The integration of multiple elements in a high-entropy state is crucial in the design of high-performance, durable electrocatalysts. High-entropy metal hydroxide organic frameworks (HE-MHOFs) are synthesized under mild solvothermal conditions. This novel crystalline metal-organic framework (MOF) features a random, homogeneous distribution of cations within high-entropy hydroxide layers. HE-MHOF exhibits excellent electrocatalytic performance for the oxygen evolution reaction (OER), reaching a current density of 100 mA cm at ≈1.64 V, and demonstrates remarkable durability, maintaining a current density of 10 mA cm for over 100 h. Notably, HE-MHOF outperforms precious metal-based electrocatalysts despite containing only ≈60% OER active metals. Ab initio calculations and operando X-ray absorption spectroscopy (XAS) demonstrate that the high-entropy catalyst contains active sites that facilitate a multifaceted OER mechanism. This study highlights the benefits of high-entropy MOFs in developing noble metal-free electrocatalysts, reducing reliance on precious metals, lowering metal loading (especially for Ni, Co, and Mn), and ultimately reducing costs for sustainable water electrolysis technologies.
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http://dx.doi.org/10.1002/adma.202408114 | DOI Listing |
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11681304 | PMC |
ACS Appl Mater Interfaces
December 2024
TCS Research, Sahyadri Park 2, Rajiv Gandhi Infotech Park, Hinjewadi Phase 3, Pune 411057, India.
Realization of a sustainable hydrogen economy in the future requires the development of efficient and cost-effective catalysts for its production at scale. MXenes (MX) are a class of 2D materials with 'n' layers of carbon or nitrogen (X) interleaved by 'n+1' layers of transition metal (M) and have emerged as promising materials for various applications including catalysts for hydrogen evolution reaction (HER). Their properties are intimately related to both their composition and their atomic structure.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Shenzhen University, Chemistry, Nanhai Ave 3688, 518060, Shenzhen, CHINA.
The high entropy alloy (HEA) possesses distinctive thermal stability and electronic characteristics, which exhibits substantial potential for diverse applications in electrocatalytic reactions. However, accurately controlling the size of HEA still remains a challenge, especially for the ultrasmall HEA nanoparticles. Herein, we firstly calculate and illustrate the size impact on the electronic structure of HEA and the adsorption energies of crucial intermediates in typical electrocatalytic reactions, such as the hydrogen evolution reaction (HER), oxygen reduction reaction (ORR), CO2 electroreduction (CO2RR) and NO3- electroreduction (NO3RR).
View Article and Find Full Text PDFNanomaterials (Basel)
December 2024
School of Intelligent Manufacturing, Luoyang Institute of Science and Technology, Luoyang 471023, China.
(AlCrMoNiTi)N high-entropy alloy nitride (HEAN) films were synthesized at various bias voltages using the co-filter cathodic vacuum arc (co-FCVA) deposition technique. This study systematically investigates the effect of bias voltage on the microstructure and performance of HEAN films. The results indicate that an increase in bias voltage enhances the energy of ions while concomitantly reducing the deposition rate.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China.
Two-dimensional (2D) high-entropy transition metal dichalcogenides (HETMDs) have gained significant interest due to their structural properties and correlated possibilities for high-end devices. However, the controlled synthesis of 2D HETMDs presents substantial challenges owing to the distinction in the inherent characteristics among diverse metal elements in the synthesis, such as saturated vapor pressure of precursors and formation energy of products. Here, we present the synthesis of a 2D HETMD single crystal with 0.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Nanjing Normal University, No. 1, Wenyuan Road, Qixia District, CHINA.
The safety and cycling stability of potassium-ion batteries (PIBs) are deeply associated with potassium-ion electrolytes. However, due to the weak Lewis acidity of potassium ions, localized high-concentration electrolytes in PIBs are prone to excessive weak solvation. Herein, we propose an entropy repair strategy for the solvation structure of potassium ions and systematically design a moderately weakly solvated high-entropy localized high-concentration electrolyte.
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