Improved chemical and mechanical stability of peptoid nanosheets by photo-crosslinking the hydrophobic core

Flood, Dillon T.; Proulx, Caroline; Robertson, Ellen J.; Battigelli, Alessia; Wang, Shuo; Schwartzberg, Adam M.; Zuckermann, Ronald N.

doi:10.1039/c6cc00588h

Cited by 19 publications

(28 citation statements)

References 31 publications

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“…To handle these shortcomings, researchers have proposed nano-particles as novel drug carriers to help patients cope with cancer [6,7,8]. Nanoparticles, like vesicles [9,10,11], nanotubes [6,7,8], micelles [12,13,14], nanofibers [15,16,17], and nanosheet [18,19] are typically commonly formed by amphiphilic copolymers via self-assembly. Nanoparticles can encapsulate drugs via physical entrapment or solubilization to achieve various advantages, including controlled drug release, decreased cytotoxicity, increased aqueous solubility, and targeted action site [4,20,21,22,23].…”

Section: Introductionmentioning

confidence: 99%

Polycaprolactone-Based Mimetic Antimicrobial Peptide Copolymers Vesicles as an Effective Drug-Carrier for Cancer Therapy

Qian

Zhou

et al. 2019

Polymers

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A novel series of amphiphilic mimicking antimicrobial peptide copolymers PCL16-b-Kn can assemble in water to form uniform vesicles. Transmission electron microscopy was used to observe the vesicular structure of the nanoparticles, and dynamic light scattering revealed their uniform size and narrow dispersion. Critical vesiculation concentrations were also tested, revealing that these vesicles can exist at low concentrations. Furthermore, in vitro and intracellular drug release of doxorubicin(DOX)-vesicles were conducted. These vesicles could encapsulate DOX and achieve efficient intracellular drug release. Overall, these copolymer vesicles exhibit potential application value as multifunctional drug-carrier systems with antibacterial capability in cancer therapy.

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Section: Introductionmentioning

confidence: 99%

Polycaprolactone-Based Mimetic Antimicrobial Peptide Copolymers Vesicles as an Effective Drug-Carrier for Cancer Therapy

Qian

Zhou

et al. 2019

Polymers

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“…The weak charge-based association that drives both the nanostructure assembly and the formation of nanostructure-enzyme complexes explains the temperature-instability of these complexes. Employing novel composites to capture nanostructures into higher order polymers [ 52 ] or the use of crosslinking [ 54 ] are potential strategies that could lead to further stabilization of the nanostructure-enzyme complexes. Protection from proteolysis could be attributable to a higher surface packing density and better sequestration of smaller enzymes associated with nanotubes.…”

Section: Discussionmentioning

confidence: 99%

Synthetic CO2-fixation enzyme cascades immobilized on self-assembled nanostructures that enhance CO2/O2 selectivity of RubisCO

Satagopan

Sun

Parquette

et al. 2017

Biotechnol Biofuels

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BackgroundWith increasing concerns over global warming and depletion of fossil-fuel reserves, it is attractive to develop innovative strategies to assimilate CO2, a greenhouse gas, into usable organic carbon. Cell-free systems can be designed to operate as catalytic platforms with enzymes that offer exceptional selectivity and efficiency, without the need to support ancillary reactions of metabolic pathways operating in intact cells. Such systems are yet to be exploited for applications involving CO2 utilization and subsequent conversion to valuable products, including biofuels. The Calvin–Benson–Bassham (CBB) cycle and the enzyme ribulose 1,5-bisphosphate carboxylase/oxygenase (RubisCO) play a pivotal role in global CO2 fixation.ResultsWe hereby demonstrate the co-assembly of two RubisCO-associated multienzyme cascades with self-assembled synthetic amphiphilic peptide nanostructures. The immobilized enzyme cascades sequentially convert either ribose-5-phosphate (R-5-P) or glucose, a simpler substrate, to ribulose 1,5-bisphosphate (RuBP), the acceptor for incoming CO2 in the carboxylation reaction catalyzed by RubisCO. Protection from proteolytic degradation was observed in nanostructures associated with the small dimeric form of RubisCO and ancillary enzymes. Furthermore, nanostructures associated with a larger variant of RubisCO resulted in a significant enhancement of the enzyme’s selectivity towards CO2, without adversely affecting the catalytic activity.ConclusionsThe ability to assemble a cascade of enzymes for CO2 capture using self-assembling nanostructure scaffolds with functional enhancements show promise for potentially engineering entire pathways (with RubisCO or other CO2-fixing enzymes) to redirect carbon from industrial effluents into useful bioproducts.Electronic supplementary materialThe online version of this article (doi:10.1186/s13068-017-0861-6) contains supplementary material, which is available to authorized users.

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“…[33,71] Photoreactive monomers were successfully introduced to the nanosheet sequence such that the sheets could be photo-crosslinked in their hydrophobic interior after their assembly to improve their chemical and mechanical stability. [72] Recent advances in characterization tools such as X-ray scattering, cryo-TEM, and computational modeling greatly deepen the understanding of the assembled structures of peptoids at the atomic scale [51,58,62,63,69], and thus facilitate their atomic-engineering. X-ray scattering is a common technique widely used in polymer field.…”

Section: Engineering the Atomic Structure Of Nanosheet Interiormentioning

confidence: 99%

Engineering the atomic structure of sequence-defined peptoid polymers and their assemblies

Xuan

Zuckermann

2020

Polymer

Self Cite

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Peptoids are a family of sequence-defined, non-natural biomimetic polymers which show excellent properties including good chemical and enzymatic stability and high structural tunability. The solid-phase submonomer synthesis method allows precise control over the identity and sequence of chemically diverse side chains, enabling the atomic engineering of their chemical structures for a variety of applications. This unprecedented level of structural control enables access to atomically defined threedimensional chain conformations and assemblies, facilitating the design and optimization of a variety of nanoscale architectures that can function in biology and materials science. In order to approach the rational design of peptoid materials in a more predictive and precise manner, it is crucial to fully understand how chemical information, in the form of the monomer sequence, encodes their folding and assembly into structurally defined, functional 3D shapes. This perspective focuses on recent studies into the atomic engineering of peptoid nanostructures by examining the impact of sequence variations on their secondary and three-dimensional structures, as well as their functional properties.

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Improved chemical and mechanical stability of peptoid nanosheets by photo-crosslinking the hydrophobic core

Abstract: Photo-crosslinking produced more robust nanosheets that can survive sonication, lyophilization, and other biochemical manipulations.

Cited by 19 publications

References 31 publications

Polycaprolactone-Based Mimetic Antimicrobial Peptide Copolymers Vesicles as an Effective Drug-Carrier for Cancer Therapy

Polycaprolactone-Based Mimetic Antimicrobial Peptide Copolymers Vesicles as an Effective Drug-Carrier for Cancer Therapy

Synthetic CO2-fixation enzyme cascades immobilized on self-assembled nanostructures that enhance CO2/O2 selectivity of RubisCO

Engineering the atomic structure of sequence-defined peptoid polymers and their assemblies

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