Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts.

Nat Commun

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China.

Published: May 2022

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.

Download full-text PDF

Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9106752PMC
http://dx.doi.org/10.1038/s41467-022-30379-4DOI Listing

Publication Analysis

Top Keywords

active sites
12
high-entropy alloys
8
unraveling electronegativity-dominated
4
electronegativity-dominated intermediate
4
intermediate adsorption
4
adsorption high-entropy
4
high-entropy alloy
4
alloy electrocatalysts
4
electrocatalysts high-entropy
4
alloys received
4

Similar Publications

Cobalt Hexacyanoferrate Cathode with Stable Structure and Fast Kinetics for Aqueous Zinc-Ion Batteries.

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 PDF

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 PDF

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 PDF

MOF confinement enables selective synthesis of novel oxazoles from indole and formaldehyde.

Chem 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 PDF

Nanoscale water behavior and its impact on adsorption: A case study with CNTs and diclofenac.

J 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.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!