Research

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11 pages, 1150 KiB

Open AccessFeature PaperArticle

Multivariate Analysis of Protein–Nanoparticle Binding Data Reveals a Selective Effect of Nanoparticle Material on the Formation of Soft Corona

by Susannah Emily Cornwell, Sarah Ogechukwu Okocha and Enrico Ferrari

Nanomaterials 2023, 13(21), 2901; https://doi.org/10.3390/nano13212901 - 04 Nov 2023

Viewed by 949

Abstract

When nanoparticles are introduced into the bloodstream, plasma proteins accumulate at their surface, forming a protein corona. This corona affects the properties of intravenously administered nanomedicines. The firmly bound layer of plasma proteins in direct contact with the nanomaterial is called the “hard [...] Read more.

When nanoparticles are introduced into the bloodstream, plasma proteins accumulate at their surface, forming a protein corona. This corona affects the properties of intravenously administered nanomedicines. The firmly bound layer of plasma proteins in direct contact with the nanomaterial is called the “hard corona”. There is also a “soft corona” of loosely associated proteins. While the hard corona has been extensively studied, the soft corona is less understood due to its inaccessibility to analytical techniques. Our study used dynamic light scattering to determine the dissociation constant and thickness of the protein corona formed in solutions of silica or gold nanoparticles mixed with serum albumin, transferrin or prothrombin. Multivariate analysis showed that the nanoparticle material had a greater impact on binding properties than the protein type. Serum albumin had a distinct binding pattern compared to the other proteins tested. This pilot study provides a blueprint for future investigations into the complexity of the soft protein corona, which is key to developing nanomedicines. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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23 pages, 4588 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Targeting Ultrasmall Gold Nanoparticles with cRGD Peptide Increases the Uptake and Efficacy of Cytotoxic Payload

by Richard D. Perrins, Lee-Anne McCarthy, Angela Robinson, Kelly L. Spry, Valentin Cognet, Avelino Ferreira, John Porter, Cristina Espinosa Garcίa, Miguel Ángel Rodriguez, Diana Lopez, Ibon Perera, Kelly Conlon, Africa Barrientos, Tom Coulter, Alessandro Pace, Sarah J. M. Hale, Enrico Ferrari and Csanad Z. Bachrati

Nanomaterials 2022, 12(22), 4013; https://doi.org/10.3390/nano12224013 - 15 Nov 2022

Cited by 5 | Viewed by 2332

Abstract

Cyclic arginyl-glycyl-aspartic acid peptide (cRGD) peptides show a high affinity towards αVβ3 integrin, a receptor overexpressed in many cancers. We aimed to combine the versatility of ultrasmall gold nanoparticles (usGNP) with the target selectivity of cRGD peptide for the directed delivery of a [...] Read more.

Cyclic arginyl-glycyl-aspartic acid peptide (cRGD) peptides show a high affinity towards αVβ3 integrin, a receptor overexpressed in many cancers. We aimed to combine the versatility of ultrasmall gold nanoparticles (usGNP) with the target selectivity of cRGD peptide for the directed delivery of a cytotoxic payload in a novel design. usGNPs were synthesized with a modified Brust-Schiffrin method and functionalized via amide coupling and ligand exchange and their uptake, intracellular trafficking, and toxicity were characterized. Our cRGD functionalized usGNPs demonstrated increased cellular uptake by αVβ3 integrin expressing cells, are internalized via clathrin-dependent endocytosis, accumulated in the lysosomes, and when loaded with mertansine led to increased cytotoxicity. Targeting via cRGD functionalization provides a mechanism to improve the efficacy, tolerability, and retention of therapeutic GNPs. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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16 pages, 3721 KiB

Open AccessArticle

AC/DC Thermal Nano-Analyzer Compatible with Bulk Liquid Measurements

by Yaroslav Odarchenko, Anna Kaźmierczak-Bałata, Jerzy Bodzenta, Enrico Ferrari and Mikhail Soloviev

Nanomaterials 2022, 12(21), 3799; https://doi.org/10.3390/nano12213799 - 28 Oct 2022

Viewed by 1440

Abstract

Nanocalorimetry, or thermal nano-analysis, is a powerful tool for fast thermal processing and thermodynamic analysis of materials at the nanoscale. Despite multiple reports of successful applications in the material sciences to study phase transitions in metals and polymers, thermodynamic analysis of biological systems [...] Read more.

Nanocalorimetry, or thermal nano-analysis, is a powerful tool for fast thermal processing and thermodynamic analysis of materials at the nanoscale. Despite multiple reports of successful applications in the material sciences to study phase transitions in metals and polymers, thermodynamic analysis of biological systems in their natural microenvironment has not been achieved yet. Simply scaling down traditional calorimetric techniques, although beneficial for material sciences, is not always appropriate for biological objects, which cannot be removed out of their native biological environment or be miniaturized to suit instrument limitations. Thermal analysis at micro- or nano-scale immersed in bulk liquid media has not yet been possible. Here, we report an AC/DC modulated thermal nano-analyzer capable of detecting nanogram quantities of material in bulk liquids. The detection principle used in our custom-build instrument utilizes localized heat waves, which under certain conditions confine the measurement area to the surface layer of the sample in the close vicinity of the sensing element. To illustrate the sensitivity and quantitative capabilities of the instrument we used model materials with detectable phase transitions. Here, we report ca. 10⁶ improvement in the thermal analysis sensitivity over a traditional DSC instrument. Interestingly, fundamental thermal properties of the material can be determined independently from heat flow in DC (direct current) mode, by using the AC (alternating current) component of the modulated heat in AC/DC mode. The thermal high-frequency AC modulation mode might be especially useful for investigating thermal transitions on the surface of material, because of the ability to control the depth of penetration of AC-modulated heat and hence the depth of thermal sensing. The high-frequency AC mode might potentially expand the range of applications to the surface analysis of bulk materials or liquid-solid interfaces. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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9 pages, 2500 KiB

Open AccessArticle

Synthesis of Highly Monodisperse Nickel and Nickel Phosphide Nanoparticles

by Hyungjin Cho, Nohyun Lee and Byung Hyo Kim

Nanomaterials 2022, 12(18), 3198; https://doi.org/10.3390/nano12183198 - 14 Sep 2022

Cited by 5 | Viewed by 2064

Abstract

Nickel and nickel phosphide nanoparticles are highly useful in various fields, owing to their catalytic and magnetic properties. Although several synthetic protocols to produce nickel and nickel phosphide nanoparticles have been previously proposed, controllable synthesis of nanoparticles using these methods is challenging. Herein, [...] Read more.

Nickel and nickel phosphide nanoparticles are highly useful in various fields, owing to their catalytic and magnetic properties. Although several synthetic protocols to produce nickel and nickel phosphide nanoparticles have been previously proposed, controllable synthesis of nanoparticles using these methods is challenging. Herein, we synthesized highly monodisperse nickel and nickel phosphide nanoparticles via thermal decomposition of nickel–oleylamine–phosphine complexes in organic solvents. The size and composition of the nickel and nickel phosphide nanoparticles were easily controlled by changing the aging temperature, precursor concentration, and phosphine surfactant type. Large-sized monodisperse nickel nanoparticles obtained using our method were successfully applied for the purification of histidine-tagged proteins. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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12 pages, 3032 KiB

Open AccessArticle

Regulation of Antimicrobial Effect of Hemicyanine-Based Photosensitizer via Supramolecular Assembly

by Huanxiang Yuan, Shaochuan Jia, Zelin Li, Jian Liu, Xiaoyu Wang and Ruilian Qi

Nanomaterials 2022, 12(17), 2905; https://doi.org/10.3390/nano12172905 - 24 Aug 2022

Cited by 2 | Viewed by 1224

Abstract

An intelligent “antimicrobial switch” has been constructed to reduce prolonged exposure of pathogenic bacteria to antibiotics, which could reversibly “turn off” or “turn on” the antimicrobial activity of hemicyanines through self-assembly or dis-assembly of cucurbit[7]uril (CB[7]). This assembly effectively inhibited the production of [...] Read more.

An intelligent “antimicrobial switch” has been constructed to reduce prolonged exposure of pathogenic bacteria to antibiotics, which could reversibly “turn off” or “turn on” the antimicrobial activity of hemicyanines through self-assembly or dis-assembly of cucurbit[7]uril (CB[7]). This assembly effectively inhibited the production of ROS under light, shielding the active site of hemicyanines and achieving on-demand antimicrobial ability. Moreover, CB[7] differentially inhibits ROS of molecules with different alkyl chain lengths, which provided reference for the subsequent design of materials with antimicrobial activity regulation, and could effectively delay or even prevent the development of pathogens resistance. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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10 pages, 2063 KiB

Open AccessArticle

Detailed Calorimetric Analysis of Mixed Micelle Formation from Aqueous Binary Surfactants for Design of Nanoscale Drug Carriers

by Ádám Juhász, László Seres, Norbert Varga, Ditta Ungor, Marek Wojnicki and Edit Csapó

Nanomaterials 2021, 11(12), 3288; https://doi.org/10.3390/nano11123288 - 03 Dec 2021

Cited by 5 | Viewed by 1660

Abstract

While numerous papers have been published according to the binary surfactant mixtures, only a few articles provide deeper information on the composition dependence of the micellization, and even less work attempts to apply the enhanced feature of the mixed micelles. The most important [...] Read more.

While numerous papers have been published according to the binary surfactant mixtures, only a few articles provide deeper information on the composition dependence of the micellization, and even less work attempts to apply the enhanced feature of the mixed micelles. The most important parameter of the self-assembled surfactants is the critical micelle concentration (cmc), which quantifies the tendency to associate, and provides the Gibbs energy of micellization. Several techniques are known for determining the cmc, but the isothermal titration calorimetry (ITC) can be used to measure both cmc and enthalpy change (Δ_micH) accompanying micelle formation. Outcomes of our calorimetric investigations were evaluated using a self-developed routine for handling ITC data and the thermodynamic parameters of mixed micelle formation were obtained from the nonlinear modelling of temperature- and composition- dependent enthalpograms. In the investigated temperature and micelle mole fractions interval, we observed some intervals where the cmc is lower than the ideal mixing model predicted value. These equimolar binary surfactant mixtures showed higher solubilization ability for poorly water-soluble model drugs than their individual compounds. Thus, the rapid and fairly accurate calorimetric analysis of mixed micelles can lead to the successful design of a nanoscale drug carrier. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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14 pages, 2890 KiB

Open AccessArticle

Designing Functionalized Polyelectrolyte Microcapsules for Cancer Treatment

by Daria Kalenichenko, Galina Nifontova, Alexander Karaulov, Alyona Sukhanova and Igor Nabiev

Nanomaterials 2021, 11(11), 3055; https://doi.org/10.3390/nano11113055 - 13 Nov 2021

Cited by 10 | Viewed by 2525

Abstract

The engineering of delivery systems for drugs and contrasting labels ensuring the simultaneous imaging and treatment of malignant tumors is an important hurdle in developing new tools for cancer therapy and diagnosis. Polyelectrolyte microcapsules (MCs), formed by nanosized interpolymer complexes, represent a promising [...] Read more.

The engineering of delivery systems for drugs and contrasting labels ensuring the simultaneous imaging and treatment of malignant tumors is an important hurdle in developing new tools for cancer therapy and diagnosis. Polyelectrolyte microcapsules (MCs), formed by nanosized interpolymer complexes, represent a promising platform for the designing of multipurpose agents, functionalized with various components, including high- and low-molecular-weight substances, metal nanoparticles, and organic fluorescent dyes. Here, we have developed size-homogenous MCs with different structures (core/shell and shell types) and microbeads containing doxorubicin (DOX) as a model anticancer drug, and fluorescent semiconductor nanocrystals (quantum dots, QDs) as fluorescent nanolabels. In this study, we suggest approaches to the encapsulation of DOX at different stages of the MC synthesis and describe the optimal conditions for the optical encoding of MCs with water-soluble QDs. The results of primary characterization of the designed microcarriers, including particle analysis, the efficacy of DOX and QDs encapsulation, and the drug release kinetics are reported. The polyelectrolyte MCs developed here ensure a modified (prolonged) release of DOX, under conditions close to normal and tumor tissues; they possess a bright fluorescence that paves the way to their exploitation for the delivery of antitumor drugs and fluorescence imaging. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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13 pages, 1834 KiB

Open AccessArticle

Assessing Fast Structure Formation Processes in Isotactic Polypropylene with a Combination of Nanofocus X-ray Diffraction and In Situ Nanocalorimetry

by Yaroslav Odarchenko, Martin Rosenthal, Jaime J. Hernandez, David Doblas, Emanuela Di Cola, Mikhail Soloviev and Dimitri A. Ivanov

Nanomaterials 2021, 11(10), 2652; https://doi.org/10.3390/nano11102652 - 09 Oct 2021

Cited by 6 | Viewed by 1887

Abstract

A combination of in situ nanocalorimetry with simultaneous nanofocus 2D Wide-Angle X-ray Scattering (WAXS) was used to study polymorphic behaviour and structure formation in a single micro-drop of isotactic polypropylene (iPP) with defined thermal history. We were able to generate, detect, and characterize [...] Read more.

A combination of in situ nanocalorimetry with simultaneous nanofocus 2D Wide-Angle X-ray Scattering (WAXS) was used to study polymorphic behaviour and structure formation in a single micro-drop of isotactic polypropylene (iPP) with defined thermal history. We were able to generate, detect, and characterize a number of different iPP morphologies using our custom-built ultrafast chip-based nanocalorimetry instrument designed for use with the European Synchrotron Radiation Facility (ESRF) high intensity nanofocus X-ray beamline facility. The detected iPP morphologies included monoclinic alpha-phase crystals, mesophase, and mixed morphologies with different mesophase/crystalline compositional ratios. Monoclinic crystals formed from the mesophase became unstable at heating rates above 40 K s⁻¹ and showed melting temperatures as low as ~30 K below those measured for iPP crystals formed by slow cooling. We also studied the real-time melt crystallization of nanogram-sized iPP samples. Our analysis revealed a mesophase nucleation time of around 1 s and the co-existence of mesophase and growing disordered crystals at high supercooling ≤328 K. The further increase of the iPP crystallization temperature to 338 K changed nucleation from homogeneous to heterogeneous. No mesophase was detected above 348 K. Low supercooling (≥378 K) led to the continuous growth of the alpha-phase crystals. In conclusion, we have, for the first time, measured the mesophase nucleation time of supercooled iPP melted under isothermal crystallization conditions using a dedicated experimental setup designed to allow simultaneous ultrafast chip-based nanocalorimetry and nanofocus X-ray diffraction analyses. We also provided experimental evidence that upon heating, the mesophase converts directly into thermodynamically stable monoclinic alpha-phase crystals via perfection and reorganization and not via partial melting. The complex phase behaviour of iPP and its dependence on both crystallization temperature and time is presented here using a time–temperature–transformation (TTT) diagram. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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11 pages, 2375 KiB

Open AccessArticle

Sulfur-Doped BiOCl with Enhanced Light Absorption and Photocatalytic Water Oxidation Activity

by Ruilian Qi, Jian Liu, Huanxiang Yuan and Yu Yu

Nanomaterials 2021, 11(9), 2221; https://doi.org/10.3390/nano11092221 - 28 Aug 2021

Cited by 11 | Viewed by 2548

Abstract

Photocatalysis is a powerful strategy to address energy and environmental concerns. Sulfur-doped BiOCl was prepared through a facial hydrothermal method to improve the photocatalytic performance. Experimental results and theoretical calculations demonstrated that the band structure of the sulfur-doped BiOCl was optimally regulated and [...] Read more.

Photocatalysis is a powerful strategy to address energy and environmental concerns. Sulfur-doped BiOCl was prepared through a facial hydrothermal method to improve the photocatalytic performance. Experimental results and theoretical calculations demonstrated that the band structure of the sulfur-doped BiOCl was optimally regulated and the light absorption range was expanded. It showed excellent visible-light photocatalytic water oxidation properties with a rate of 141.7 μmol h⁻¹ g⁻¹ (almost 44 times of that of the commercial BiOCl) with Pt as co-catalyst. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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Review

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30 pages, 1839 KiB

Open AccessEditor’s ChoiceReview

Microfluidics Technology for the Design and Formulation of Nanomedicines

by Eman Jaradat, Edward Weaver, Adam Meziane and Dimitrios A. Lamprou

Nanomaterials 2021, 11(12), 3440; https://doi.org/10.3390/nano11123440 - 18 Dec 2021

Cited by 21 | Viewed by 5286

Abstract

In conventional drug administration, drug molecules cross multiple biological barriers, distribute randomly in the tissues, and can release insufficient concentrations at the desired pathological site. Controlling the delivery of the molecules can increase the concentration of the drug in the desired location, leading [...] Read more.

In conventional drug administration, drug molecules cross multiple biological barriers, distribute randomly in the tissues, and can release insufficient concentrations at the desired pathological site. Controlling the delivery of the molecules can increase the concentration of the drug in the desired location, leading to improved efficacy, and reducing the unwanted effects of the molecules under investigation. Nanoparticles (NPs), have shown a distinctive potential in targeting drugs due to their unique properties, such as large surface area and quantum properties. A variety of NPs have been used over the years for the encapsulation of different drugs and biologics, acting as drug carriers, including lipid-based and polymeric NPs. Applying NP platforms in medicines significantly improves the disease diagnosis and therapy. Several conventional methods have been used for the manufacturing of drug loaded NPs, with conventional manufacturing methods having several limitations, leading to multiple drawbacks, including NPs with large particle size and broad size distribution (high polydispersity index), besides the unreproducible formulation and high batch-to-batch variability. Therefore, new methods such as microfluidics (MFs) need to be investigated more thoroughly. MFs, is a novel manufacturing method that uses microchannels to produce a size-controlled and monodispersed NP formulation. In this review, different formulation methods of polymeric and lipid-based NPs will be discussed, emphasizing the different manufacturing methods and their advantages and limitations and how microfluidics has the capacity to overcome these limitations and improve the role of NPs as an effective drug delivery system. Full article

(This article belongs to the Special Issue Nanomaterials for Applied Nanotechnology and Nanoscience)

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