Structure and Function of Iron-Loaded Synthetic Melanin

Li, Yiwen; Xie, Yijun; Wang, Zhao; Zang, Nanzhi; Carniato, Fabio; Huang, Yongfeng; Andolina, Christopher M.; Parent, Lucas R.; Ditri, Treffly B.; Walter, Éric; Botta, Maurizio; Rinehart, Jeffrey D.; Gianneschi, Nathan C.

doi:10.1021/acsnano.6b05502

Cited by 134 publications

(147 citation statements)

References 54 publications

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“…In a typical synthesis, approximately 50 mg products could be obtained, determined by weighing after lyophilization. The Mn loading efficiency reached 10.2% wt/wt (Table S1, Supporting Information), which is much higher than previous studies 13, 29, 32, 33. It suggests more efficient synthesis and higher yields than conventional PPD approaches.…”

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confidence: 68%

Novel Intrapolymerization Doped Manganese‐Eumelanin Coordination Nanocomposites with Ultrahigh Relaxivity and Their Application in Tumor Theranostics

et al. 2018

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While magnetic resonance imaging contrast agents have potential in noninvasive image‐guided tumor treatment, further developments are needed to increase contrast, biodegradability, and safety. Here, novel engineered manganese‐eumelanin coordination nanocomposites (MnEMNPs) are developed via a facile one‐pot intrapolymerization doping (IPD) approach in aqueous solution, through simple chemical oxidation–polymerization of the 3,4‐dihydroxy‐DL‐phenylalanine precursor with potassium permanganate serving as the Mn source and an oxidant. The resulting MnEMNPs possess ultrahigh longitudinal relaxivity (r 1 value up to 60.8 mM−1 s−1 at 1.5 T) attributed to the high manganese doping efficiency (>10%) and geometrically confined conformation. Due to their high manganese chelation stability, excellent biocompatibility, and strong near‐infrared absorption, high‐performance longitudinal‐transverse (T 1 ‐T 2) dual‐modal magnetic resonance/photoacoustic imaging and photothermal tumor ablation are achieved. Furthermore, the hydrogen peroxide‐triggered decomposition behavior of MnEMNPs circumvents the poor biodegradation issue of many nanomaterials. This facile, convenient, economical, and efficient IPD strategy will open up new avenues for the development of high‐performance multifunctional theranostic nanoplatforms in bionanomedicine.

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confidence: 68%

Novel Intrapolymerization Doped Manganese‐Eumelanin Coordination Nanocomposites with Ultrahigh Relaxivity and Their Application in Tumor Theranostics

et al. 2018

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“…In our previous work, it was shown that increasing Fe(III) ion concentration within polydopamine nanoparticles led to antiferromagnetic coupling that correlated with decreases in MR contrast. To investigate whether Gd(III)–Gd(III) coupling or the formation of Gd oxide phases at high concentrations could be playing a role in the decrease in r 1 , the magnetic properties of GdPD‐NPs were investigated by variable‐temperature magnetic susceptibility measurements from 2 to 300 K under a 5000 Oe magnetic field (Figure S9, Supporting Information).…”

Section: Selected Relaxation Parameters Obtained From the Analysis Ofmentioning

confidence: 92%

“…In our previous study describing tunable Fe(III) loadings in PD‐NPs via the prepolymerization chelation strategy, we found that antiferromagnetic coupling between Fe(III) centers lowered their r 1 as we increased Fe(III) loadings in the particles . We hypothesized that Gd(III) would exhibit much less antiferromagnetic coupling because of the poor radial extension of the f‐orbitals.…”

Section: Selected Relaxation Parameters Obtained From the Analysis Ofmentioning

confidence: 96%

High Relaxivity Gadolinium‐Polydopamine Nanoparticles

Wang

Carniato

Xie

et al. 2017

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This study reports the preparation of a series of gadolinium-polydopamine nanoparticles (GdPD-NPs) with tunable metal loadings. GdPD-NPs are analyzed by nuclear magnetic relaxation dispersion and with a 7-tesla (T) magnetic resonance imaging (MRI) scanner. A relaxivity of 75 and 10.3 mM s at 1.4 and 7 T is observed, respectively. Furthermore, superconducting quantum interference device magnetometry is used to study intraparticle magnetic interactions and determine the GdPD-NPs consist of isolated metal ions even at maximum metal loadings. From these data, it is concluded that the observed high relaxivities arise from a high hydration state of the Gd(III) at the particle surface, fast rate of water exchange, and negligible antiferromagnetic coupling between Gd(III) centers throughout the particles. This study highlights design parameters and a robust synthetic approach that aid in the development of this scaffold for T -weighted, high relaxivity MRI contrast agents.

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“…Additionally, by coating iron oxide (Fe 3 O 4 ) surfaces with PDA, or the absorption of metal ions (i.e., Fe 3+ , Fe 2+ , Gd 3+ and Mn 2+ ) into PDA NPs, PDA can be used for magnetic resonance imaging. Li et al employed electron paramagnetic resonance, magnetometry, and nuclear magnetic relaxation dispersion to characterise PDA NPs loaded with iron [89]. The results indicated the presence of isolated iron centres with paramagnetic properties within the NPs, resulting in the measured magnetic resonance imaging signals [89].…”

Section: Biomedical Applications Of Pda Coatingsmentioning

confidence: 99%

“…Li et al employed electron paramagnetic resonance, magnetometry, and nuclear magnetic relaxation dispersion to characterise PDA NPs loaded with iron [89]. The results indicated the presence of isolated iron centres with paramagnetic properties within the NPs, resulting in the measured magnetic resonance imaging signals [89]. Similarly, magnetic NPs were coated with PDA as described by Mrowczynski et al [90].…”

Section: Biomedical Applications Of Pda Coatingsmentioning

confidence: 99%

From Bioinspired Glue to Medicine: Polydopamine as a Biomedical Material

et al. 2020

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Biological structures have emerged through millennia of evolution, and nature has fine-tuned the material properties in order to optimise the structure-function relationship. Following this paradigm, polydopamine (PDA), which was found to be crucial for the adhesion of mussels to wet surfaces, was hence initially introduced as a coating substance to increase the chemical reactivity and surface adhesion properties. Structurally, polydopamine is very similar to melanin, which is a pigment of human skin responsible for the protection of underlying skin layers by efficiently absorbing light with potentially harmful wavelengths. Recent findings have shown the subsequent release of the energy (in the form of heat) upon light excitation, presenting it as an ideal candidate for photothermal applications. Thus, polydopamine can both be used to (i) coat nanoparticle surfaces and to (ii) form capsules and ultra-small (nano)particles/nanocomposites while retaining bulk characteristics (i.e., biocompatibility, stability under UV irradiation, heat conversion, and activity during photoacoustic imaging). Due to the aforementioned properties, polydopamine-based materials have since been tested in adhesive and in energy-related as well as in a range of medical applications such as for tumour ablation, imaging, and drug delivery. In this review, we focus upon how different forms of the material can be synthesised and the use of polydopamine in biological and biomedical applications. platform is highlighted ( Figure 1A). Then, theoretical and experimental proof of the chemical formation of polydopamine-based structures is summarised ( Figure 1B,C). This is then followed by descriptions of the unique (physicochemical) properties of polydopamine. Their applications as adhesive and in energy-related applications are also highlighted ( Figure 1D). Throughout, their wide range of applications in the biomedical field (thanks to their biocompatibility) is thoroughly explained. This includes examples of theranostic and drug delivery applications derived from different types of polydopamine-based configurations: adhesive, particle coating agent, capsule, and NPs/composites, respectively ( Figure 1C,E). Lastly, some challenges to make PDA into functional tools for future clinical applications are envisaged. Materials 2019, 12, x FOR PEER REVIEW 2 of 22polydopamine-based structures is summarised ( Figure 1B,C). This is then followed by descriptions of the unique (physicochemical) properties of polydopamine. Their applications as adhesive and in energy-related applications are also highlighted ( Figure 1D). Throughout, their wide range of applications in the biomedical field (thanks to their biocompatibility) is thoroughly explained. This includes examples of theranostic and drug delivery applications derived from different types of polydopamine-based configurations: adhesive, particle coating agent, capsule, and NPs/composites, respectively ( Figure 1C,E). Lastly, some challenges to make PDA into functional tools for future clinical applicatio...

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Structure and Function of Iron-Loaded Synthetic Melanin

Cited by 134 publications

References 54 publications

Novel Intrapolymerization Doped Manganese‐Eumelanin Coordination Nanocomposites with Ultrahigh Relaxivity and Their Application in Tumor Theranostics

Novel Intrapolymerization Doped Manganese‐Eumelanin Coordination Nanocomposites with Ultrahigh Relaxivity and Their Application in Tumor Theranostics

High Relaxivity Gadolinium‐Polydopamine Nanoparticles

From Bioinspired Glue to Medicine: Polydopamine as a Biomedical Material

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