Radical-Enriched Artificial Melanin

Cao, Wei; Mantanona, Alex J.; Mao, Haochuan; McCallum, Naneki C.; Jiao, Yang; Battistella, Claudia; Caponetti, Valeria; Zang, Nanzhi; Thompson, Matthew P.; Montalti, Marco; Wasielewski, Michael R.; Rinehart, Jeffrey D.; Gianneschi, Nathan C.

doi:10.1021/acs.chemmater.0c01573

Cited by 19 publications

(33 citation statements)

References 55 publications

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“…Nevertheless, as recently demonstrated by the same authors, material selectivity becomes preferable for the differential coating of a multi-material structure [93]. [35], with permission from American Chemical Society, 2020.…”

Section: Functionalization and Coating: Use As A Bio-template Or As Amentioning

confidence: 86%

“…(2) Antioxidant and free radical scavenging activity. Melanin as well as artificial MNP, possessing various reductive functional groups as catechol, amine, and imine, exhibit a broad action of Radical-enriched artificial MNP have been even reported to be so efficient to work even as ionizing radiation-protector able to scavenge reactive oxygen species produced upon X-ray exposure [35]. 3Metal-Chelation properties.…”

Section: Introductionmentioning

confidence: 99%

“…Due to the presence of stable π-electron free radical species, paramagnetism is a characteristic feature naturally occurring in melanin, giving persistent electron spin resonance (ESR or EPR). Similarly, PDA exhibits a single-line ESR spectrum [35,43]. Thanks to this combination of features MNP are not simply carriers for the delivery of therapeutic or imaging agents but are themselves suitable to generate diagnostic signals, as in the case of PAI or FI or to perform dark or light stimulated therapeutic action as in the case of antioxidant (AOX) therapy and PTT respectively.…”

Section: Introductionmentioning

confidence: 99%

“…Melanin as well as artificial MNP, possessing various reductive functional groups as catechol, amine, and imine, exhibit a broad action of defense against multiple reactive oxygen and nitrogen species (RONS), including O 2 •− , H 2 O 2 , • OH, • NO, and ONOO − , that are generated, e.g., after solar exposure, as well as in diseases [ 34 ]. Radical-enriched artificial MNP have been even reported to be so efficient to work even as ionizing radiation-protector able to scavenge reactive oxygen species produced upon X-ray exposure [ 35 ]. Metal-Chelation properties.…”

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Bio-Applications of Multifunctional Melanin Nanoparticles: From Nanomedicine to Nanocosmetics

et al. 2020

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Bioinspired nanomaterials are ideal components for nanomedicine, by virtue of their expected biocompatibility or even complete lack of toxicity. Natural and artificial melanin-based nanoparticles (MNP), including polydopamine nanoparticles (PDA NP), excel for their extraordinary combination of additional optical, electronic, chemical, photophysical, and photochemical properties. Thanks to these features, melanin plays an important multifunctional role in the design of new platforms for nanomedicine where this material works not only as a mechanical support or scaffold, but as an active component for imaging, even multimodal, and simple or synergistic therapy. The number of examples of bio-applications of MNP increased dramatically in the last decade. Here, we review the most recent ones, focusing on the multiplicity of functions that melanin performs in theranostics platforms with increasing complexity. For the sake of clarity, we start analyzing briefly the main properties of melanin and its derivative as well as main natural sources and synthetic methods, moving to imaging application from mono-modal (fluorescence, photoacoustic, and magnetic resonance) to multi-modal, and then to mono-therapy (drug delivery, anti-oxidant, photothermal, and photodynamic), and finally to theranostics and synergistic therapies, including gene- and immuno- in combination to photothermal and photodynamic. Nanomedicine aims not only at the treatment of diseases, but also to their prevention, and melanin in nature performs a protective action, in the form of nanopigment, against UV-Vis radiations and oxidants. With these functions being at the border between nanomedicine and cosmetics nanotechnology, recently examples of applications of artificial MNP in cosmetics are increasing, paving the road to the birth of the new science of nanocosmetics. In the last part of this review, we summarize and discuss these important recent results that establish evidence of the interconnection between nanomedicine and cosmetics nanotechnology.

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Section: Functionalization and Coating: Use As A Bio-template Or As Amentioning

confidence: 86%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Bio-Applications of Multifunctional Melanin Nanoparticles: From Nanomedicine to Nanocosmetics

et al. 2020

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Interactive Materials for Bidirectional Redox‐Based Communication

Wang

Zong

et al. 2021

Advanced Materials

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Emerging research indicates that biology routinely uses diffusible redox‐active molecules to mediate communication that can span biological systems (e.g., nervous and immune) and even kingdoms (e.g., a microbiome and its plant/animal host). This redox modality also provides new opportunities to create interactive materials that can communicate with living systems. Here, it is reported that the fabrication of a redox‐active hydrogel film can autonomously synthesize a H2O2 signaling molecule for communication with a bacterial population. Specifically, a catechol‐conjugated/crosslinked 4‐armed thiolated poly(ethylene glycol) hydrogel film is electrochemically fabricated in which the added catechol moieties confer redox activity: the film can accept electrons from biological reductants (e.g., ascorbate) and donate electrons to O2 to generate H2O2. Electron‐transfer from an Escherichia coli culture poises this film to generate the H2O2 signaling molecule that can induce bacterial gene expression from a redox‐responsive operon. Overall, this work demonstrates that catecholic materials can participate in redox‐based interactions that elicit specific biological responses, and also suggests the possibility that natural phenolics may be a ubiquitous biological example of interactive materials.

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Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Kim

Argenziano

Zhao

et al. 2022

Adv Materials Inter

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and electron-transfer, and then controlling these mechanisms for user-defined purposes. For energy applications (e.g., capacitors and batteries), the focus is on storing large quantities of electrons and controlling their discharge. [1][2][3] For information processing applications (e.g., electronics), [4,5] materials are desired that can gate and rectify electron-flow. [6,7] Other applications focus on materials that offer state-dependent properties (e.g., optoelectronics) [8] or memory (e.g., memristors). [9] With the growing emphasis on safety and sustainability, and the expanding interest in life-science applications, there is an increasing interest in the development of electronic materials that function in aqueous systems. [10] In aqueous systems, electron-transfer is constrained by the solvent and typically occurs through at least two distinctly different mechanisms each of which favors different types of materials. [11][12][13] One electron-transfer mechanism is a metal-like conductivity. [14,15] Carbon-based nanomaterials have been especially important for conferring such conductivity [14,16] with benefits that include enhanced double layer charge storage for energy applications [17][18][19][20][21] and electrocatalytic properties for sensing applications. [22][23][24] A second electron-transfer mechanism involves reduction-oxidation (redox) reactions. Redox polymers offer such properties and have been used in applications that include energy Electronic materials that allow the controlled flow of electrons in aqueous media are required for emerging applications that require biocompatibility, safety, and/or sustainability. Here, a composite hydrogel film composed of graphene and catechol is electrofabricated, and that this composite offers synergistic properties is reported. Graphene confers metal-like conductivity and enables charge-storage through an electrical double layer mechanism. Catechol confers redox-activity and enables charge-storage through a redox mechanism. Importantly, there are two functional populations of catechols: conducting-catechols (presumably in intimate contact with graphene) allow direct electron-transfer; and non-conducting-catechols (presumably physically separated from graphene) require diffusible mediators to enable electrontransfer. Using a variety of spectroelectrochemical measurements, that the capacity of the composite for charge-storage increases in proportion to the extent by which the catechol-groups can undergo redox-state switching is demonstrated. To illustrate the broad relevance of this work, how the redoxstate switching can be related to both the charge storage of energy materials and the memory of molecular electronic materials is discussed. The authors believe this work is significant because it demonstrates that: conducting and redox-active components enable distinctly different mechanisms for chargestorage and electron-transfer; these components act synergistically; and mediators provide unique opportunities to extend the capabilities of electronic materials.

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Radical-Enriched Artificial Melanin

Cited by 19 publications

References 55 publications

Bio-Applications of Multifunctional Melanin Nanoparticles: From Nanomedicine to Nanocosmetics

Bio-Applications of Multifunctional Melanin Nanoparticles: From Nanomedicine to Nanocosmetics

Interactive Materials for Bidirectional Redox‐Based Communication

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

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