Unraveling Compressive Strain and Oxygen Vacancy Effect of Iridium Oxide for Proton‐Exchange Membrane Water Electrolyzers DOI Open Access

Meihuan Liu,

Xiaoyan Zhong, Xiaoxia Chen

et al.

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

Published: March 11, 2025

Abstract Iridium‐based electrocatalysts are commonly regarded as the sole stable operating acidic oxygen evolution reaction (OER) catalysts in proton‐exchange membrane water electrolysis (PEMWE), but linear scaling relationship (LSR) of multiple intermediates binding inhibits enhancement its activity. Herein, compressive strain and vacancy effect exists iridium dioxide (IrO 2 )‐based catalyst by a doping engineering strategy for efficient OER In situ synchrotron characterizations elucidate that can enhance Ir─O covalency reduce Ir─Ir bond distance, (O v ) an electronic regulator causes rapid adsorption molecules on Ir adjacent Ov (Ir─O pair site to be coupled directly into * O─O intermediates. Importantly, hence, volcano‐shape curves established between strain/oxygen current using probe reaction. Theoretical calculation reveals Ni dopant modulate 5 d ‐ O p ‐band centers increasing overlap orbits trigger continuous metal site‐oxygen synergistic mechanism (MS‐O V SM) pathway, successfully breaking LSR during OER. Therefore, resultant (PEMWE) device fabricated T‐0.24Ni/IrO delivers density 500 mA cm −2 operates stably h.

Language: Английский

Advance in rare earth element modified nanomaterials for enhanced electrocatalytic water splitting DOI
Le Li,

Shuanqiang Liu,

Ying Li

et al.

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 85, P. 818 - 831

Published: Aug. 28, 2024

Language: Английский

Citations

4
Visualization of the Distance-Dependent Synergistic Interaction in Heterogeneous Dual-Site Catalysis DOI

Shuaiwei Jiang,

Jiawei Xue,

Tong Liu

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(42), P. 29084 - 29093

Published: Oct. 11, 2024

Understanding the characteristics of interfacial hydroxyl (OH) at solid/liquid electrochemical interface is crucial for deciphering synergistic catalysis. However, it remains challenging to elucidate influences spatial distance between OH and neighboring reactants on reaction kinetics atomic level. Herein, we visualize distance-dependent interaction in heterogeneous dual-site catalysis by using ex-situ infrared nanospectroscopy situ spectroscopy techniques. These spectroscopic techniques achieve direct identification distribution species reveal that facilitates reactant deprotonation process depending site distances catalysts. Via modulating Ir-Co pair distances, find dynamic equilibrium generation consumption accounts high-efficiency synergism optimized 7.9 Å. At farther or shorter inaccessibility resistance with intermediates lead accumulation, thereby diminishing effect. Hence, a volcano-shaped curve has been established mass activity formic acid oxidation as probe reaction. This notion could also be extended oxophilic metals, like Ir-Ru pairs, where volcano curves further evidence universal significance distances.

Language: Английский

Citations

4
Supersaturated Doping-Induced Maximized Metal–Support Interaction for Highly Active and Durable Oxygen Evolution DOI
Hanwen Liu, Wenhui Shi, Yaqing Guo

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(43), P. 29724 - 29735

Published: Oct. 14, 2024

Metal–support interaction (MSI) is pivotal and ubiquitously used in the development of next-generation catalysts, offering a pathway to enhance both catalytic activity stability. However, owing lattice mismatch poor solubility, traditional catalysts often exhibit metal-on-support heterogeneous structure with limited interfaces and, consequently, compromised enhancement properties. Herein, we report universal tunable method for supersaturated doping transition-metal carbides via strongly nonequilibrium carbothermal shock synthesis, characterized by rapid heating swift quenching. Our results enable ∼20 at. % Ni2FeCo Mo2C, significantly surpassing thermodynamic equilibrium limit <3 %. The supersaturation ensures more catalytically active NiFeCo sufficient resulting maximized MSI (Max-MSI) effect. Max-MSI enables outstanding particularly stability alkaline oxygen evolution reaction, showing an overpotential 284 mV at 100 mA cm–2 stable 700 h, while individual Mo2C only last less than 70 10 h (completely dissolved), respectively. In particular, SD-Mo2C catalyst also exhibits excellent durability up 400 7 M KOH. Such improved attributed that led each Mo atom binding adjacent heteroatoms, thus elevating dissolution potential corrosion resistance high current density. Additionally, highly dispersed facilitates formation dense oxyhydroxide coating during reconstruction, further protecting integrated durable operation. Furthermore, synthesis has been successfully scaled fabricate large (16 cm2) electrodes adaptable nickel foam substrates, indicating promising industrial applications. strategy allows general versatile production various doped carbides, such as Ni2FeCo-doped TiC, NbC, W2C, unlocking or adjustable diverse

Language: Английский

Citations

4
Design of Electrocatalysts with High Performance Based on Thermodynamics and Kinetics: Progress and Prospects DOI
Minshu Du,

Feihan Yu,

Shumin Gong

et al.

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

Published: Oct. 15, 2024

Abstract Efficient and robust electrocatalysts play a central role in clean energy conversion, enabling number of sustainable processes for future technologies. The traditional explorations electrocatalyst relying on the trial‐and‐error approaches are definitely tedious inefficient. Theoretical progresses reactive thermodynamics kinetics recent years have initiated powerful theory‐guided design strategy electrocatalysts. Herein, this review first summarizes principles activity stability, presenting thermodynamics, kinetics, synergistic thermokinetic correlation electrocatalytic reaction. Second, screening criterion, reasonable design, mechanistic understanding, performance evaluation typical as divided into oriented‐, oriented‐designs discussed. necessity correlating rational mechanism clarification is highlighted. Finally, conclusions perspectives development highly efficient proposed.

Language: Английский

Citations

4
Electronic Structure Engineering of Single‐Atom Tungsten on Vacancy‐enriched V3S4 Nanosheets for Efficient Hydrogen Evolution DOI Creative Commons
Min Xi, Hua Zhang, Lingfeng Yang

et al.

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

Published: Oct. 28, 2024

Abstract Constructing single‐atom catalysts (SACs) and optimizing the electronic structure between metal atoms support interactions is deemed one of most effective strategies for boosting catalytic kinetics hydrogen evolution reaction (HER). Herein, a sulfur vacancy defect trapping strategy developed to anchor tungsten single onto ultrathin V 3 S 4 nanosheets with high loading 25.1 wt.%. The obtained W‐V catalyst exhibits low overpotential 54 mV at 10 mA cm −2 excellent long‐term stability in alkaline electrolytes. Density functional theory calculations reveal that situ anchoring W triggers delocalization redistribution electron density, which effectively accelerates water dissociation facilitates adsorption/desorption, thus enhancing HER activity. This work provides valuable insights into understanding highly active large‐scale production.

Language: Английский

Citations

4
“Similar stacking”‐inspired compressive strain of heterogeneous phosphide for efficient hydrogen evolution DOI Creative Commons
Tianyi Xu,

Dongxu Jiao,

Jinchang Fan

et al.

Carbon Energy, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Abstract Strain effects have garnered significant attention in catalytic applications due to their ability modulate the electronic structure and surface adsorption properties of catalysts. In this study, we propose a novel approach called “similar stacking” for stress modulation, achieved through loading Co 2 P on Ni (Ni P/Co P). Theoretical simulations reveal that compressive strain induced by influences orbital overlap electron transfer with hydrogen atoms. Furthermore, number stacked layers can be adjusted varying precursor soaking time, which further modulates range adsorption. Under 2‐h condition, effect proves favorable efficient production. Experimental characterizations using X‐ray diffraction, high‐angel annular dark‐field scanning transmission election microscope (HAADF‐STEM), absorption near‐edge spectroscopy successfully demonstrate lattice contraction bond length shortening Co–P. Remarkably, our catalyst shows an ultrahigh current density 1 A cm −2 at overpotential only 388 mV, surpassing commercial Pt/C, while maintaining long‐term stability. This material design strategy similar stacking opens up new avenues modulation deeper development electrocatalysts.

Language: Английский

Citations

0
Interfacial Engineering of MoS2-FeCoS2@NG Nanocomposite: An Efficient Electrocatalyst for Enhanced Flexible Zinc-Air Battery Performance DOI
Mallappa Mahanthappa, S M Ahmed, Debabrata Chanda

et al.

New Journal of Chemistry, Journal Year: 2025, Volume and Issue: 49(6), P. 2432 - 2442

Published: Jan. 1, 2025

MoS 2 –FeCoS @NG materials are excellent electrocatalysts for ORR and (OER) pose a considerable obstacle in the development of future rechargeable zinc–air batteries.

Language: Английский

Citations

0
Spin Magnetic Effect Activate Dual Site Intramolecular O─O Bridging for Nickel‐Iron Hydroxide Enhanced Oxygen Evolution Catalysis DOI Creative Commons

Haohai Dong,

Lanke Luo,

Shaobing Zhou

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 21, 2025

Abstract The oxygen evolution reaction (OER) involves the recombination of diamagnetic hydroxyl (OH) or water (H 2 O) into paramagnetic triplet state (O ). spin conservation intermediates plays a crucial role in OER, however, research on dynamics during catalytic process remains its early stages. Herein, β ‐Ni(OH) and Fe‐doped (Ni 5 Fe 1 ) are utilized as model catalysts to understand mechanism magnetic effects at iron (III) sites OER. Combined with characterization, it is founded that introduction transforms antiferromagnetic Ni(OH) ferromagnetic material. Testing response catalyst under an external field, OER activity Ni significantly enhanced comparison . This improvement likely due sites, which promote enhance kinetics, thereby increasing efficiency. Combining experimental theoretical discovered accelerate formation heterogeneous dual‐site O─O bridging, represented ─Ni─O─O─Fe─, effectively enhancing kinetics reaction. study provides perspective structure‐function relationship iron‐based has significant implications for design new catalysts.

Language: Английский

Citations

0
Spiny Co3O4@Hollow Carbon Spheres─Polyacrylonitrile/Carbon Black Fiber-Based Bifunctional Air Electrodes DOI

Yongsong Tan,

Xiaorong Shi,

Weiyi Han

et al.

Langmuir, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 23, 2025

In the realm of zinc-air batteries, high bifunctional catalytic efficacy is intimately tied to evaluation catalysts. Consequently, pursuit proficient catalysts that can efficiently catalyze both oxygen reduction reaction (ORR) and evolution (OER) remains a paramount objective in this research area. study, spiny cobalt tetroxide (Co3O4) encapsulated hollow carbon spheres (HCSs) are constructed by anchoring Co3O4 onto HCS via hydrothermal or annealing treatment. The strategic interface design encourages an abundance sites while simultaneously facilitating proliferation Co3O4, offering expansive surface area abundant active sites. Co3+ ions induction vacancies endow it with outstanding activity stability. After spray-coating subsequent catalyst on flexible carbon-based polyacrylonitrile (PAN) nanofiber support, HCS-PAN/carbon black (C) 800 air electrode successfully integrated. Moreover, optimized HCS-PAN/C displays decreased potential difference (ΔE) 0.77 V for catalyzing ORR OER performance. This work introduces promising candidate approach exploring innovative electrocatalysts, targeting enhanced efficiency portable energy storage applications.

Language: Английский

Citations

0
Molecular Nanojunction Catalyst for Oxygen Evolution Reaction DOI Open Access
Kuo Wei, Zhiping Liu, Guangyuan Feng

et al.

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

Published: Jan. 26, 2025

Abstract Achieving close integration and strong electronic communication between molecular catalysts conductive substrates is crucial for developing the stability catalytic activity of nanomaterials. However, constructing heterostructure catalyst usually need complex demanding synthesis processes. Herein, a facile universal “molecular nanojunction” strategy developed to prepare with high by improving coplanarity nanojunction facilitating efficient electron transfer. The density function theory (DFT) calculations in situ characterization indicate that reduces excessive * OH adsorption accelerates deprotonation process, thereby promoting oxygen generation. shows better evolution reaction (OER) performance than most reported catalysts. What's more, are applied alkaline anion exchange membrane (AEM) electrolysis cells, exhibiting excellent performance.

Language: Английский

Citations

0