Alkaline Phosphatase-Instructed Self-Assembly of Gadolinium Nanofibers for Enhanced T<sub>2</sub>-Weighted Magnetic Resonance Imaging of Tumor

Liu, Dong; Qian, Junchao; Hai, Zijuan; Xu, Jinyong; Du, Wei; Zhong, Kai; Liang, Gaolin

doi:10.1021/acs.analchem.7b00621

Cited by 72 publications

(52 citation statements)

References 28 publications

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“…Such kinetic control may be particularly useful for selectively targeting the desired cancer cells, 51 thus greatly reducing the off-target effects of assemblies. Although in this work we demonstrate the use of EISA for inhibiting cancer cells, the insights obtained here should be applicable to other applications, like molecular imaging, 25 , 52 analyte detection, 53 and vaccine adjuvants, 6 as well as the understanding of cytotoxicity of pathogenic assemblies (e.g., β-amyloids). 54 Moreover, the recent advances in structural biology and cell biology have revealed that nature uses a dynamic continuum of protein assemblies to control cellular processes.…”

Section: Discussionmentioning

confidence: 88%

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Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

et al. 2017

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Enzyme-instructed self-assembly (EISA) represents a dynamic continuum of supramolecular nanostructures that selectively inhibits cancer cells via simultaneously targeting multiple hallmark capabilities of cancer, but how to design the small molecules for EISA from the vast molecular space remains an unanswered question. Here we show that the self-assembling ability of small molecules controls the anticancer activity of EISA. Examining the EISA precursor analogues consisting of an N-capped d-tetrapeptide, a phosphotyrosine residue, and a diester or a diamide group, we find that, regardless of the stereochemistry and the regiochemistry of their tetrapeptidic backbones, the anticancer activities of these precursors largely match their self-assembling abilities. Additional mechanistic studies confirm that the assemblies of the small peptide derivatives result in cell death, accompanying significant rearrangement of cytoskeletal proteins and plasma membranes. These results imply that the diester or diamide derivatives of the d-tetrapeptides self-assemble pericellularly, as well as intracellularly, to result in cell death. As the first case to correlate thermodynamic properties (e.g., self-assembling ability) of small molecules with the efficacy of a molecule process against cancer cells, this work provides an important insight for developing a molecular dynamic continuum for potential cancer therapy, as well as understanding the cytotoxicity of pathogenic assemblies.

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Section: Discussionmentioning

confidence: 88%

“…Despite the promise of EISA in selectively inhibiting cancer cells or molecular imaging, 25 there are several important questions that remain to be answered. Of special significance is how to design a small molecule for EISA.…”

Section: Introductionmentioning

confidence: 99%

Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

et al. 2017

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“…It was speculated that the reason behind this phenomenon is the poor interaction between the CsgA or CsgA‐DDDEEK nanofibers. Meanwhile, the values of G ′ were larger than those of G ″ in the whole range (0.1–10 Hz), indicating that the BL21‐Gold (DE3) cells with CsgA or BL21‐Gold (DE3) mutants with CsgA‐DDDEEK can withstand external shear force to some extent . The interaction force was BL21‐Gold (DE3) mutants > BL21‐Gold (DE3) cells > wt‐ E. coli , indicating that CsgA or CsgA‐DDDEEK played a key role in their mechanical property.…”

Section: Resultsmentioning

confidence: 97%

A Universal and Ultrastable Mineralization Coating Bioinspired from Biofilms

Xiao

Wang

et al. 2018

Adv Funct Materials

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A simple and universal method for manufacturing a mineralization coating on various surfaces is developed using a biofilm-based material obtained from engineered curli nanofibers. The amyloid protein (CsgA) is the main proteinaceous component in the Escherichia coli (E. coli) biofilm, which can withstand detergents in the harsh environment. The peptide sequence DDDEEK is bioinspired from salivary acquired pellicles in the dental plaque biofilm, having a strong ability to absorb mineral ions and induce the formation of biominerals. The bioinspired coating is successfully secreted by the engineered E. coli, which is transformed with a recombinant plasmid for expression with T7 promoter (PET), namely PET-22b-CsgA-DDDEEK plasmid. The uniform coating can bear shear force and stay on virtually any type of material surface for at least one month. Moreover, the coated slices had a good mineralization performance and better stability than hydroxyapatite (HA)-spray slices. Furthermore, MG63 cells on the bioactive HA layer induced by the coating possess a better growth capacity than those on the commercial product Matrigel. The animal experiment results suggest that the coated Ti 6 Al 4 V screws with induced HA present better osteogenicity and osseointegration than HAsprayed screws after 12 weeks, as well as no extra immunogenicity. Thus, the coating is highly promising for biomedical applications.

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“…In vivo MRI results suggested that only the apoptotic tumors in the mice intravenously injected with Fe 3 O 4 @5 NPs , but not those in other three groups, had obviously enhanced T 2 ‐weighted MR contrast. Interestingly, Liang and co‐workers recently found that intracellular alkaline phosphatase (ALP) instructed self‐assembly of a Gd peptide into supramolecular hydrogel could be used for enhanced T 2 ‐weighted MRI of the enzyme activity in vitro and in tumor . T 1 and T 2 ‐weighted phantom MRI indicated that the r 1 value of the hydrogel (8.89 m m −1 s −1 ) is a little higher than that of Gd(III)‐diethylenediaminepentaacetic acid (Gd‐DTPA) (4.62 m m −1 s −1 ) while the r 2 value of the hydrogel (61.5 m m −1 s −1 ) is one order of magnitude higher than that of Gd‐DTPA (4.40 m m −1 s −1 ) at 9.4 T. This result suggests that the intracellular self‐assembled Gd‐nanofibers in hydrogels greatly reduce the transverse relaxation time T 2 but not the longitudinal relaxation time T 1 of surrounding water protons.…”

Section: Intracellular Self‐assembly Of Nanoprobes For Mrimentioning

confidence: 99%

Intracellular Self‐Assembly of Nanoprobes for Molecular Imaging

Hai

Liang

2018

Adv. Biosys.

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being conjugated with targeting warheads and loaded with a large number of diverse imaging agents, the multifunctional NPs are fabricated for multimodal imaging with enhanced imaging sensitivity and selectivity. Second, the uptake of NPs with appropriate size by the kidney (renal clearance) and reticular endothelial system of the liver is lower. Therefore, increased circulation time and more chances to reach the target site are achieved by NPs than small molecules. [6] Third, due to the enhanced permeability and retention effect induced by the fenestrated vasculature structures, NPs are more efficiently accumulated at the vascular angiogenic sites like tumors. [7] Fourth, once uptaken by the cells (or tissues), NPs always have longer retention time (i.e., aggregation/assembly-induced retention effect) in the cells (or the bodies) than small molecular probes, which is good for molecular imaging. [8] Nevertheless, NPs always face the problems of reproducibility and quantification, difficulty in their fabrication, as well as cell membrane translocation when applied for molecular imaging. [9] Luckily, a "smart" intracellular self-assembly strategy emerged at the right moment to overcome the above limitations of NPs, which starts with a small molecular probe to quickly translocate cell membrane but ends up with nanostructures (nanoparticles or nanofibers) with amplified imaging signals and longer retention time at the targeted sites. Intracellular Self-Assembly of NanoprobesSelf-assembly is a prevalent and important process in nature, for example, the 25 nm wide microtubules to govern cellular mitosis, 5-6 nm thick cell membranes to maintain cell integrity, and 2 nm wide DNA double strand to store genetic information are the typical presentations of molecular self-assembly in biological systems. [10] Molecular self-assembly is a "bottomup" fabrication process in which small building blocks selfassemble through various noncovalent interactions (e.g., π-π stacking, hydrogen bonding, metal coordination, host-guest interaction, electrostatic, hydrophobic, and van der Waals interactions) to build up highly ordered nanostructures. [11] Up to date, lots of self-assembly systems have been developed to ex situ or in situ fabricate biocompatible nanomaterials for biomedical applications. [8] Compared with ex situ self-assembly, in situ self-assembly (e.g., intracellular self-assembly) in which small molecules transform into nanoprobes under intelligent Molecular imaging can be roughly defined as the characterization and measurement of biological processes at the molecular and cellular level. Nanoprobes (NPs) are advantageous over small molecular probes for molecular imaging in the amount of signaling molecule as well as signal intensity. Compared with ex situ self-assembling strategies for NP fabrication, those intracellular intelligent self-assembling strategies that use small molecules to prepare NPs in situ with amplified signals and longer retention time are more efficient and attractive. This review summarizes recent adva...

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Alkaline Phosphatase-Instructed Self-Assembly of Gadolinium Nanofibers for Enhanced T₂-Weighted Magnetic Resonance Imaging of Tumor

Cited by 72 publications

References 28 publications

Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

A Universal and Ultrastable Mineralization Coating Bioinspired from Biofilms

Intracellular Self‐Assembly of Nanoprobes for Molecular Imaging

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Alkaline Phosphatase-Instructed Self-Assembly of Gadolinium Nanofibers for Enhanced T2-Weighted Magnetic Resonance Imaging of Tumor

Cited by 72 publications

References 28 publications

Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

Self-Assembling Ability Determines the Activity of Enzyme-Instructed Self-Assembly for Inhibiting Cancer Cells

A Universal and Ultrastable Mineralization Coating Bioinspired from Biofilms

Intracellular Self‐Assembly of Nanoprobes for Molecular Imaging

Contact Info

Product

Resources

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Alkaline Phosphatase-Instructed Self-Assembly of Gadolinium Nanofibers for Enhanced T₂-Weighted Magnetic Resonance Imaging of Tumor