpy)₂dppz]²⁺

Analytical Chemistry, Год журнала: 2024, Номер 96(12), С. 5022 - 5028

Опубликована: Март 12, 2024

For conventional potential-resolved ratiometric electrochemiluminescence (ECL) systems, the introduction of multiplex coreactants is imperative. However, undesirable interactions between different inevitably affect analytical accuracy and sensitivity. Herein, through coordination aggregation-induced emission ligands with gadolinium cations, self-luminescent metal–organic framework (Gd-MOF) prepared serves as a novel coreactant-free anodic ECL emitter. By intercalation [Ru(bpy)2dppz]2+ light switch effect into DNA duplex, one high-efficiency cathodic probe obtained using K2S2O8 coreactant. In presence acetamiprid, strong affinity target its aptamer induces release [Ru(bpy)2dppz]2+, resulting in decreasing cathode signal an increasing anode owing to resonance energy transfer from Gd-MOF [Ru(bpy)2dppz]2+. this way, efficient dual-signal aptasensor constructed for analysis exhibiting remarkably low detection limit 0.033 pM. Strikingly, by only exogenous coreactant, cross interference multiple can be eliminated, thus improving accuracy. The developed high-performance sensing platform successfully applied monitor residual level acetamiprid real samples, demonstrating potential application field food security.

Язык: Английский

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Biphase Pd Nanosheets with Atomic‐Hybrid RhO_x/Pd Amorphous Skins Disentangle the Activity‐Stability Trade‐Off in Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 29, 2024

Abstract The activity‐stability trade‐off relationship of oxygen reduction reaction (ORR) is a tricky issue that strikes the electrocatalyst population and hinders widespread application fuel cells. Here neoteric biphase Pd nanosheets are structured with ultrathin two‐dimensional crystalline inner cores ≈1 nm thin atomic‐hybrid RhO x /Pd amorphous skins, named c/a‐Pd@PdRh NSs, for disentangling this dilemma alkaline ORR developed. superthin skins significantly amplify quantity flexibly low‐coordinated atoms electrocatalysis. An in situ selected oxidation top‐surface Rh dopants creates atomically hybrid disorder surfaces. Detailed energy spectra theoretical simulation confirm these interfaces can arouse surface charge redistribution, causing significant electron deficiency lowered d ‐band center Pd. Meanwhile, anticorrosive Rh/RhO species thermodynamically passivate neighboring from oxidative dissolution. Thanks to amplified interfacial effects, NSs simultaneously exhibit superhigh activity (5.92 A mg −1 , 22.8 times Pt/C) an outstanding long‐lasting stability after 100k cycles accelerated durability test, showcasing unprecedented electrocatalysts breaking ORR. This work paves bran‐new strategy designing high‐performance through creating modulated on low‐dimensional nanomaterials.

Язык: Английский

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Improvement in ORR Durability of Fe Single-Atom Carbon Catalysts Hybridized with CeO₂ Nanozyme

Nano Letters, Год журнала: 2024, Номер 24(29), С. 9034 - 9041

Опубликована: Июль 11, 2024

FeNC catalysts are considered one of the most promising alternatives to platinum group metals for oxygen reduction reaction (ORR). Despite extensive research on improving ORR activity, undesirable durability is still a critical issue its practical application. Herein, inspired by antioxidant mechanism natural enzymes, CeO

Язык: Английский

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MOF-Derived Cobalt Nanoparticles with Dispersed Iron Phthalocyanines as Bifunctional Oxygen Electrocatalysts

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(11), С. 4779 - 4788

Опубликована: Март 7, 2024

Iron phthalocyanine (FePc), characterized by its distinctive Fe–N4 sites, represents a macromolecular catalyst with promising applications in bifunctional oxygen catalysis. However, inherently flat and symmetrical configuration often results relatively weak electrocatalytic performance. In this study, novel approach was employed first anchoring the Co-based zeolitic imidazolate framework onto microsized carbon spheres derived from Zn-based coordination polymer, followed incorporation of dispersed FePc molecules. The resultant catalyst, denoted as FePc-CoNC-CMS, exhibited remarkable reduction reaction/oxygen evolution reaction (ORR/OER) activity an alkaline medium, notably achieving half-wave potential 0.87 V overpotential 313 mV at 10 mA cm–2. Both experimental theoretical investigations revealed that presence on cobalt surface induced significant alterations electron distribution within Fe center, thereby regulating adsorption affinity sites toward oxygen. This structural modification led to outstanding activity. When applied zinc–air batteries, it demonstrated excellent power density 147.6 mW cm–2 satisfactory charge–discharge stability over period 70 h pioneering work integrates metal–organic framework-derived metal–carbon nanomaterials catalysts, offering efficient pathway for multifunctional applications.

Язык: Английский

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Recent strategies to improve the electroactivity of metal–organic frameworks for advanced electrocatalysis

Deleted Journal, Год журнала: 2024, Номер 1(2), С. 181 - 206

Опубликована: Авг. 4, 2024

Abstract Metal–organic frameworks (MOFs) have emerged as promising materials in the realm of electrocatalysis due to their high surface area, tunable porosity, and versatile chemical functionality. However, practical application has been hampered by inherent limitations such low electrical conductivity a limited number active metal sites. Researchers addressed these challenges through various strategies, including enhancing incorporating conductive nanoparticles, modifying structure composition MOFs replacing nodes functionalizing linkers, preparing catalysts thermal processes decarburization conversion into oxides, phosphides (MPs), sulfides (MSs). This review provided comprehensive summary strategies that were employed enhance electroactivity for improved electrocatalytic performance recent years. It also explored future directions potential innovations design synthesis MOF‐based electrocatalysts, offering valuable insights advancing sustainable energy technologies.

Язык: Английский

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