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Polyamide plays a pivotal role in engineering thermoplastics. Constrained by the harsh conditions and arduous procedures for its industrial synthesis, developing facile synthesis of polyamides is still challengeable and holds profound significance. Herein, we successfully utilized water as one of the monomers to synthesize functional polyamides under ambient conditions. A powerful multicomponent polymerization of water, isocyanides, and chlorooximes was established in phosphate-buffered saline. Soluble and thermally stable polyamides with high weight-average molecular weights (up to 53900) were obtained in excellent yields (up to 95%). The polymerization exhibits unique polymerization-induced emission characteristics, successfully converting non-emissive monomers into unconventional emissive polymers. Notably, the resultant polyamides could undergo effective post-modification via the hydroxyl-yne click reaction. By incorporating various functional groups into the polyamide, its emission color could be fine-tuned from blue to green and to red. Remarkably, the refractive index (n) of the polyamide at 589 nm could be increased from 1.6173 to 1.7227 and the Δn could be unprecedentedly as high as 0.1054 for non-heavy atom-containing polymers after post-modification, and its micron-thick films exhibited excellent transparency in the visible region. Thus, this work not only establishes a powerful polymerization toward novel polyamides but also opens up an avenue for their versatile functionalization.
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With the development of miniaturization and integration of electrical and electronic equipment, the heat accumulation problems caused by the long-term operation of devices have become more and more serious. High thermal-conductivity and high-performance plastic composites have attracted significant interest from both academia and industry. Numerous studies have been recently conducted to enhance the thermal conductivity (TC) of nanofiller-filled polymeric composites. However, the homogeneous dispersion and directional arrangement of nanofillers in the resin matrix are the key factors limiting their effectiveness in enhancing thermal conductivity. Based on the feasibility considerations of mass production and industrial application, this paper reports on a novel preparation method of Poly(decamethylene terephthalamide)/graphite nanoparticle (GNP) nanocomposites with high thermal conductivity. Without borrowing solvents or other reagents, this method can effectively strip the inexpensive scaled graphite into nanoscale for its uniform dispersion and orientation arrangement by relying only on mechanical external forces. The whole technology is simple, green, and easy to industrialize. The fillers were well-dispersed and aligned in the PA10T, which played a role in significantly enhancing the thermal conductivity of the PA10T. In addition, we found that the thermal conductivity of the composites reached 1.20 W/(m·K) at 10 wt% filler content, which was 330% higher than that of the pure matrix. The mechanical properties of the composites were also significantly improved. This work provides guidance for the easy fabrication of thermally conductive composites with aligned structures.
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Two new triarylamine-based diamine monomers, namely, N,N'-bis(4-methoxyphenyl)-N,N'-bis(4-(4-aminophenyl-4'-methoxyphenylamino)phenyl)-p-phenylenediamine (3) and N,N'-bis(4-methoxyphenyl)-N,N'-bis(4-((4-aminophenyl-1-naphthyl)amino)phenyl)-p-phenylenediamine (7), were successfully synthesized and led to two series of electroactive polyamides by polycondensation reactions with common aromatic dicarboxylic acids. The polymers demonstrated multicolored electrochromism, high optical contrast, and remarkable enhancements in redox and electrochromic stability. Compared to other triarylamine-based polymers, the studied polyamides exhibited enhanced electrochromic stability (only 3~6% decay of its coloration efficiency at 445 nm after 14,000 switching cycles) at the first oxidation stage. The polyamides also showed strong absorption in the near-infrared region upon oxidation. Polymers with multicolored electrochromism and high redox stability can be developed by incorporation of four triarylamine cores in each repeat unit and electron-donating methoxy groups on the active sites of the triphenylamine units.
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Multi-responsive nanomembranes are a new class of advanced materials that can be harnessed in complex architectures for micro and nano-manipulators, artificial muscles, energy harvesting, soft robotics, and sensors. The design and fabrication of responsive membranes must meet such challenges as trade-offs between responsiveness and mechanical durability, volumetric low-cost production ensuring low environmental impact, and compatibility with standard technologies or biological systems This work demonstrates the fabrication of multi-responsive, mechanically robust poly(1,3-diaminopropane) (pDAP) nanomembranes and their application in fast photoactuators. The pDAP films are developed using a plasma-assisted polymerization technique that offers large-scale production and versatility of potential industrial relevance. The pDAP layers exhibit high elasticity with the Young's modulus of ≈7 GPa and remarkable mechanical durability across 20-80 °C temperatures. Notably, pDAP membranes reveal immediate and reversible contraction triggered by light, rising temperature, or reducing relative humidity underpinned by a reversible water sorption mechanism. These features enable the fabrication of photoactuators composed of pDAP-coated Si nanocantilevers, demonstrating ms timescale response to light, tens of µm deflections, and robust performance up to kHz frequencies. These results advance fundamental research on multi-responsive nanomembranes and hold the potential to boost versatile applications in light-to-motion conversion and sensing toward the industrial level.
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As one of the five major engineering plastics, polyamide brings many benefits to humans in the fields of transportation, clothing, entertainment, health, and more. However, as the production of polyamide increases year by year, the pollution problems it causes are becoming increasingly severe. This article reviews the current recycling and treatment processes of polyamide, such as chemical, mechanical, and energy recovery, and degradation methods such as thermal oxidation, photooxidation, enzyme degradation, etc. Starting from the synthesis mechanism of polyamide, it discusses the advantages and disadvantages of different treatment methods of polyamide to obtain more environmentally friendly and economical treatment schemes. Finding enzymes that can degrade high-molecular-weight polyamides, exploring the recovery of polyamides under mild conditions, synthesizing environmentally degradable polyamides through copolymerization or molecular design, and finally preparing degradable bio-based polyamides may be the destination of polyamide.
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The work presents the synthesis of a series of linear polyamidoamines by polycondensation of sebacoyl dichloride with endogenous polyamines: putrescine, spermidine, spermine, and norspermidine-a biogenic polyamine not found in the human body. During the synthesis carried out via interfacial reaction, hydrophilic, semi-crystalline polymers with an average viscosity molecular weight of approximately 20,000 g/mol and a melting point of approx. 130 °C were obtained. The structure and composition of the synthesized polymers were confirmed based on NMR and FTIR studies. The cytotoxicity tests performed on human fibroblasts and keratinocytes showed that the polymers obtained with spermine and norspermidine were strongly cytotoxic, but only in high concentrations. All the other examined polymers did not show cytotoxicity even at concentrations of 2000 µg/mL. Simultaneously, the antibacterial activity of the obtained polyamides was confirmed. These polymers are particularly active against E. Coli, and virtually all the polymers obtained demonstrated a strong inhibitory effect on the growth of cells of this strain. Antimicrobial activity of the tested polymer was found against strains like Staphylococcus aureus, Staphylococcus epidermidis, and Pseudomonas aeruginosa. The broadest spectrum of bactericidal action was demonstrated by polyamidoamines obtained from spermine, which contains two amino groups in the repeating unit of the chain. The obtained polymers can be used as a material for forming drug carriers and other biologically active compounds in the form of micro- and nanoparticles, especially as a component of bactericidal creams and ointments used in dermatology or cosmetology.
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Escherichia coli , Espermidina/análogos & derivados , Espermina , Humanos , Espermina/farmacología , Poliaminas/farmacología , Antibacterianos/farmacología , Polímeros/farmacologíaRESUMEN
Transcription therapy is an emerging approach that centers on identifying the factors associated with the malfunctioning gene transcription machinery that causes diseases and controlling them with designer agents. Until now, the primary research focus in therapeutic gene modulation has been on small-molecule drugs that target epigenetic enzymes and critical signaling pathways. However, nucleic acid-based small molecules have gained popularity in recent years for their amenability to be pre-designed and realize operative control over the dynamic transcription machinery that governs how the immune system responds to diseases. Pyrrole-imidazole polyamides (PIPs) are well-established DNA-based small-molecule gene regulators that overcome the limitations of their conventional counterparts owing to their sequence-targeted specificity, versatile regulatory efficiency, and biocompatibility. Here, we emphasize the rational design of PIPs, their functional mechanisms, and their potential as targeted transcription therapeutics for disease treatment by regulating the immune response. Furthermore, we also discuss the challenges and foresight of this approach in personalized immunotherapy in precision medicine.
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Ácidos Nucleicos , Humanos , ADN , InmunidadRESUMEN
Despite the polymer industry's reliance on nylon polymers, numerous questions remain about their crystal structures, modeling, and other features. This work discusses the thermodynamic properties and molecular modeling of a polyamides nylon 66α, 610α, and 77γ crystal structure systems for use in various electronics and Nano-devices that feature distinct properties such as exceptional optoelectronic properties at a low cost compared to other structures. This study looked at the crystal structure of a linear polyamide chain made up of repeating units. The influence of the thermal expansion coefficient and thermodynamic parameters on crystal structures' characteristics at different temperatures has previously been explored. The findings of this study demonstrate, on the one hand, the influence of the amorphous phase on the final thermodynamic characteristics of semi-crystalline polymers and, on the other hand, pave the way for greater improvement in the durability of these polymers by increasing their crystalline features. The values of the thermodynamic parameters for nylon 66α, 610α and 77γ such as enthalpy (ΔHExp.) were 35.08, 40.25, and 1.44 kJ/mol, entropy (ΔSExp.) 113.75, 128.84, and 15.10 J/mol-K, free energy (ΔGExp.) was -44.57, -46.62, and -6.86 kJ/mol, respectively. When the nylon data is compared, the nylon 610α exhibits a significantly higher free energy, at high temperatures, the process is spontaneous and exergonic, making it a potentially viable material for use as fibers and engineering thermoplastics.
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Gradient porous materials, particularly carbon-based materials, hold immense potential in the fields of batteries, energy storage, electrocatalysis, and sensing, among others, by synergistically combining the attributes associated with each pore size within a unified structural framework. In this study, we developed a gradient porous aramid (GP-Aramid) by incorporating cellulose acetate as a porosity promoter in the polymer casting solution in different proportions. These GP-Aramids were subsequently transformed into their pyrolyzed counterparts (GP-Pyramids), retaining their original structures while displaying diverse cellular or dense microstructures inherited from the parent aramid, as confirmed via scanning electron microscopy. X-ray diffraction spectra provided evidence of the conversion of aramids into carbonaceous materials. The materials showed structural defects observed through the intensity ratio of the G and D bands (ID/IG = 1.05) in the Raman spectra, while X-ray photoelectron spectra (XPS) revealed that the carbonization process yielded pyrolyzed carbon materials unusually rich in nitrogen (6%), oxygen (20%), and carbon (72%), which is especially relevant for catalysis applications. The pyrolyzed materials showed bulk resistivities from 5.3 ± 0.3 to 34.2 ± 0.6 depending on the meta- or para-orientation of the aramid and the porous structure. This work contributes to understanding these gradient porous aromatic polyamides' broader significance and potential applications in various fields.
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The use of polymers in the transportation industry represents a great opportunity to meet the growing demand for lightweight structures and to reduce polluting emissions. In this context, additive manufacturing represents a very effective fabrication route for mechanical components with sophisticated geometry that cannot be pursued by conventional methods. However, understanding the mechanical properties of 3D-printed polymers plays a crucial role in the performance and durability of polymer-based products. Polyamide is a commonly used material in 3D printing because of its excellent mechanical properties. However, the layer-by-layer deposition process and ensuing auxiliary steps (e.g., post-processing heating) may affect the microstructure and mechanical properties of 3D-printed nylon with respect to the bulk counterpart. In this work, we explore the effect of displacement rate and heat exposure on the mechanical properties of 3D-printed polyamide (PA12) specimens obtained by selective laser sintering (SLS). Moreover, the thermal characteristics of the powders and sintered material were evaluated using differential scanning calorimetry (DSC). Our results highlight the expected rate dependency of mechanical properties and show that a post-processing heat treatment partly affects mechanical behavior.
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The aim of this study was to compile a detailed phytochemical profile and assess the antioxidant properties of bee-collected pollen (PBP) obtained from corn poppy (Papaver rhoeas L.) plants. To achieve this, a lipid fraction was prepared for quantifying fatty acids using GC-FID. Extractable and alkaline-hydrolysable PBP fractions (obtained from a defatted sample) were used to determine the qualitative and quantitative profiles of phenolic compounds, phenylamides and alkaloids using UHPLC/Q-ToF-MS. Additionally, various spectrophotometric assays (TAC, FRP, CUPRAC, DPPHâ¦) were conducted to evaluate the antioxidant properties. Phenolic compounds were more present in the extractable fraction than in the alkaline-hydrolysable fraction. Luteolin was the predominant compound in the extractable fraction, followed by tricetin and various derivatives of kaempferol. This study presents one of the first reports on the quantification of tricetin aglycone outside the Myrtaceae plant family. The alkaline-hydrolysable fraction exhibited a different phenolic profile, with a significantly lower amount of phenolics. Kaempferol/derivatives, specific compounds like ferulic and 5-carboxyvanillic acids, and (epi)catechin 3-O-gallate were the predominant compounds in this fraction. Regarding phenylamides, the extractable fraction demonstrated a diverse range of these bioactive compounds, with a notable abundance of different spermine derivatives. In contrast, the hydrolysable fraction contained six spermine derivatives and one spermidine derivative. The examined fractions also revealed the presence of seventeen different alkaloids, belonging to the benzylisoquinoline, berberine and isoquinoline classes. The fatty-acid profile confirmed the prevalence of unsaturated fatty acids. Furthermore, both fractions exhibited significant antioxidant activity, with the extractable fraction showing particularly high activity. Among the assays conducted, the CUPRAC assay highlighted the exceptional ability of PBP's bioactive compounds to reduce cupric ions.
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Thiazol-based molecules have practically infinite biological implementation. Today, there are many medical applications for compounds containing the thiazole moiety owing to their presence in most clinically applied anticancer drugs, such as dasatinib, dabrafenib, ixabepilone, patellamide A and epothilone. In this study, the polycondensation, of a new group of thiazole-containing polyamides with the formulas PA1-4 was carried out by the interaction of 2-aminothiazole diphenyl sulfide and variable diacid chlorides in dimethyl formamide in the presence of potassium carbonate anhydrous as a catalyst. Fourier transform-infrared spectroscopy (FTIR) was initially used to figure out the PA1-4 structures, which were further characterized using solubility, gel permeation chromatography (GPC), X-ray diffraction analyses (XRD) and scanning electron microscopy (SEM). The solubility results revealed that the presence of heteroaromatic thiazole ring units and sulfur content in the polyamides main chain, made the solubility easier as it increases the chain packing distance. From the values of average molecular weight, it was clear that all synthesized polyamides have almost the same chain length which ranged from 37,561.80 to 39,827.66. Moreover, the thermogravimetric analysis (TGA) confirm that PA1-4 were thermally stable even at high temperatures especially the polyamides which were synthesized from aromatic diacid chlorides. Furthermore, the newly synthesized polyamides were investigated for their antimicrobial properties against different species of Gram-positive and Gram-negative bacteria and also against different fungi. The results revealed that compound PA2 showed the highest antibacterial activity. Also, their inhibitory activity against breast carcinoma cells (MCF-7 cell line) and colon carcinoma cells (HCT cell line) was evaluated. It was clear that there was an enhancement in the anticancer activity for the synthesized polyamides owing to the presence of the thiazole moiety as well as sulfur linkage. According to the results of the 50% inhibitory concentration (IC50), the synthesized polymers were found to be more active against the MCF-7 cell line than the HCT cell line.
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Chiral aggregation-induced emission (AIE) molecules have drawn attention for their helical self-assembly and special optical properties. The helical self-assembly of AIE-active chiral non-linear main-chain polymers can produce some desired optical features. In this work, a series of V-shaped chiral AIE-active polyamides P1-C3, P1-C6, P1-C12 and linear P2-C3, P2-C6, bearing n-propyl/hexyl/dodecyl side-chains, based on tetraphenylbutadiene (TPB), were prepared. All target main-chain polymers exhibit distinct AIE characteristics. The polymer P1-C6 with moderate length alkyl chains shows better AIE properties. The V-shaped main-chains and the chiral induction of (1R,2R)-(+)-1,2-cyclohexanediamine in each repeating unit promote the polymer chains display helical conformation, and multiple helical polymer chains induce nano-fibers helicity when the polymer chains aggregate and self-assemble in THF/H2 O mixtures. Simultaneously, the helical conformation polymer chains and helical nano-fibers cause P1-C6 produce strong circular dichroism (CD) signals with positive Cotton effect. Moreover, P1-C6 could also occur fluorescence quenching response to Fe3+ selectively with a low detection limit of 3.48â µmol/L.
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The preservation of nucleus structure during microscopy imaging is a top priority for understanding chromatin organization, genome dynamics, and gene expression regulation. In this review, we summarize the sequence-specific DNA labelling methods that can be used for imaging in fixed and/or living cells without harsh treatment and DNA denaturation: (i) hairpin polyamides, (ii) triplex-forming oligonucleotides, (iii) dCas9 proteins, (iv) transcription activator-like effectors (TALEs) and (v) DNA methyltransferases (MTases). All these techniques are capable of identifying repetitive DNA loci and robust probes are available for telomeres and centromeres, but visualizing single-copy sequences is still challenging. In our futuristic vision, we see gradual replacement of the historically important fluorescence in situ hybridization (FISH) by less invasive and non-destructive methods compatible with live cell imaging. Combined with super-resolution fluorescence microscopy, these methods will open the possibility to look into unperturbed structure and dynamics of chromatin in living cells, tissues and whole organisms.
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Técnicas Biosensibles , Hibridación Fluorescente in Situ/métodos , ADN/química , Cromatina/genética , Microscopía Fluorescente/métodosRESUMEN
Laser-based powder bed fusion (LPBF) of polymers allows for the additive manufacturing of dense components with high mechanical properties. Due to inherent limitations of present material systems suitable for LPBF of polymers and required high processing temperatures, the present paper investigates the in situ modification of material systems using powder blending of p-aminobenzoic acid and aliphatic polyamide 12, followed by subsequent laser-based additive manufacturing. Prepared powder blends exhibit a considerable reduction of required processing temperatures dependent on the fraction of p-aminobenzoic acid, allowing for the processing of polyamide 12 at a build chamber temperature of 141.5 °C. An elevated fraction of 20 wt% of p-aminobenzoic acid allows for obtaining a considerably increased elongation at break of 24.65% ± 2.87 while exhibiting a reduced ultimate tensile strength. Thermal investigations demonstrate the influence of the thermal material history on thermal properties, associated with the suppression of low-melting crystalline fractions, yielding amorphous material properties of the previously semi-crystalline polymer. Based on complementary infrared spectroscopic analysis, the increased presence of secondary amides can be observed, indicating the influence of both covalently bound aromatic groups and hydrogen-bound supramolecular structures on emerging material properties. The presented approach represents a novel methodology for the energy-efficient in situ preparation of eutectic polyamides, potentially allowing for the manufacturing of tailored material systems with adapted thermal, chemical, and mechanical properties.
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The growing quantities of plastic waste have raised environmental concerns, with almost a quarter of disposed plastics being sent to landfill. This has motivated research efforts into various recycling technologies to ease dependence on fossil resources, increasing circularity. Irradiation of various kinds, such as electron beam, beta and gamma rays, has been studied in the past as a way of revamping end-of-life polymer properties. The present work focuses on the effects of gamma radiation on the processability of new and recycled polymers, which is intimately linked with their rheological properties. In this study, both virgin and recycled polymers were irradiated under different radiation doses and the effects of the radiation on their viscosity assessed and compared. Results were analyzed making use of different theoretical relationships, and the causes of the changes in rheology were investigated by means of various characterization techniques, such as GPC, FTIR, EPR and DSC. Finally, the rheological curves of all samples were fitted to the Ostwald-de Waele relationship and the dependence of its parameters on the absorbed dose fitted to a function.
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Recently, bio-based manufacturing processes of value-added platform chemicals and polymers in biorefineries using renewable resources have extensively been developed for sustainable and carbon dioxide (CO2) neutral-based industry. Among them, bio-based diamines, aminocarboxylic acids, and diacids have been used as monomers for the synthesis of polyamides having different carbon numbers and ubiquitous and versatile industrial polymers and also as precursors for further chemical and biological processes to afford valuable chemicals. Until now, these platform bio-chemicals have successfully been produced by biorefinery processes employing enzymes and/or microbial host strains as main catalysts. In this review, we discuss recent advances in bio-based production of diamines, aminocarboxylic acids, and diacids, which has been developed and improved by systems metabolic engineering strategies of microbial consortia and optimization of microbial conversion processes including whole cell bioconversion and direct fermentative production.
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Diaminas , Nylons , Nylons/metabolismo , Diaminas/metabolismo , Polímeros , Ingeniería Metabólica , FermentaciónRESUMEN
The adoption of new synthesis strategy and monomers significantly promotes the construction of porous organic polymers (POPs) and their promising applications. A fabricating method of porous polyimides is developed via sequential imidization and cross-linking reaction among self-condensable building blocks, as reported in the authors' previous manuscript. Herein, porous polyureas (A-POPs) are prepared starting from 4-ethynylaniline and diisocyanate monomers, while porous polyamides (B-POPs) are synthesized from 4-ethynylbenzoic acid and diisocyanate monomers. It is found that decreasing the monomer content in solvent can effectively inhibit the premature phase separation and facilitate the evolution of integrated network. Eventually, a maximum surface area of 425 m2 g-1 is achieved for porous polyureas when the content of monomers is 10%. To the best knowledge, A-POPs are the porous polyureas with the highest surface areas reported up to now. The as-prepared porous polyurea (AN-POP) exhibits the maximum adsorption capacity of 1093.87 ± 5.23 mg g-1 and removal rate of 99.96% for Au(III), due to its high surface area and the coordination between the heteroatoms (N and O) in A-POPs and metal ions. Besides, the porous polyurea also exhibits excellent renewable efficiency and high selectivity to Au(III).
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Nylons , Polímeros , Adsorción , PorosidadRESUMEN
Objectives: This study aimed to assess the color stability, surface roughness, and flexural properties of the injection-molded thermoplastic polyamide Vertex ThermoSens denture base resin following a 3-minute immersion in Polident 3-minute denture cleanser. Methods: Sixty specimens (Vertex ThermoSens) were processed and divided into two main groups (n = 30) based on the type of test. Group 1 was further subdivided into two subgroups (n = 15): the control group immersed in distilled water (G1DW) and the test group immersed in Polident cleanser solution (G1PD). Group 2 was divided into three subgroups: a non-immersed group (G2None), a group immersed in distilled water (G2DW), and a group immersed in Polident cleanser solution (G2PD). Color change (∆E) and surface roughness measurements were conducted for group 1, and flexural modulus (E) test was performed for group 2. The CIE Lab* formula was utilized to calculate ∆E. An optical 3D surface analyzer and a three-point bending test were employed for surface roughness and E assessments, respectively. Data were subjected to statistical analysis using a paired-sample t-test for differences within each group before and after immersion. Furthermore, independent-sample t-tests and one-way ANOVA were conducted to analyze differences between groups. A significance level of P < 0.05 was considered. Results: The results revealed a slight, statistically insignificant (P > 0.05) ∆E in all color components (L*, a*, b*) after immersion in distilled water. However, after immersion in the denture cleanser, only the L* component exhibited a statistically significant ∆E (P = 0.002), which was slight in magnitude. Additionally, a significant difference was found in the ∆E between G1DW and G1PD, with G1PD showing a higher change (P = 0.007). A significant increase in surface roughness after immersion was observed in G1PD (P = 0.017), with a notable difference between G1DW and G1PD. However, the E remained unaffected (P = 0.537). Conclusion: Denture cleansers have the potential to modify the properties of thermoplastic polyamide resin. Further research is needed to explore the clinical implications of these observed changes on denture performance.
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Malignancy of medulloblastoma depends on its molecular classification. Sonic Hedgehog (SHH)-type medulloblastoma with p53 mutation was recognized as one of the most aggressive types of tumors. We developed a novel drug, chlorambucil-conjugated PI-polyamides (Chb-M'), which was designed to compete with the RUNX consensus DNA-binding site. Chb-M' specifically recognizes this consensus sequence and alkylates it to inhibit the RUNX transcriptional activity. In-silico analysis showed all the RUNX families were upregulated in the SHH-type medulloblastoma. Thus, we tested the anti-tumor effects of Chb-M' in vitro and in vivo using Daoy cell lines, which belong to SHH with p53 mutation. Chb-M' inhibited tumor growth of Daoy cells by inducing apoptosis. The same inhibitory effect was also observed by knocking down of RUNX1 or RUNX2, but not RUNX3. Apoptosis array analysis showed that Chb-M' treatment induced phosphorylation of p53 serine 15 residues. In a subcutaneous tumor model, intratumoral injection of Chb-M' induced tumor growth retardation. Chb-M' mediated inhibition of RUNX1 and RUNX2 can be a novel therapeutic strategy for SHH-type medulloblastoma with p53 mutation.