Pd@Fe2O3 Superparticles with Enhanced Peroxidase Activity by Solution Phase Epitaxial Growth
Abstract: Compared to conventional deposition techniques for the epitaxial growth of metal oxide structures on a bulk metal substrate, wet-chemical synthesis based on a dispersible template offers advantages such as low cost, high throughput, and the capability to prepare metal/metal oxide nanostructures with controllable size and morphology. However, the synthesis of such organized multicomponent architectures is difficult because the size and morphology of the components are dictated by the interplay of interfacial strain and facet-specific reactivity. Here we show that solution-processable two-dimensional Pd nanotetrahedra and nanoplates can be used to direct the epitaxial growth of γ-Fe2O3 nanorods. The interfacial strain at the Pd−γ-Fe2O3 interface is minimized by the formation of an FexPd “buffer phase” facilitating the growth of the nanorods. The γ-Fe2O3 nanorods show a (111) orientation on the Pd(111) surface. Importantly, the Pd@γ-Fe2O3 hybrid nanomaterials exhibit enhanced peroxidase activity compared to ...
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TL;DR: A new class of single-atom nanozymes with atomically dispersed enzyme-like active sites in nanomaterials is discovered, which significantly enhanced catalytic performance, and the underlying mechanism is uncovered.
Abstract: Conventional nanozyme technologies face formidable challenges of intricate size-, composition-, and facet-dependent catalysis and inherently low active site density. We discovered a new class of single-atom nanozymes with atomically dispersed enzyme-like active sites in nanomaterials, which significantly enhanced catalytic performance, and uncovered the underlying mechanism. With oxidase catalysis as a model reaction, experimental studies and theoretical calculations revealed that single-atom nanozymes with carbon nanoframe–confined FeN5 active centers (FeN5 SA/CNF) catalytically behaved like the axial ligand–coordinated heme of cytochrome P450. The definite active moieties and crucial synergistic effects endow FeN5 SA/CNF with a clear electron push-effect mechanism, as well as the highest oxidase-like activity among other nanozymes (the rate constant is 70 times higher than that of commercial Pt/C) and versatile antibacterial applications. These suggest that the single-atom nanozymes have great potential to become the next-generation nanozymes.
486 citations
TL;DR: This review will introduce the enzymatic features of iron oxide nanozyme (IONzyme), and summarize its novel applications in biomedicine.
Abstract: Iron oxide nanoparticles have been widely used in many important fields due to their excellent nanoscale physical properties, such as magnetism/superparamagnetism. They are usually assumed to be biologically inert in biomedical applications. However, iron oxide nanoparticles were recently found to also possess intrinsic enzyme-like activities, and are now regarded as novel enzyme mimetics. A special term, "Nanozyme", has thus been coined to highlight the intrinsic enzymatic properties of such nanomaterials. Since then, iron oxide nanoparticles have been used as nanozymes to facilitate biomedical applications. In this review, we will introduce the enzymatic features of iron oxide nanozyme (IONzyme), and summarize its novel applications in biomedicine.
377 citations
TL;DR: This review systematically summarized the studies on the structure–activity relationship of nanozymes in recent years, aiming to illustrate the catalytic mechanism of nanoZymes and clarify the key factors regulating their behavior, so as to provide ideas and inspiration for the de novo design of nano zymes.
289 citations
TL;DR: A photosensitized metal-organic framework (PSMOF) is developed by using a derivative of Ru(bpy)32+ with stronger visible-light absorption as a PS linker that exhibited excellent oxidase-like activity, which could be modulated by switching light on and off.
Abstract: Nanomaterials with enzyme-like characteristics (nanozymes) have been developed to mimic enzymes because of their low cost, high stability, and large-scale production. By using light as an external stimulation, one can modulate nanozymes' catalytic activities with controlled spatial and temporal precision. A few inorganic photoactive materials have been investigated to construct light-responsive oxidase-like nanozymes. However, these materials suffered from limited absorbance of visible light. To address this challenge, herein we have developed a photosensitized metal-organic framework (PSMOF) by using a derivative of Ru(bpy)32+ with stronger visible-light absorption as a PS linker. The PSMOF exhibited excellent oxidase-like activity, which could be modulated by switching light on and off. Moreover, the PSMOF was used to detect glutathione levels in both normal and cancer cells with good selectivity and high sensitivity. This study not only provides a smart strategy to modulate nanozymes' activities but also broadens the sensing applications of nanozymes.
128 citations
TL;DR: It is predicted that INAzymes with superior activities, specificity, and stability will enrich the research of nanozymes and pave new ways in designing multifunctional nanozzyme strategies, covering from synthetic strategies to versatile applications in biodetection and therapeutics.
116 citations
References
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TL;DR: A comprehensive review of 1D nanostructures can be found in this article, where the authors provide a comprehensive overview of current research activities that concentrate on one-dimensional (1D) nanostructure (wires, rods, belts and tubes).
Abstract: This article provides a comprehensive review of current research activities that concentrate on one-dimensional (1D) nanostructures—wires, rods, belts, and tubes—whose lateral dimensions fall anywhere in the range of 1 to 100 nm. We devote the most attention to 1D nanostructures that have been synthesized in relatively copious quantities using chemical methods. We begin this article with an overview of synthetic strategies that have been exploited to achieve 1D growth. We then elaborate on these approaches in the following four sections: i) anisotropic growth dictated by the crystallographic structure of a solid material; ii) anisotropic growth confined and directed by various templates; iii) anisotropic growth kinetically controlled by supersaturation or through the use of an appropriate capping reagent; and iv) new concepts not yet fully demonstrated, but with long-term potential in generating 1D nanostructures. Following is a discussion of techniques for generating various types of important heterostructured nanowires. By the end of this article, we highlight a range of unique properties (e.g., thermal, mechanical, electronic, optoelectronic, optical, nonlinear optical, and field emission) associated with different types of 1D nanostructures. We also briefly discuss a number of methods potentially useful for assembling 1D nanostructures into functional devices based on crossbar junctions, and complex architectures such as 2D and 3D periodic lattices. We conclude this review with personal perspectives on the directions towards which future research on this new class of nanostructured materials might be directed.
8,259 citations
TL;DR: It is reported that magnetite nanoparticles in fact possess an intrinsic enzyme mimetic activity similar to that found in natural peroxidases, which are widely used to oxidize organic substrates in the treatment of wastewater or as detection tools.
Abstract: Nanoparticles containing magnetic materials, such as magnetite (Fe3O4), are particularly useful for imaging and separation techniques. As these nanoparticles are generally considered to be biologically and chemically inert, they are typically coated with metal catalysts, antibodies or enzymes to increase their functionality as separation agents. Here, we report that magnetite nanoparticles in fact possess an intrinsic enzyme mimetic activity similar to that found in natural peroxidases, which are widely used to oxidize organic substrates in the treatment of wastewater or as detection tools. Based on this finding, we have developed a novel immunoassay in which antibody-modified magnetite nanoparticles provide three functions: capture, separation and detection. The stability, ease of production and versatility of these nanoparticles makes them a powerful tool for a wide range of potential applications in medicine, biotechnology and environmental chemistry.
4,500 citations
TL;DR: This review discusses various nanomaterials that have been explored to mimic different kinds of enzymes and covers their kinetics, mechanisms and applications in numerous fields, from biosensing and immunoassays, to stem cell growth and pollutant removal.
Abstract: Over the past few decades, researchers have established artificial enzymes as highly stable and low-cost alternatives to natural enzymes in a wide range of applications. A variety of materials including cyclodextrins, metal complexes, porphyrins, polymers, dendrimers and biomolecules have been extensively explored to mimic the structures and functions of naturally occurring enzymes. Recently, some nanomaterials have been found to exhibit unexpected enzyme-like activities, and great advances have been made in this area due to the tremendous progress in nano-research and the unique characteristics of nanomaterials. To highlight the progress in the field of nanomaterial-based artificial enzymes (nanozymes), this review discusses various nanomaterials that have been explored to mimic different kinds of enzymes. We cover their kinetics, mechanisms and applications in numerous fields, from biosensing and immunoassays, to stem cell growth and pollutant removal. We also summarize several approaches to tune the activities of nanozymes. Finally, we make comparisons between nanozymes and other catalytic materials (other artificial enzymes, natural enzymes, organic catalysts and nanomaterial-based catalysts) and address the current challenges and future directions (302 references).
2,951 citations
TL;DR: Pd-Pt bimetallic nanodendrites consisting of a dense array of Pt branches on a Pd core by reducing K2PtCl4 with L-ascorbic acid in the presence of uniform Pd nanocrystal seeds in an aqueous solution showed relatively large surface areas and particularly active facets toward the oxygen reduction reaction (ORR), the rate-determining step in a proton-exchange membrane fuel cell.
Abstract: Controlling the morphology of Pt nanostructures can provide a great opportunity to improve their catalytic properties and increase their activity on a mass basis. We synthesized Pd-Pt bimetallic nanodendrites consisting of a dense array of Pt branches on a Pd core by reducing K2PtCl4 with L-ascorbic acid in the presence of uniform Pd nanocrystal seeds in an aqueous solution. The Pt branches supported on faceted Pd nanocrystals exhibited relatively large surface areas and particularly active facets toward the oxygen reduction reaction (ORR), the rate-determining step in a proton-exchange membrane fuel cell. The Pd-Pt nanodendrites were two and a half times more active on the basis of equivalent Pt mass for the ORR than the state-of-the-art Pt/C catalyst and five times more active than the first-generation supportless Pt-black catalyst.
2,695 citations
TL;DR: It is observed that the slow rate of the reaction along with the shape directing effect of the constituents of the extract are responsible for the formation of single crystalline gold nanotriangles.
Abstract: Biogenic gold nanotriangles and spherical silver nanoparticles were synthesized by a simple procedure using Aloe vera leaf extract as the reducing agent. This procedure offers control over the size of the gold nanotriangle and thereby a handle to tune their optical properties, particularly the position of the longitudinal surface plasmon resonance. The kinetics of gold nanotriangle formation was followed by UV-vis-NIR absorption spectroscopy and transmission electron microscopy (TEM). The effect of reducing agent concentration in the reaction mixture on the yield and size of the gold nanotriangles was studied using transmission electron microscopy. Monitoring the formation of gold nanotriangles as a function of time using TEM reveals that multiply twinned particles (MTPs) play an important role in the formation of gold nanotriangles. It is observed that the slow rate of the reaction along with the shape directing effect of the constituents of the extract are responsible for the formation of single crystalline gold nanotriangles. Reduction of silver ions by Aloe vera extract however, led to the formation of spherical silver nanoparticles of 15.2 nm +/- 4.2 nm size.
1,801 citations