High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH and H intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.
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http://dx.doi.org/10.1038/s41467-022-30379-4 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
Center of Nanomaterials for Renewable Energy, State Key Laboratory of Electrical Insulation and Power Equipment, School of Electrical Engineering, Xi'an Jiaotong University, Xìan, Shaanxi 710049, China.
Prussian blue analogues (PBAs) show great promise as cathode candidates for aqueous zinc-ion batteries thanks to their high operating voltage, open-framework structure, and low cost. However, suffering from numerous vacancies and crystal water, the electrochemical performance of PBAs remains unsatisfactory, with limited capacity and poor cycle life. Here, a simple coprecipitation method is shown to synthesize well-crystallized cobalt hexacyanoferrate (CoHCF) with a small amount of water and high specific surface area.
View Article and Find Full Text PDFNano Lett
January 2025
Department of Chemical and Biomolecular Engineering, National University of Singapore, 117585, Singapore.
Establishing optimized metal-support interaction (MSI) between active sites and the substrate is essential for modulating the adsorption properties of key reaction intermediates during catalysis, thereby enhancing the catalytic performance. In this study, catalyst composites with varying degrees of MSI are constructed using ruthenium (Ru) and different carbon nanotubes, and their performance for alkaline hydrogen evolution reaction (HER) is systematically investigated. Detailed kinetic assessments reveal that catalysts with a strong MSI exhibit superior HER activity.
View Article and Find Full Text PDFChem Asian J
January 2025
East China University of Science and Technology, School of Materials Science and Engineering, 130# Meilong Road, Shanghai, 200237, Shanghai, CHINA.
Li-ion capacitors (LICs) integrate the desirable features of lithium-ion batteries (LIBs) and supercapacitors (SCs), but the kinetic imbalance between the both electrodes leads to inferior electrochemical performance. Thus, constructing an advanced anode with outstanding rate capability and terrific redox kinetics is crucial to LICs. Herein, heterostructured ZnS/SnS2 nanosheets encapsulated into N-doped carbon microcubes (ZnS/SnS2@NC) are successfully fabricated.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
Department of Chemistry and Chemical Engineering, Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University, Shantou 515063, China.
Herein, we report the successful guidance of indole and formaldehyde reactivity by precisely tuning the pore size and active sites of MOF, altering their intrinsic reaction pathways. This led to the first example of novel compounds synthesized through the synergistic catalysis enabled by MOF confinement. Detailed mechanistic studies revealed that the confined environment within the MOF pores promoted the occurrence of multi-stage cascade reactions and stabilized specific reaction pathways.
View Article and Find Full Text PDFJ Chem Phys
January 2025
Departamento de Física, Instituto de Física e Matemática, Universidade Federal de Pelotas, Caixa Postal 354, Pelotas, Brazil.
Water is a fundamental component of life, playing a critical role in regulating metabolic processes and facilitating the dissolution and transport of essential molecules. However, emerging contaminants, such as pharmaceuticals, pose significant challenges to water quality and safety. Nanomaterial-based technologies emerge as a promising solution for removing those contaminants from water.
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