Electronic control of DNA-based nanoswitches and nanodevices

Ranallo, Simona; Amodio, Alessia; Idili, Andrea; Porchetta, Alessandro; Ricci, Francesco

doi:10.1039/c5sc03694a

Cited by 51 publications

(46 citation statements)

References 60 publications

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“…We employed square wave voltammetry (SWV; Supporting Information, Figure S4), which quantitatively suggested that about 20 mm of Cu 2+ was electrochemically released from the electrode. [22] The absence of NP precipitation and/or aggregation was proven by a combination of UV/Vis spectroscopy, DLS and TEM analyses, confirming that Au NP 1 is stable under the release conditions ( Supporting Information, Figures S6-S8). Kinetic measurements (Figure 2) of the initial rate of HPNPP transphosphorylation confirmed that the catalytic system achieved the same activity after the electrochemical release of Cu 2+ (v init = 7.4(AE 1.2) 10 À9 m s À1 ) as compared to manual addition (v init = 7.7(AE 1.2) 10 À9 m s À1 ).…”

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confidence: 61%

“…[21] Finally, Cu 2+ and Cd 2+ metal ions were chosen for their different standard reduction potentials (respectively À0.40 and + 0.34 V for Cd 2+ and Cu 2+ , relative to the standard hydrogen electrode). [22] We focused our initial investigations on the electrochemical generation of metal ions from a source in order to switch on catalytic activity. To that purpose, we used a carbon chip [23] previously coated with a film of Cu 0 .…”

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confidence: 99%

“…The deposition was carried out by dipping the electrode into an aqueous solution of Cu(NO 3 ) 2 and by applying a fixed reductive potential of À1.0 V vs. Ag/AgCl. [22] Cu 2+ ions were released from the electrode into a buffered solution containing Au NP 1 and HPNPP by applying a potential oxidative ramp from À0.3 to 0.5 V vs. Ag/AgCl for 60 seconds. We employed square wave voltammetry (SWV; Supporting Information, Figure S4), which quantitatively suggested that about 20 mm of Cu 2+ was electrochemically released from the electrode.…”

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confidence: 99%

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Reversible Electrochemical Modulation of a Catalytic Nanosystem

et al. 2016

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A catalytic system based on monolayer-functionalized gold nanoparticles (Au NPs) that can be electrochemically modulated and reversibly activated is reported. The catalytic activity relies on the presence of metal ions (Cd 2+ and Cu 2+ ), which can be complexed by the nanoparticle-bound monolayer. This activates the system towards the catalytic cleavage of 2-hydroxypropyl-p-nitrophenyl phosphate (HPNPP), which can be monitored by UV/Vis spectroscopy. It is shown that Cu 2+ metal ions can be delivered to the system by applying an oxidative potential to an electrode on which Cu 0 was deposited. By exploiting the different affinity of Cd 2+ and Cu 2+ ions for the monolayer, it was also possible to upregulate the catalytic activity after releasing Cu 2+ from an electrode into a solution containing Cd 2+ . Finally, it is shown that the activity of this supramolecular nanosystem can be reversibly switched on or off by oxidizing/reducing Cu/Cu 2+ ions under controlled conditions. Complexityisemergingasamajorthemeinchemistry. [1] Notonly does it mark a shift from the study of relatively simple molecules to complex molecular structures similar to those found in nature, but it also marks a shift from the study of single molecules to networks of molecules. [2][3][4] Within the subfield of catalysis, [5] the emergence of nanozymes, defined as nanomaterials with enzyme-like activity, nicely illustrates this development. [6] Nanozymes are prepared following a bottom-up strategy relying on the use of simple synthetic components for the formation of structures with a size and structural complexity similar to that of enzymes. [7,8] Their high stability, uniformity, and ease of modification is favoring applications in the fields of sensing, [9] materials science, [10] and systems chemistry. [11] The observation that nanozymes can exhibit an emerging property such as cooperativity is indeed a sign that significant progress has been made in the design of functional complex systems. [12] However, whereas nature has gained exquisite control over the complex biological machinery by using specific triggers to up-and down-regulate catalytic processes, similar regulatory pathways are still largely inexistent for nanozymes. Herein, we present a simple setup for the reversible activation and modulation of nanozymes using an electronic input. The electrochemical activation is highly attractive because of its ease of implementation, cleanliness, precision, and rapid response. [13][14][15][16] The availability of this kind of regulatory mechanism will strongly determine the success of chemists in constructing synthetic networks for studying complexity on the systems level.The main component of our system is Au NP 1, which are gold nanoparticles (d = 1.5 AE 0.3 nm) covered with C9-thiols terminating with a 1,4,7-triazacyclononane (TACN) head group (Figure 1 a). [11] Such nanoparticle-bound TACN moieties are able to coordinate Zn 2+ -metal ions forming a supra-

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Reversible Electrochemical Modulation of a Catalytic Nanosystem

et al. 2016

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“…It has already been demonstrated that DNA molecular machines can be controlled using electrical signals, using electrochemical control of pH and pH-sensitive structures such as imotifs or triplexes 14,15 or electronically triggered release of a signalling species from a surface 16 . In an alternative architecture, an enzymatic logic gate under certain conditions produces NADH, which activates an electrochemical process that leads to release of DNA from an alginate matrix 17 .…”

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confidence: 99%

Towards a bioelectronic computer: A theoretical study of a multi-layer biomolecular computing system that can process electronic inputs

Dunn

Trefzer

Johnson

et al. 2018

Preprint

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DNA molecular machines have great potential for use in computing systems. Since Adleman originally introduced the concept of DNA computing through his use of DNA strands to solve a Hamiltonian path problem, a range of DNA-based computing elements have been developed, including logic gates, neural networks, finite state machines (FSMs) and nondeterministic universal Turing machines. It has also been established that DNA molecular machines can be controlled using electrical signals and that the state of DNA nanodevices can be measured using an electrochemical readout. However, to the best of our knowledge there has as yet been no demonstration of a fully integrated biomolecular computing system that has multiple levels of information processing capacity, can accept electronic inputs and is capable of independent operation. In this paper we address the question of how such a system could work. We present simulation results showing that such an integrated hybrid system could convert electrical impulses into biomolecular signals, perform logical operations and take a decision, storing its history. We also illustrate theoretically how such a system could potentially be used to perform a task such as controlling an autonomous robot navigating through a maze.All rights reserved. No reuse allowed without permission.(which was not peer-reviewed) is the author/funder, who has granted bioRxiv a license to display the preprint in perpetuity.

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“…For example, sequences of DNA are rationally designed to recognize a specific target molecule and convert the recognition event into a useful function (i.e., signal production or release of a cargo) . Despite the great advantages represented by such nanodevices, their target‐induced actuation is usually achieved by exogenously adding them into a sample . To make a better control of activating DNA‐based nanodevices, we need to find a precisely controllable way out of common basic mechanism.…”

Section: Introductionmentioning

confidence: 99%

Electronic Activation of a DNA Nanodevice Using a Multilayer Nanofilm

Jeong

Ranallo

Rossetti

et al. 2016

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A method to control activation of a DNA nanodevice by supplying a complementary\ud DNA (cDNA) strand from an electro-responsive nanoplatform is reported. To develop\ud functional nanoplatform, hexalayer nanofilm is precisely designed by layer-by-layer\ud assembly technique based on electrostatic interaction with four kinds of materials:\ud Hydrolyzed poly(β-amino ester) can help cDNA release from the film. A cDNA is\ud used as a key building block to activate DNA nanodevice. Reduced graphene oxides\ud (rGOs) and the conductive polymer provide conductivity. In particular, rGOs efficiently\ud incorporate a cDNA in the film via several interactions and act as a barrier. Depending\ud on the types of applied electronic stimuli (reductive and oxidative potentials), a\ud cDNA released from the electrode can quantitatively control the activation of DNA\ud nanodevice. From this report, a new system is successfully demonstrated to precisely\ud control DNA release on demand. By applying more advanced form of DNA-based\ud nanodevices into multilayer system, the electro-responsive nanoplatform will expand\ud the availability of DNA nanotechnology allowing its improved application in areas\ud such as diagnosis, biosensing, bioimaging, and drug delivery

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Electronic control of DNA-based nanoswitches and nanodevices

Abstract: Here we demonstrate that we can rationally and finely control the functionality of different DNA-based nanodevices and nanoswitches using electronic inputs.

Cited by 51 publications

References 60 publications

Reversible Electrochemical Modulation of a Catalytic Nanosystem

Reversible Electrochemical Modulation of a Catalytic Nanosystem

Towards a bioelectronic computer: A theoretical study of a multi-layer biomolecular computing system that can process electronic inputs

Electronic Activation of a DNA Nanodevice Using a Multilayer Nanofilm

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