Assembly and Valence Modulation of Ordered Bimetallic MOFs for Highly Efficient Electrocatalytic Water Oxidation DOI Creative Commons

Yaling Wu,

Zhaopeng Sun, Yingying Chen

et al.

Molecules, Journal Year: 2024, Volume and Issue: 29(24), P. 5845 - 5845

Published: Dec. 11, 2024

Metal synergy can enhance the catalytic performance, and a prefabricated solid precursor guide ordered embedding, of secondary metal source ions for rapid synthesis bimetallic organic frameworks (MM'-MOFs) with stoichiometric ratio 1:1. In this paper, Co-MOF-1D containing well-defined binding sites was synthesized by mechanical ball milling, which used as template induced introduction Fe to successfully assemble Co1Fe1-MOF-74@2 (where @2 denotes template-directed MOF-74). Its electrocatalytic performance is superior that conventional one-step-synthesized Co1Fe1-MOF-74@1 @1 one-step MOF-74), two sources, Co Fe, close Meanwhile, iron valence states (FeII FeIII) in were further regulated obtain materials Co1Fe1(II)-MOF-74@2 Co1Fe1(III)-MOF-74@2. The electrochemical test results confirm state has better than Co1Fe1(III)-MOF-74@2 oxygen evolution reaction (OER) process. This phenomenon related gradual increase Co1Fe1(II)-MOF-74@2, promotes continuous improvement MOF before reaching optimal steady makes OER reach optimum when FeII/FeIII mixed-valence reaches certain proportion. provides new idea directed optimization highly efficient catalysts.

Language: Английский

Selective activation of peroxymonosulfate through gating heteronuclear diatomic distance for flexible generation of high-valent cobalt-oxo species or sulfate radicals DOI

Jingjing Jiang,

Yanan Zhang, Yansong Liu

et al.

Water Research, Journal Year: 2025, Volume and Issue: unknown, P. 123488 - 123488

Published: March 1, 2025

Language: Английский

Citations

2
Interface-Sensitive Soft X-ray Absorption Spectroscopy by Electron/Ion-Yield Methods and Its Application to Solid–Liquid Interfaces for SrTiO3 and CoOOH DOI
Zi Wang,

Ryo Toyoshima,

Kota Enomoto

et al.

The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 27, 2025

Language: Английский

Citations

0
Electrochemical reduction for modulating spin state of nickel: A pathway to improved water and seawater oxidation DOI
Shuai Yu, Shucheng Liu, Tao Zhang

et al.

Applied Physics Letters, Journal Year: 2025, Volume and Issue: 126(4)

Published: Jan. 27, 2025

Understanding the electronic structure of catalysts is crucial for analyzing electrocatalyst behavior. Here, we present a straightforward method to modify configuration active sites in nickel-iron-niobium layered double hydroxides (NiFeNb-LDHs) via electrochemical reduction (ER), uncovering key factors that enhance oxygen evolution reaction (OER) activity. The results indicate ER-NiFeNb-LDHs display excellent OER performance and long-term stability over 60 h various electrolytes (271.99 mV@50 mA cm−2 1M KOH 280.56 +0.5M NaCl). Furthermore, cell voltage two-electrode electrolyzer ǁ Pt/C achieves current density 50 at an ultra-low 1.58 V, significantly outperforming commercial RuO2ǁPt/C. X-ray absorption spectroscopy, magnetic characterization, functional theory calculations reveal unsaturated coordination environment created by ER modifies state distribution between eg t2g orbitals, effectively lowering spin nickel enhancing its

Language: Английский

Citations

0
Spin‐Selective Catalysts for Oxygen‐Involved Electrocatalysis DOI Creative Commons
Haifan Li, Quan Quan, Chun‐Yuen Wong

et al.

Advanced Energy and Sustainability Research, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

The sluggish kinetics of oxygen‐involved electrolysis, such as oxygen evolution reaction (OER) and reduction (ORR), hinders the efficiency pertaining energy conversion process, which can be promoted by using spin‐selective materials to align spin direction intermediates. This review delivers a thorough timely overview state‐of‐the‐art catalysts for OER ORR. Primarily, fundamental principle process is depicted spin‐sensitive pathways, pointing out that existence spin‐polarized adsorption sites necessary development catalysts. Subsequently, approaches investigating spin‐related transition during electrocatalysis are introduced reviewing in situ technologies theoretical calculations. Then, reported categorized into intrinsic materials, doping‐induced multiple magnetic composites discuss their application electrocatalytic ORR well mechanism polarization. Finally, open questions prospects this field concluded, aiming offer clear route designing novel highly‐efficient industrial electrocatalysis.

Language: Английский

Citations

0
Optimizing Electron Delocalization in Cobalt Clusters via d‐d Orbital Coupling for Efficient Bifunctional Oxygen Electrocatalysis DOI
Xin Yu Wang,

Sichen Huo,

Yanjie Chen

et al.

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

Published: April 14, 2025

Abstract Cobalt atom cluster (Co AC )‐based electrocatalysts usually exhibit high activity for oxygen reduction reaction (ORR), but display limited performance in evolution (OER). To enhance their bifunctional catalytic efficiency, it is crucial to tailor the d ‐orbital electronic structure of Co through orbital coupling effect, optimizing chemisorption O‐intermediates. Herein, a 3 ‐4 strategy used construct ‐molybdenum carbide/nanocarbon cake ‐Mo x C/CC) catalyst with hollow ORR/OER zinc‐air batteries (ZABs). Experimental and theoretical results confirm that 4 transition metal Mo, fewer electrons more unfilled orbitals, interacts strongly sites ‐ coupling, promoting electron enrichment triggering delocalization. This process accelerates rate‐limiting steps *OH desorption ORR *OOH formation OER, leading an ultra‐low potential gap 0.604 V improved stability. Notably, C/CC‐based liquid flexible all‐solid‐state ZABs excellent open‐circuit voltages 1.49 1.47 V, power densities 146.4 103.4 mW cm −2 , respectively, highlighting replace precious catalysts. study may open new avenues manipulating properties ‐based boosting strategy.

Language: Английский

Citations

0
Manipulating Electron Structure through Dual-Interface Engineering of 3C-SiC Photoanode for Enhanced Solar Water Splitting DOI Creative Commons
Hui Zeng, Satoru Yoshioka, Weimin Wang

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: April 17, 2025

Interface engineering is crucial for enhancing the efficiency of semiconductor-based solar energy devices. In this work, we report a novel dual-interface strategy by designing Ni(OH)2/Co3O4/3C-SiC photoanode that achieves remarkable enhancements in photoelectrochemical (PEC) water splitting performance. The optimized delivers photocurrent density 1.68 mA cm-2 at 1.23 V vs reversible hydrogen electrode (RHE), representing an 8-fold increase compared to pristine 3C-SiC, along with excellent operational stability. architecture, Co3O4 serves as highly efficient hole-extraction layer and forms p-n junction separation photogenerated electron-hole pairs. At Ni(OH)2/Co3O4 interface, formation Ni-O-Co bonds facilitates rapid charge transfer accelerates oxygen evolution reaction (OER) kinetics. microwave photoconductivity decay (μ-PCD) measurements confirm prolonged minority carrier lifetime, demonstrating critical role electronic structure modulation improving reducing recombination. Using advanced synchrotron radiation X-ray absorption spectroscopy, unveil modifications interfacial induced their roles PEC These findings establish clear relationship between modulation, dynamics, performance, providing new insights into interface design strategies solar-driven systems.

Language: Английский

Citations

0
Unraveling the Synergistic Effect of Hollow Sea Urchin-like Ag–Co3O4 Heterostructures in Electrochemical Dehydrogenation Reactions: Interface-Enhanced Electron Transfer and Desorption Process DOI
Yuqiu Wang, Lin Miao, Renyi Shi

et al.

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 7966 - 7978

Published: April 29, 2025

Language: Английский

Citations

0
High-efficiency ammonia electrosynthesis from nitrate on ruthenium-induced trivalent cobalt sites DOI Creative Commons
Longcheng Zhang, Yuan Liu, Ling Li

et al.

Energy & Environmental Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This work highlights the potential of nitrate reduction as a viable and sustainable alternative for green ammonia production, bridging gap between fundamental research industrial application.

Language: Английский

Citations

0
Orbital-level band gap engineering of RuO2 for enhanced acidic water oxidation DOI Creative Commons
Xing Wang, Wei Pi, Z. Y. Li

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: May 24, 2025

Developing efficient and stable oxygen evolution reaction electrocatalysts under acidic conditions is crucial for advancing proton-exchange membrane water electrolysers commercialization. Here, we develop a representative strategy through p-orbital atoms (N, P, S, Se) doping in RuO2 to precisely regulate the lattice oxygen-mediated mechanism-oxygen vacancy site mechanism pathway. In situ ex measurements along with theoretical calculations demonstrate that Se dynamically adjusts band gap between Ru-eg O-p orbitals during process. This modulation accelerates electron diffusion external circuit, promotes process, enhances catalytic activity. Additionally, it facilitates feedback stabilizes vacancies, thereby promoting process enhancing stability. The resulting Se-RuOx catalyst achieves performance industrial minimal charge overpotential of 1.67 V achieve current density 1 A cm-2 maintain long-term cyclability over 1000 h. work presents unique method guiding future development high-performance metal oxide catalysts.

Language: Английский

Citations

0
Steering the adsorption modes and oxidation state of Co oxyhydroxide active sites to unlock selective glucose oxidation to formate for efficient solar reforming of biomass to green hydrogen DOI Creative Commons
Xin Zhao, Zhonghan Zhang, Chenfei Li

et al.

eScience, Journal Year: 2025, Volume and Issue: unknown, P. 100431 - 100431

Published: May 1, 2025

Language: Английский

Citations

0