Network-based redox communication between abiotic interactive materials

Li, Jinyang; Zhao, Zhiling; Kim, Eunkyoung; Rzasa, John R.; Zong, Guanghui; Wang, Lai-Xi; Bentley, William E.; Payne, G. L.

doi:10.1016/j.isci.2022.104548

Cited by 5 publications

(6 citation statements)

References 54 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…To facilitate interpretation, it is common to display time series data as phase plane plots of output versus input potential. [11,12] The first phase plane plot of Figure 3c shows the electrical current and optical absorbance output responses as a function of imposed potential. When the potential was swept into the oxidative region (approximately +0.3 V versus Ag/ AgCl), the optical absorbance was observed to increase which is consistent with the switching of the catechol to the oxidized quinone.…”

Section: Molecular Switching Of Conducting Catecholmentioning

confidence: 99%

“…The creation of improved electronic materials relies on understanding the mechanisms responsible for charge-storage storage, [25][26][27][28][29][30][31][32][33] optoelectronics, [34][35][36] organic electronics, [7,37,38] and bioelectronics. [12,[39][40][41] Interestingly, the characterization of redox polymers often focuses on their conducting properties although some recent studies found that the addition of diffusible redox mediators can enhance their functional capacities (e.g., for charge storage and molecular memory). [42][43][44] While various composite materials systems have been prepared from carbon-based nanomaterials, redox polymers, and in some cases, redox mediators, [45][46][47][48] the electron-transfer mechanisms within these composites are not fully resolved.…”

Section: Introductionmentioning

confidence: 99%

“…[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.…”

mentioning

confidence: 99%

See 2 more Smart Citations

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Kim

Argenziano

Zhao

et al. 2022

Adv Materials Inter

Self Cite

View full text Add to dashboard Cite

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.

show abstract

Section: Molecular Switching Of Conducting Catecholmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

mentioning

confidence: 99%

See 1 more Smart Citation

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Kim

Argenziano

Zhao

et al. 2022

Adv Materials Inter

Self Cite

View full text Add to dashboard Cite

show abstract

“…Incubation of these cultures with a previously oxidized film (“Cat Ox film”) resulted in a delayed response: presumably, the culture provided the reducing equivalents to convert the oxidized film to its reduced state, thus allowing the film to generate H 2 O 2 in the presence of O 2 . More broadly, we believe MEP could become a new tool for redox biology − both to understand the redox activities of native materials (e.g., melanins) and for the design of redox-based interactive materials. , …”

Section: Integrating Electrochemistry Into Materials Science and Biologymentioning

confidence: 99%

“…More broadly, we believe MEP could become a new tool for redox biology 149−151 both to understand the redox activities of native materials (e.g., melanins) and for the design of redox-based interactive materials. 151,152 Fourth, an electrofabricated composite catechol−graphene− chitosan (Cat−Gr−Chit) film was shown to offer synergistic conducting and redox properties. 153 Figure 14a shows the twostep electrofabrication of this composite: a graphene−chitosan film was first assembled by cathodic co-deposition from a solution of chitosan with dispersed graphene, and then, catechol was anodically grafted to the graphene−chitosan film.…”

Section: Electroassembly Of Collagen "Molten Fibrils"mentioning

confidence: 99%

Electro-Biofabrication. Coupling Electrochemical and Biomolecular Methods to Create Functional Bio-Based Hydrogels

et al. 2023

Self Cite

View full text Add to dashboard Cite

Twenty years ago, this journal published a review entitled "Biofabrication with Chitosan" based on the observations that (i) chitosan could be electrodeposited using low voltage electrical inputs (typically less than 5 V) and (ii) the enzyme tyrosinase could be used to graft proteins (via accessible tyrosine residues) to chitosan. Here, we provide a progress report on the coupling of electronic inputs with advanced biological methods for the fabrication of biopolymer-based hydrogel films. In many cases, the initial observations of chitosan's electrodeposition have been extended and generalized: mechanisms have been established for the electrodeposition of various other biological polymers (proteins and polysaccharides), and electrodeposition has been shown to allow the precise control of the hydrogel's emergent microstructure. In addition, the use of biotechnological methods to confer function has been extended from tyrosinase conjugation to the use of protein engineering to create genetically fused assembly tags (short sequences of accessible amino acid residues) that facilitate the attachment of function-conferring proteins to electrodeposited films using alternative enzymes (e.g., transglutaminase), metal chelation, and electrochemically induced oxidative mechanisms. Over these 20 years, the contributions from numerous groups have also identified exciting opportunities. First, electrochemistry provides unique capabilities to impose chemical and electrical cues that can induce assembly while controlling the emergent microstructure. Second, it is clear that the detailed mechanisms of biopolymer self-assembly (i.e., chitosan gel formation) are far more complex than anticipated, and this provides a rich opportunity both for fundamental inquiry and for the creation of high performance and sustainable material systems. Third, the mild conditions used for electrodeposition allow cells to be co-deposited for the fabrication of living materials. Finally, the applications have been expanded from biosensing and lab-on-a-chip systems to bioelectronic and medical materials. We suggest that electro-biofabrication is poised to emerge as an enabling additive manufacturing method especially suited for life science applications and to bridge communication between our biological and technological worlds.

show abstract

Constraint Coupling of Redox Cascade and Electron Transfer Synchronization on Electrode‐Nanosensor Interface for Repeatable Detection of Tumor Biomarkers

Xie,

Jin,

Wang

et al. 2023

Small Methods

View full text Add to dashboard Cite

Quantitative analysis of up‐regulated biomarkers in pathological tissues is helpful to tumor surgery yet the loss of biomarker extraction and time‐consuming operation limited the accurate and quick judgement in preoperative or intraoperative diagnosis. Herein, an immobilization‐free electrochemical sensing platform is developed by constraint coupling of electron transfer cascade on electrode‐nanosensor interface. Specifically, electrochemical indicator (Ri)‐labeled single‐stranded DNA on electroactive nanodonor (polydopamine, PDA) can be responsively detached by formation of DNA complex through the recognition and binding with targets. By applying the oxidation potential of Ri, nanosensor collisions on electrode surface trigger a cascade redox cycling of PDA and Ri through synchronous electron transfer, which boost the amplification of current signal output. The developed nanosensor exhibit excellent linear response toward up‐regulated biomarkers (miRNA‐21, ATP, and VEGF) with low detection limits (32 fM, 386 pM, and 2.8 pM). Moreover, background influence from physiological interferent is greatly reduced by restricted electron transfer coupling on electrode. The practical applicability is illustrated in sensitive and highly repeatable profiling of miRNA‐21 in lysate of tumor cells and tumor tissue, beneficial for more reliable diagnosis. This electrochemical platform by employing electron transfer cascades at heterogeneous interfaces offers a route to anti‐interference detection of biomarkers in tumor tissues.

show abstract

Network-based redox communication between abiotic interactive materials

Cited by 5 publications

References 54 publications

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Electro-Biofabrication. Coupling Electrochemical and Biomolecular Methods to Create Functional Bio-Based Hydrogels

Constraint Coupling of Redox Cascade and Electron Transfer Synchronization on Electrode‐Nanosensor Interface for Repeatable Detection of Tumor Biomarkers

Contact Info

Product

Resources

About