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Platinum (Pt)-based nanozymes display exceptional stability and catalytic activity in the activation of HO, making them ideal peroxidase (POD)-like substitutes for immunoassay applications. However, specific catalytic progress is hindered by the excessive orbital overlaps between Pt and oxygen-based intermediates. Herein, a highly efficient mesoporous medium-entropy alloy (m-MEA) nanozyme is reported to selectively enhance POD activity through synergy interaction of multiple elements. Such synergy reduces the 5 orbital energy of Pt, thereby lowering antibonding energy levels and weakening - orbital hybridization between the O 2 and Pt 5. The reduced orbital overlap lowers energetic barriers and suppresses the excessive adsorption of oxygenated intermediates (*OH/*OH), as well as weakens oxygen poisoning of active sites. In addition, the exposed mesoporous structure of m-MEA nanozyme ensures accessible active sites, resulting in a high POD specific activity of 304 ± 1.69 U mg, which is 6.58- and 507-folds higher than that of mesoporous Pt and nonporous MEA nanozymes, respectively. The m-MEA-based immunoassay platform has been utilized for the detection of prostate-specific antigens, achieving an exceptionally low detection limit of 1.20 pg mL, surpassing the sensitivity of traditional enzyme-linked assays.
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http://dx.doi.org/10.1021/acsnano.5c06349 | DOI Listing |
Water Res
September 2025
State Key Laboratory of Soil Pollution Control and Safety, Department of Environmental Science, Zhejiang University, Hangzhou 310058, China; Future Environment Laboratory, Innovation Center of Yangtze River Delta, Zhejiang University, Jiaxing 314100, China. Electronic address:
Accelerating the rate-limiting surface Fe(III)/Fe(II) redox cycling is pivotal for efficient iron-mediated Fenton-like decontamination, yet conventional reductants (e.g., toxic hydroxylamine, thiosulfate) suffer from secondary toxicity, self-quenching, and heavy metal leaching.
View Article and Find Full Text PDFAdv Mater
September 2025
School of Materials Science and Chemical Engineering, Harbin University of Science and Technology, Harbin, 150080, China.
The polysulfide shuttling and sluggish sulfur redox kinetics hinder the commercialization of lithium-sulfur (Li-S) batteries. Herein, the fabrication of phosphorus (P)-doped iron telluride (FeTe) nanoparticles with engineered Te vacancies anchored on nitrogen (N)-doped carbon (C) (P-FeTe@NC) is presented as a multifunctional sulfur host. Theoretical and experimental analyses show that Te vacancies create electron-deficient Fe sites, which chemically anchor polysulfides through enhanced Fe─S covalent interactions.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Key Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, P. R. China.
Facing the massive energy consumption of over 200 TWh y of chlor-alkali industry, developing high-activity and durable non-precious CER (chlorine evolution reaction) catalysts is urgently needed to address the high overpotentials and suppress the dissolution high-valance metal species. Herein, a carbon quantum dots functionalized trimetallic Fe/Co/Ni spinel oxide nanotube architecture (FCNO@CQDs) is constructed, featuring t-to-π* π-backbonding for dramatically enhanced CER activity and stability. The reverse electron flow from Co d-obritals to the vacant CQDs' π* orbitals can upshift the d-band center for enhanced intermediate adsorption, while stabilizing high-valent Co centers via increased bond order.
View Article and Find Full Text PDFPhys Chem Chem Phys
September 2025
Institute of Materials Intelligent Technology, Liaoning Academy of Materials, Shenyang 110004, China.
Axial ligand engineering is a promising strategy to enhance the performance of single-atom catalysts (SACs) in electrocatalysis. However, a single non-metallic axial coordination atom linked to monolayer SACs (MSACs) often exhibits insufficient stability. In this work, we designed a series of bilayer SACs (BSACs) with vertically stacked FeN and MN (M = Sc-Zn) layers bridged by axial non-metallic atoms (C, N, O, P, S, and Se).
View Article and Find Full Text PDFChem Sci
August 2025
ARC Ctr. Excellence Electromat Sci., University of Wollongong Innovation Campus, North Wollongong NSW 2500 Australia.
Hard carbon is the most commercially viable anode material for sodium-ion batteries (SIBs), yet its application in ester-based electrolytes is hindered by sluggish interfacial ion diffusion and limited sodium nucleation kinetics. After comprehensive evaluation, an interfacial chemistry regulation strategy was proposed based on orbital hybridization between bismuth and electrolyte ions, which was realized through the introduction of ammonium bismuth citrate. The surface bismuth particles regulate the formation of a NaF-rich SEI through improved anion affinity.
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