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Recent Advances in the Use of Iron–Gold Hybrid Nanoparticles for Biomedical Applications Nanomaterials 2021, 11, X for PEER REVIEW 2 of 25

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Recent Advances in the Use of Iron–Gold Hybrid Nanoparticles for Biomedical Applications Nanomaterials 2021, 11, X for PEER REVIEW 2 of 25 nanomaterials Review Recent Advances in the Use of Iron–Gold Hybrid Nanoparticles for Biomedical Applications Nanomaterials 2021, 11, x FOR PEER REVIEW 2 of 25 Mariam Abdulaziz M. Tarkistani, Varsha Komalla and Veysel Kayser * (http://creativecommons.org/licenses Sydney Pharmacy School, Faculty of Medicine and Health, The University of Sydney, Camperdown, NSW Sydney Pharmacy School, Faculty of Medicine and Health, The University of Sydney, /by/4.0/). 2006, Australia; [email protected] (M.A.M.T.); [email protected] (V.K.) * Correspondence:Camperdown, [email protected]; NSW 2006, Australia; [email protected] Tel.: +61-2-9351-3391 (M.A.M.T.); [email protected] (V.K.) * Correspondence: [email protected]; Tel.: +61-2-9351-3391 Abstract: Recently, there has been an increased interest in iron–gold-based hybrid nanostructures, due to their combined outstanding optical and magnetic properties resulting from the usage of two Abstract: Recently, there has been an increased interest in iron–gold-based hybrid nanostructures, separate metals. The synthesis of these nanoparticles involves thermal decomposition and due to their combined outstanding optical and magnetic properties resulting from the usage of modification of their surfaces using a variety of different methods, which are discussed in this two separate metals. The synthesis of these nanoparticles involves thermal decomposition and review. In addition, different forms such as core–shell, dumbbell, flower, octahedral, star, rod, and modification of their surfaces using a variety of different methods, which are discussed in this review. Janus-shaped hybrids are discussed, and their unique properties are highlighted. Studies on In addition, different forms such as core–shell, dumbbell, flower, octahedral, star, rod, and Janus- combining optical response in the near-infrared window and magnetic properties of iron–gold- shaped hybrids are discussed, and their unique properties are highlighted. Studies on combining based hybrid nanoparticles as multifunctional nanoprobes for drug delivery, magnetic– optical response in the near-infrared window and magnetic properties of iron–gold-based hybrid photothermal heating as well as contrast agents during magnetic and optical imaging and nanoparticles as multifunctional nanoprobes for drug delivery, magnetic–photothermal heating magnetically-assisted optical biosensing to detect traces of targeted analytes inside the body has as well as contrast agents during magnetic and optical imaging and magnetically-assisted optical been reviewed. biosensing to detect traces of targeted analytes inside the body has been reviewed. Keywords: nanomaterials; nanohybrids; magnetic plasmonic nanoparticles; gold nanoparticles; Keywords: nanomaterials; nanohybrids; magnetic plasmonic nanoparticles; gold nanoparticles; iron iron oxide nanoparticles; surface functionalization; biomedical applications oxide nanoparticles; surface functionalization; biomedical applications Citation: Tarkistani, M.A.M.; Komalla, V.; Kayser, V. Recent Advances in the Use of Iron–Gold 1. Introduction Hybrid Nanoparticles for Biomedical 1. Introduction Applications. Nanomaterials 2021, 11, Nanoparticles (NPs) usually possess distinct chemical and physical properties Nanoparticles (NPs) usually possess distinct chemical and physical properties com- 1227. https://doi.org/10.3390/compared to macromolecules, mainly due to their smaller sizes. These properties include pared to macromolecules, mainly due to their smaller sizes. These properties include nano11051227 conductance, magnetism, chemical interactions, and optical properties [1] as well as conductance, magnetism, chemical interactions, and optical properties [1] as well as surface surface area, shape, magnetism, and permeability, affecting their characteristics and Academic Editor: Magdalena O´cwieja area, shape, magnetism, and permeability, affecting their characteristics and making them makingunique them unique in their in functioning their functioning [2]. [2]. NPs areNPs ubiquitously are ubiquitously present present around around us in us nature, in nature, for forinstance, instance, in inour our food, food, e.g., e.g., casein Received: 8 April 2021 casein micelles [3]; in the biological matter such as viruses [4]; and other environmental Accepted: 28 April 2021 micelles [3]; in the biological matter such as viruses [4]; and other environmental sources sources such as ash, sand, and dust [5]. Due to their smaller sizes, NPs can pass through Published: 6 May 2021 such as ash, sand, and dust [5]. Due to their smaller sizes, NPs can pass through the the biologicalbiological membranes membranes and and interact interact actively actively with with cell cell organelles organelles and and cellular cellular structures structures such such as proteins, DNA, and RNA [1], and hence, they can be used as delivery vehicles for Publisher’s Note: MDPI stays neutral as proteins, DNA, and RNA [1], and hence, they can be used as delivery vehicles for drugs with regard to jurisdictional claimsdrugs in toto improve improve their their circulation circulation time time and and bioavailability bioavailability [6]. [6]. published maps and institutional affil-Cancer Canceris one of is the one major of the causes major of causes death of worldwide. death worldwide. Patients, Patients, when treated when treatedwith with iations. traditionaltraditional chemotherapy, chemotherapy, suffer from suffer various from variousside effects, side effects,as small as molecule small molecule drugs are drugs are non-selectivenon-selective and affect and normal affect normalcells or cellstissues or tissuesalong with along cancerous with cancerous cells [7]. cells Within [7]. Within cancerouscancerous cells, the cells, small the size small of NPs size ofcan NPs enhance can enhance the concentration the concentration of the drugs of the inside drugs inside the tumorthe by tumor preferential by preferential accumu accumulationlation due to the due large to the pore large size pore of neo-vasculatures size of neo-vasculatures and and Copyright: © 2021 by the authors.defectivedefective lymphatic lymphatic system, system,which is which defined is definedas an enhanced as an enhanced penetration penetration and retention and retention Licensee MDPI, Basel, Switzerland.effect [8].effect [8]. This article is an open access article DifferentDifferent types typesof NPs of NPsthat thatare arefrequently frequently used used in in medicine includeinclude metallic metallic nanopar- distributed under the termsnanoparticles, and ticles, dendrimers,dendrimers, liposomes,liposomes, carbon nanotubes, and nanocrystals [9]. [9]. Among Among these, conditions of the Creative Commonsthese, magneticmagnetic iron iron oxide oxide NPs, NPs, particularly particularly maghemite (ɤ-Fe2OO33)) and and magnetite magnetite (Fe 3OO44)) with a Attribution (CC BY) license (https://with a size ofof lessless than than 20 20 nm, nm, exhibit exhibit superparamagnetic superparamagnetic behavior. behavior. These These structural structural properties creativecommons.org/licenses/by/propertiesmake make the the NPs NPs ideal ideal for severalfor several biomedical biomedical applications, applications, including including magnetic magnetic resonance 4.0/). resonance imaging (MRI) [10], magnetically guided drug delivery [11], magnetic hyperthermia [12], and biosensors [13]. On the other hand, gold NPs are the most widely used and studied due to their easy preparation, high stability, well-established surface functionalization chemistry, and Nanomaterials 2021, 11, 1227. https://doi.org/10.3390/nano11051227 https://www.mdpi.com/journal/nanomaterials unique optical properties. Furthermore, gold NPs exhibit localized surface plasmon resonance providing efficient absorption and scattering of light at specific wavelengths. These wavelengths can be tuned according to their shapes and sizes. This property makes gold NPs an ideal choice as calorimetric sensors and nanoprobes for surface-enhanced Raman spectroscopy (SERS) and labels for imaging or photothermal agents for cancer Nanomaterials 2021, 11, 1227 2 of 23 imaging (MRI) [10], magnetically guided drug delivery [11], magnetic hyperthermia [12], and biosensors [13]. On the other hand, gold NPs are the most widely used and studied due to their easy preparation, high stability, well-established surface functionalization chemistry, and unique optical properties. Furthermore, gold NPs exhibit localized surface plasmon reso- nance providing efficient absorption and scattering of light at specific wavelengths. These wavelengths can be tuned according to their shapes and sizes. This property makes gold NPs an ideal choice as calorimetric sensors and nanoprobes for surface-enhanced Raman spectroscopy (SERS) and labels for imaging or photothermal agents for cancer therapy. Gold NPs can be easily functionalized using thiols and amines, while iron-oxide NPs can be functionalized using catechols, silanes, diol carboxylic groups, or amines [14,15]. In the last few years, new composite nanostructures have attracted considerable atten- tion, particularly those based on bimodal metals, such as gold (Au) and iron (Fe3O4). More specifically, since Au possesses excellent properties as mentioned earlier, the construction of Au–iron oxide-based nanostructures would be extremely valuable providing complemen- tary modalities for accurate imaging or diagnosis or offer an additional therapeutic avenue for enhanced cancer treatment,
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