ATP-Driven Temporal Control over Structure Switching of Polymeric Micelles

Dong, Bingyang; Liu, Li; Hu, Cong

doi:10.1021/acs.biomac.8b00769

Cited by 15 publications

(15 citation statements)

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“…The difficulty in implementing such a concept in synthetic system is related to the need for highest levels of programmability and ability for deterministic autonomous reconfiguration leading to multiple transient dynamic steady-state (DySS) structures, which is a profound challenge in supramolecular chemistry. [24][25][26] On the contrary, DNA shows great potential to program reaction networks and pathways for self-assemblies in a systems chemistry approach. [27][28][29] Herein, we demonstrate pathway complexity in ATP-fueled transient DNA polymerizations from a species pool realizing autonomous and transient multiple DySS structures (Figure 1a,b).…”

Section: Introductionmentioning

confidence: 99%

Pathway Complexity in Fuel-Driven DNA Nanostructures with Autonomous Reconfiguration of Multiple Dynamic Steady States

Deng

Walther

2020

J. Am. Chem. Soc.

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We introduce pathway complexity on a multicomponent systems level in chemically fueled transient DNA polymerization systems, achieving autonomous evolution over multiple structural dynamic steady states from monomers to dimers, oligomers of dimers to randomized polymer structures before being ultimately degraded back to monomers once the fuel is consumed. The enabling key principle is to design monomer species having kinetically selected molecular recognition in the structure-forming step and which are reconfigured in an enzymatic reaction network. This non-equilibrium systems chemistry approach to pathway complexity provides new conceptual insights in fuel-driven automatons and autonomous materials design.Nature relies on non-equilibrium structures and processes to perform work by dissipating energy stored in ATP or GTP. 1-4 Pathway complexity plays a pivotal role to associate those dynamic structures and thus realize a living system. For instance, intracellular signaling networks involve multiple steps of ATP/GTP-powered phosphorylation and enzyme activation for downstream regulations. 5-8 Thus far, synthetic systems with fuel-driven transient properties are developed in the fields of systems chemistry, materials science and synthetic biology. 4,[9][10][11][12] Synthetic systems requiring continuous energy influx have extended the features and functions of present-day functional materials. [13][14] Most presently existing fuel-driven systems show single trajectories of their non-equilibrium states, such as helical structure switching, 15 supramolecular polymerization, 14, 16 nanoreactors, 13, 17 transient hydrogels, [18][19] and photonic materials. 20 On the contrary, in classical supramolecular chemistry, pathway complexity is regularly exploited to transiently pass energetically downhill from metastable structures to equilibrium. 21-22 A relevant example showing multiple states in an autonomous fashion is the case of supramolecular helicity switching coupled to hydrolysis of environmental ATP to ADP, AMP, and to adenosine. 15 In directly chemically driven systems, Boekhoven and coworkers recently showed that small fuel amounts allowed the formation of reversibly assembling transient clusters, while large fuel amounts lead to a trapping of aggregates in a non-transient fashion. 23 Critically, pathway-controlled uphill fuel-driven systems involving multiple building blocks with an autonomous structural reconfiguration of multiple dynamic transient states have not been shown by any previous report. Such a concept would however be very valuable to promote a further integration of systems chemistry concepts with reaction networks and dissipative and transient structure formation.The difficulty in implementing such a concept in synthetic system is related to the need for highest levels of programmability and ability for deterministic autonomous reconfiguration leading to multiple transient dynamic steady-state (DySS) structures, which is a profound challenge in supramolecular chemistry. 24-26 On the contrary, DNA ...

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Section: Introductionmentioning

confidence: 99%

Pathway Complexity in Fuel-Driven DNA Nanostructures with Autonomous Reconfiguration of Multiple Dynamic Steady States

Deng

Walther

2020

J. Am. Chem. Soc.

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“…Besides this specific ligand receptor, also the 4,6‐diamino‐1, 3,5‐triazine (DAT) motif has been reported to be able to bind with ATP via hydrogen bonding. [ 198 ] Liu and co‐workers tethered such DAT motifs to a block copolymer. Those block copolymers formed large polymeric aggregates at pH 7.4 due to the relative hydrophobicity and hydrogen bonding of the DAT motif (Figure 20c).…”

Section: Atp‐fueled Self‐assembling Systems With Autonomous Operationmentioning

confidence: 99%

“…By fueling a system consisting of PDAT micelles and alkaline phosphatase, temporal division of the polymeric micelles was obtained, and multiple reciprocating division–fusion motions were achieved by repeated ATP fueling (Figure 20c,e). [ 198 ] It is worthy to note that the conclusion of droplets disruption rather than contraction by ATP might be derived from the changes of both droplet size and number after adding ATP.…”

Section: Atp‐fueled Self‐assembling Systems With Autonomous Operationmentioning

confidence: 99%

ATP‐Responsive and ATP‐Fueled Self‐Assembling Systems and Materials

2020

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his/her body weight in ATP each day, which is enabled through a very efficient ADP/ATP recycling system. [7] Aside of the fascinating non-equilibrium succeeded by exploiting ATP/GTP as chemical fuels to drive structures and functions, it is also important to realize that ATP and other nucleoside phosphates can be used as biological and chemical signals. [8-10] Lots of biological processes such as chromatin remodeler activation, [11] inflammatory signaling, [12] and cell differentiation [13] are mediated by ATP signaling. Additionally, cancer cells have a higher concentration of ATP, [14] which in turn provides a handle to develop new types of molecular therapies. This of course requires to develop sophisticated carriers or self-assembling structures that highly specifically react to ATP and potentially even to its concentration, ideally without any interference from other nucleoside phosphates. [15-20] For such cases, it is also important to realize that ATP is used as a chemical signal rather than a chemical fuel, as the primary objective may not be to harvest its energy from hydrolysis for functions, but just to use its chemical structure for a change of function. Overall, it becomes clear that the use of ATP (and similarly GTP) as a trigger or as a chemical fuel is of high relevance to interact with living systems and also to be able to create active devices in long term that can create work and allow for active communication in a biological environment using the fuels available therein. [21] In the scope of this review on ATP-dependent systems, and being set at the interface of near-equilibrium responsive materials versus non-equilibrium active materials, it is useful to begin Adenosine triphosphate (ATP) is a central metabolite that plays an indispensable role in various cellular processes, from energy supply to cell-tocell signaling. Nature has developed sophisticated strategies to use the energy stored in ATP for many metabolic and non-equilibrium processes, and to sense and bind ATP for biological signaling. The variations in the ATP concentrations from one organelle to another, from extracellular to intracellular environments, and from normal cells to cancer cells are one motivation for designing ATPtriggered and ATP-fueled systems and materials, because they show great potential for applications in biological systems by using ATP as a trigger or chemical fuel. Over the last decade, ATP has been emerging as an attractive co-assembling component for man-made stimuli-responsive as well as for fuel-driven active systems and materials. Herein, current advances and emerging concepts for ATP-triggered and ATP-fueled self-assemblies and materials are discussed, shedding light on applications and highlighting future developments. By bringing together concepts of different domains, that is from supramolecular chemistry to DNA nanoscience, from equilibrium to nonequilibrium self-assembly, and from fundamental sciences to applications, the aim is to cross-fertilize current approaches with the ultimate aim to bring ...

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“…Recent attempts to achieve temporal regulation are, in general, concerned with transient assembly or conformational changes of supramolecular polymers and of colloidal systems. [7][8][9][10][11][12][13][14][15][16][17][18] Most of these systems are examples of fundamental design strategies to build a transient change in self-assembled structures. However, temporally programmed functions similar to natural systems are very few.…”

Section: Introductionmentioning

confidence: 99%