Porphyrin-Cored Polymer Nanoparticles: Macromolecular Models for Heme Iron Coordination

Rodriguez, Kyle J.; Hanlon, Ashley M.; Lyon, Christopher K.; Cole, Justin P.; Tuten, Bryan T.; Tooley, Christian; Berda, Erik B.; Pazicni, Samuel

doi:10.1021/acs.inorgchem.6b01113

Cited by 25 publications

(17 citation statements)

References 43 publications

(50 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Metal‐center reduction using sodium ascorbate induced superstructure rearrangement to one‐order backward. Nanoclusters in metal‐SCNP and subdomains in nanoparticle are potentially important in the enzyme‐mimic catalysis fields via controlling interior size/composition on demand by means of pH/reduction mediation.…”

Section: Discussionmentioning

confidence: 99%

“…By metal–ligand complexation, Barner‐Kowollik achieved selective‐point folding and repeating‐unit folding, Lemcoff synthesized SCNP catalysts, Pomposo and Meijer fulfilled catalytic selectivity, and Zimmerman realized catalytic click reaction in water and cells. Berda reported protein‐mimicking SCNPs . All these suggest the robustness in preparation of metal‐SCNPs.…”

Section: Introductionmentioning

confidence: 91%

See 1 more Smart Citation

Metal‐Folded Single‐Chain Nanoparticle: Nanoclusters and Self‐Assembled Reduction‐Responsive Sub‐5‐nm Discrete Subdomains

Cui

Gao

Ding

et al. 2017

Macromol. Rapid Commun.

View full text Add to dashboard Cite

Easy access to discrete nanoclusters in metal-folded single-chain nanoparticles (metal-SCNPs) and independent ultrafine sudomains in the assemblies via coordination-driven self-assembly of hydrophilic copolymer containing 9% imidazole groups is reported herein. H NMR, dynamic light scattering, and NMR diffusion-ordered spectroscopy results demonstrate self-assembly into metal-SCNPs (>70% imidazole-units folded) by neutralization in the presence of Cu(II) in water to pH 4.6. Further neutralization induces self-assembly of metal-SCNPs (pH 4.6-5.0) and shrinkage (pH 5.0-5.6), with concurrent restraining residual imidazole motifs and hydrophilic segment, which organized into constant nanoparticles over pH 5.6-7.5. Atomic force microscopy results evidence discrete 1.2 nm nanoclusters and sub-5-nm subdomains in metal-SCNP and assembled nanoparticle. Reduction of metal center using sodium ascorbate induces structural rearrangement to one order lower than the precursor. Enzyme mimic catalysis required media-tunable discrete ultrafine interiors in metal-SCNPs and assemblies have hence been achieved.

show abstract

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 91%

Metal‐Folded Single‐Chain Nanoparticle: Nanoclusters and Self‐Assembled Reduction‐Responsive Sub‐5‐nm Discrete Subdomains

Cui

Gao

Ding

et al. 2017

Macromol. Rapid Commun.

View full text Add to dashboard Cite

show abstract

“…Initial steps have been undertaken in this endeavor such as the work of the Berda team, who synthesized porphyrin‐cored nanoparticles (PCPNs) as heme iron protein models (Figure ). By carefully designing a four‐armed polymer with a heme moiety embedded within a hydrophobic core, these authors were able to demonstrate that the PCPNs could be used as synthetic analogues towards native systems with both redox chemistry as well as ligand‐binding reactivity . Further developments from the Berda laboratory include the use of both Passerini and Ugi chemistries to generate dipeptide based crosslinks.…”

Section: Architecture Beyond Intramolecular Crosslinksmentioning

confidence: 99%

“…By carefully designing a four-armed polymer with a heme moiety embedded within a hydrophobic core, these authors were able to demonstrate that the PCPNs could be used as synthetic analogues towards native systems with both redox chemistry as well as ligand-binding reactivity. [55] Further developments from the Berda laboratory include the use of both Passerini and Ugi chemistries to generate dipeptide based crosslinks. Further, these authors were able to incorporate a small level of secondary structure by creating an internal domain by introducing internal α-hydrazino turns based on the sequential folding of hydrazone motifs.…”

Section: Incorporating Defined Domains Into Scnpsmentioning

confidence: 99%

Macromolecular Superstructures: A Future Beyond Single Chain Nanoparticles

Frisch

Tuten

Barner‐Kowollik

2020

Israel Journal of Chemistry

Self Cite

View full text Add to dashboard Cite

Over the last 100 years polymer chemistry has flourished in all areas and enabled control over synthetic polymer architectures – including chain lengths, dispersity and monomer sequences. Compared to the architectures of biomacromolecules, these scientific achievements mainly took place on the level of primary structures. The plethora of functions carried out by proteins in nature, however, does not only result from their primary structure, but from its folding into perfectly defined 3D structures. Striving towards a similar architectural control and function in synthetic polymers, the field of single chain nanoparticles (SCNPs) emerged. In this review, we analyze the state of the art and identify what is currently standing between polymer chemistry and perfectly controlled synthetic macromolecular architectures. Based on the current challenges in the field of SCNPs, we discuss potential avenues to break today's barriers and explore future applications reaching beyond the current‐state‐of‐the‐art.

show abstract

“…Rodriguez et al recently synthesized a porphyrin‐cored polymer nanoparticle that was designed using a tetrafunctionalized porphyrin macroinitiator and MMA and 9‐anthracenylmethyl methacrylate as co‐monomers . The resultant nanoparticle was probed as a heme model mimic by exposing the system to reductants and exogenous ligands.…”

Section: Protein‐like Functionmentioning

confidence: 99%

Protein‐like structure and activity in synthetic polymers

Cole

Hanlon

Rodriguez

et al. 2016

J. Polym. Sci. Part A: Polym. Chem.

Self Cite

View full text Add to dashboard Cite

The structure and activity of proteins is the gold standard for functional polymeric materials. This highlight seeks to calibrate the reader with respect to recent attempts to mimic the various structural and functional traits of proteins using the techniques of modern polymer chemistry. From advances in sequence-controlled polymers (primary structure), to peptidomimetics, foldamers, single-chain nanoparticles (secondary and tertiary structure), accessing the various structural aspects of protein chemistry is a vibrant research area. Likewise, the properties and utility of proteins in applications such as catalysis and molecular recognition are being emulated in the laboratory to great effect. Rather than provide an exhaustive review on any one of these topics, this article seeks to highlight the common thread among them, encouraging discussion and collaboration that will result in the next generation of smart materials with advanced structure and function.

show abstract

Porphyrin-Cored Polymer Nanoparticles: Macromolecular Models for Heme Iron Coordination

Cited by 25 publications

References 43 publications

Metal‐Folded Single‐Chain Nanoparticle: Nanoclusters and Self‐Assembled Reduction‐Responsive Sub‐5‐nm Discrete Subdomains

Metal‐Folded Single‐Chain Nanoparticle: Nanoclusters and Self‐Assembled Reduction‐Responsive Sub‐5‐nm Discrete Subdomains

Macromolecular Superstructures: A Future Beyond Single Chain Nanoparticles

Protein‐like structure and activity in synthetic polymers

Contact Info

Product

Resources

About