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2.
ACS Nano ; 2021 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-34709028

RESUMO

Harata-Kodaka's rule predicting the induced chirality of the guest molecules by cyclodextrins has been discovered in the 1970-1990s, yet its ability to control the supramolecular handedness of self-assembled structures has not been sufficiently recognized. Here we show that in a coordinating self-assembly system that is able to form racemic cone shells symmetry breaking occurs if the ligand is prethreaded into α-cyclodextrin prior to metal ion addition, and the handedness of cone shells can be rationally manipulated by creating the two scenarios of the Harata-Kadaka rule through controlling the host-guest dynamics. Since the coordination complexes have strong self-assembling ability, the coordinating ligand would dethread from the cavity of α-cyclodextrin but leaving the induced chirality to the coordinating self-assembly, thus catalyzing symmetry breaking. This work reveals that the dynamic factors such as concentration and molar ratio may play important roles in symmetry breaking at the supramolecular level. The current strategy provides a promising method for the symmetry breaking and manipulation of the handedness of self-assembled materials formed by achiral molecules.

3.
Langmuir ; 37(44): 13125-13131, 2021 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-34714092

RESUMO

Enzyme-instructed self-assembly is an increasingly attractive topic owing to its broad applications in biomaterials and biomedicine. In this work, we report an approach to construct enzyme-responsive aqueous surfactant two-phase (ASTP) systems serving as enzyme substrates by using a cationic surfactant (myristoylcholine chloride) and a series of anionic surfactants. Driven by the hydrophobic interaction and electrostatic attraction, self-assemblies of cationic-anionic surfactant mixtures result in biphasic systems containing condensed lamellar structures and coexisting dilute solutions, which turn into homogeneous aqueous phases in the presence of hydrolase (cholinesterase). The enzyme-sensitive ASTP systems reported in this work highlight potential applications in the active control of biomolecular enrichment/release and visual detection of cholinesterase.

4.
JACS Au ; 1(2): 156-163, 2021 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-34467281

RESUMO

Intelligent control over the handedness of circularly polarized luminescence (CPL) is of special significance in smart optoelectronics, information storage, and data encryption; however, it still remains a great challenge to rationally design a CPL material that displays reversible handedness inversion without changing the system composition. Herein, we show this comes true by coupling the two scenarios of Harata-Kodaka's rule on the same supramolecular platform of crystalline microtubes self-assembled from surfactant-cyclodextrin host-guest complexes. Upon coassembling a linear dye with its electronic transition dipole moment outside of the cavity of ß-CyD, the chirality transfer from the induced chirality of SDS in the SDS@2ß-CyD microtubes to the dye generates left-handed CPL at room temperature. Upon elevating temperature, the dye forms inclusion complex with ß-CyD, so that right-handed CPL is induced because the polar group of the dye is outside of the cavity of ß-CyD. This process is completely reversible. We envision that host-guest chemistry would be very promising in creating smart CPL inversion materials for a vast number of applications.

5.
Nat Commun ; 12(1): 5496, 2021 09 17.
Artigo em Inglês | MEDLINE | ID: mdl-34535652

RESUMO

Purely-organic clusterization-triggered emission (CTE) has displayed promising abilities in bioimaging, chemical sensing, and multicolor luminescence. However, it remains absent in the field of circularly polarized luminescence (CPL) due to the difficulties in well-aligning the nonconventional luminogens. We report a case of CPL generated with CTE using the solid phase molecular self-assembly (SPMSA) of poly-L-lysine (PLL) and oleate ion (OL), that is, the macroscopic CPL supramolecular film self-assembled by the electrostatic complex of PLL/OL under mechanical pressure. Well-defined interface charge distribution, given by lamellar mesophases of OL ions, forces the PLL chains to fold regularly as a requirement of optimal electrostatic interactions. Further facilitated by hydrogen bonding, the through-space conjugation (TSC) of orderly aligned electron-rich O and N atoms leads to CTE-based CPL, which is capable of transferring energy to an acceptor via a Förster resonance energy transfer (FRET) process, making it possible to develop environmentally friendly and economic CPL from sustainable and renewable materials.

6.
ACS Appl Mater Interfaces ; 13(35): 41997-42004, 2021 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-34431657

RESUMO

Wearable sensing technologies have gained increasing interest in biomedical fields because they are convenient and could efficiently monitor health conditions by detecting various physiological signals in real time. However, common film sensors often neglect body moisture and enhance the sensitivity by enhancing the conductive dopants and self-healing ability. We report in this work a supramolecular film sensor based on solid-phase molecular self-assembly (SPMSA), which smartly utilizes the body moisture to enhance the sensitivity for human-machine interaction. The carbon nanotube (CNT)-doped SPMSA film is able to capture environmental moisture quickly. Upon contact to human skin, the moisture not only promotes the junction between CNTs but also contributes to the conductivity. As a result, the sensitivity can be enhanced 4 times. In this way, we are able to obtain the highest sensitivity of 700% with the lowest CNT doping rate of 0.5%. Furthermore, the current sensor displays damage-inert sensing performance. In the presence of a hole of up to 50% of the film area, the sensitivity remains unaffected due to the decreases in the absolute conductivity of the film sensor before and after a trigger to the same extent. In this way, we have developed a new principle in the design of a film sensor for human-machine interaction, which releases the sensor from focus on promoting conductivity and self-healing materials.

7.
Langmuir ; 37(27): 8348-8355, 2021 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-34210141

RESUMO

Recent years have witnessed a growing interest in the design of enzyme-responsive molecular assemblies that hold appealing applications in the fields of disease-related sensing, imaging, and drug delivery. Cyclodextrins (CDs) are amylase-cleavable host molecules that can associate with surfactants, alkanes, alkyl amines, fatty alcohols, and aromatic compounds to form diverse supramolecular structures. In this work, we report a versatile supramolecular platform to construct enzyme-responsive nanosystems via host-guest interactions, in which complexation between CDs and surfactants eventually leads to the formation of a variety of nanostructures such as vesicles and microtubes. These supramolecular structures are capable of loading water-soluble molecules or functional nanoparticles, which can be actively released on-demand in the presence of α-amylase. This universal strategy to fabricate enzyme-responsive supramolecular systems was further demonstrated with a range of surfactants with anionic, cationic, and nonionic headgroups. Our results highlight a versatile platform for the exploration of biologically responsive self-assembly with potential applications as controlled-release systems and microrobots.


Assuntos
Ciclodextrinas , Nanopartículas , Nanoestruturas , Cátions
8.
ACS Appl Mater Interfaces ; 13(29): 34843-34850, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34254772

RESUMO

Adhesives are crucial both in nature and in diversified artificial fields, and developing environment-friendly adhesives with economic procedures remains a great challenge. We report that folic acid-based coacervates can be a new category of excellent adhesives for all kinds of surfaces with long-lasting adhesiveness. Aided by the electrostatic interaction between the π-π stacked folic acid quartets and polycations, the resultant coacervates are able to interact with diversified substrates via a polyvalent hydrogen bond, coordination, and electrostatic interactions. The adhesivity to wood is superior to the strong commercial glues, but without releasing any toxic components. Upon evaporating water, the coacervate can be casted into a non-adhesive flexible self-supporting film, which restores the adhesive coacervate immediately on contacting water with original adhesive ability. In this way, the coacervate can be facilely tailored into a double-sided tape (DST), which is convenient for storage and application under ambient conditions. Given its excellent adhesive performance, release of nontoxic gases, and convenience in storage and application, the folic acid-based DST is very promising as a new adhesive material.

9.
Cancer Biol Med ; 2021 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-33856140

RESUMO

OBJECTIVE: The proportion of patients with stage I lung adenocarcinoma (LUAD) has dramatically increased with the prevalence of low-dose computed tomography use for screening. Up to 30% of patients with stage I LUAD experience recurrence within 5 years after curative surgery. A robust risk stratification tool is urgently needed to identify patients who might benefit from adjuvant treatment. METHODS: In this first investigation of the relationship between metabolic reprogramming and recurrence in stage I LUAD, we developed a recurrence-associated metabolic signature (RAMS). This RAMS was based on metabolism-associated genes to predict cancer relapse and overall prognoses of patients with stage I LUAD. The clinical significance and immune landscapes of the signature were comprehensively analyzed. RESULTS: Based on a gene expression profile from the GSE31210 database, functional enrichment analysis revealed a significant difference in metabolic reprogramming that distinguished patients with stage I LUAD with relapse from those without relapse. We then identified a metabolic signature (i.e., RAMS) represented by 2 genes (ACADM and RPS8) significantly related to recurrence-free survival and overall survival times of patients with stage I LUAD using transcriptome data analysis of a training set. The training set was well validated in a test set. The discriminatory power of the 2 gene metabolic signature was further validated using protein values in an additional independent cohort. The results indicated a clear association between a high risk score and a very poor patient prognosis. Stratification analysis and multivariate Cox regression analysis showed that the RAMS was an independent prognostic factor. We also found that the risk score was positively correlated with inflammatory response, the antigen-presenting process, and the expression levels of many immunosuppressive checkpoint molecules (e.g., PD-L1, PD-L2, B7-H3, galectin-9, and FGL-1). These results suggested that high risk patients had immune response suppression. Further analysis revealed that anti-PD-1/PD-L1 immunotherapy did not have significant benefits for high risk patients. However, the patients could respond better to chemotherapy. CONCLUSIONS: This study is the first to highlight the relationship between metabolic reprogramming and recurrence in stage I LUAD, and is the first to also develop a clinically feasible signature. This signature may be a powerful prognostic tool and help further optimize the cancer therapy paradigm.

10.
J Colloid Interface Sci ; 597: 325-333, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-33887560

RESUMO

HYPOTHESIS: Distinguishing substituted aromatic isomers is a challenging task because of the great similarity of their physicochemical properties. Considering xylene isomers have drastically different geometrical shapes, we predict this would show great impact on the self-assembling behavior of various xylene isomer@cyclodextrin inclusion complex. EXPERIMENTS: Through host-guest crystalline self-assembly, among three isomers, only ortho-xylene is capable to form hydrogels with α-cyclodextrin. ROESY NMR, molecular simulations and circular dichroism spectra suggest that the ortho selectivity comes from the difference in the conformation of host-guest building block. The larger volume, and steric hinderance of the ortho isomer make it most possibly decrease their tendency to adopt more mobile orientations in cyclodextrin-based complex as meta and para isomers do, resulting in gel formation. FINDINGS: Herein, we report a novel, facile and environmentally-friendly protocol on the recognition of ortho benzene isomers using α-cyclodextrin through host-guest crystalline self-assembly. Visual recognition of ortho-xylene is achieved through amplifying the structural difference of xylene isomers at molecular scale into macroscopic scale. We believe this work unveils subtle rules to control macroscopic assemblies at the molecular level and highlights the potential of using macrocyclic compounds to improve the quality and reduce the energy bill for separation in petrochemical industry.

11.
J Colloid Interface Sci ; 594: 727-736, 2021 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-33789184

RESUMO

HYPOTHESIS: One of the main advances in double-chain surfactant systems has been their progress from the construction of assemblies to the transformation application in medicine and material science, especially to the drug delivery systems. Thus, it is critical to develop stimuli-responsive assemblies based on double-chain surfactants. We predicted that reversible assembly switching can be achieved by manipulation of the ternary host-guest competitive complexation among ß-cyclodextrin (ß-CD), surfactants, and designed azobenzene (Azo). EXPERIMENTS: In this work, Azo was introduced into vesicles using supramolecular assembly strategy. Vesicles are formed only when Azo moieties are in trans-form. UV switching of Azo groups led to fast disruption of the Azo@ß-CD complexes and relatively slow disintegration of the vesicles. With the alterative irradiation of UV and Vis light, the photoisomerization of azo group provokes the reversible disassembly and reassembly of vesicles. FINDINGS: This photo-responsive supramolecular strategy offered a controllable way to prepare responsive vesicles assembled from complex double-chain surfactants, such as phospholipids, which could be further used in drug delivery systems. This new perspective is instructive for the design and functional use of complex surfactants assembly. Importantly, the study results paved the way for the development of novel light-responsive assembly materials operating in aqueous media and biological field.

12.
Plant Physiol Biochem ; 160: 175-183, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33497848

RESUMO

Peanut is an important oilseed crop whose production is threatened by various abiotic and biotic stresses. Study of the molecular mechanism of salt tolerance could provide important information for the salt tolerance of this crop. WRKY transcription factors (TFs) are one of the largest TF families in plants and are involved in growth and development, defense regulation and the stress response. Here, we cloned a novel WRKY transcription factor gene belonging to the WRKY IIc subfamily, AhWRKY75, from the salt-tolerant mutant M34. The expression of AhWRKY75 was induced by NaCl stress treatment. After salt treatment, AhWRKY75-overexpressing peanuts grew better than wild-type plants. Furthermore, several genes related to the reactive oxygen species (ROS) scavenging system were up-regulated; the activities of superoxide dismutase (SOD), peroxidase (POD) and catalase (CAT) were significantly higher in transgenic lines than in non-transgenic control plants; and the malondialdehyde (MDA) and superoxide anion contents were significantly lower in transgenic lines than in control plants. The net photosynthetic rate (Pn), stomatal conductance (GS) and transpiration rate (Tr) of transgenic lines were significantly higher in transgenic plants than in control plants, and the intercellular CO2 concentration (Ci) was significantly lower in transgenic plants than in control plants. These results demonstrated that the AhWRKY75 gene conferred salt tolerance in transgenic peanut lines by improving the efficiency of the ROS scavenging system and photosynthesis under stress treatment. This study identifies a novel WRKY gene for enhancing the tolerance of peanut and other plants to salt stress.


Assuntos
Arachis , Proteínas de Plantas/fisiologia , Tolerância ao Sal , Fatores de Transcrição/fisiologia , Arachis/genética , Arachis/fisiologia , Regulação da Expressão Gênica de Plantas , Proteínas de Plantas/genética , Plantas Geneticamente Modificadas/fisiologia , Tolerância ao Sal/genética , Estresse Fisiológico , Fatores de Transcrição/genética
13.
J Cell Physiol ; 236(3): 1950-1966, 2021 03.
Artigo em Inglês | MEDLINE | ID: mdl-32722851

RESUMO

Osteolysis is a common medical condition characterized by excessive activity of osteoclasts and bone resorption, leading to severe poor quality of life. It is essential to identify the medications that can effectively suppress the excessive differentiation and function of osteoclasts to prevent and reduce the osteolytic conditions. It has been reported that Carnosol (Car), isolated from rosemary and salvia, has anti-inflammatory, antioxidative, and anticancer effects, but its activity on osteolysis has not been determined. In this study, we found that Car has a strong inhibitory effect on the receptor activator of nuclear factor-κB ligand (RANKL)-induced osteoclast differentiation dose-dependently without any observable cytotoxicity. Moreover, Car can inhibit the RANKL-induced osteoclastogenesis and resorptive function via suppressing NFATc1, which is a result of affecting MAPK, NF-κB and Ca2+ signaling pathways. Moreover, the particle-induced osteolysis mouse model confirmed that Car could be effective for the treatment of bone loss in vivo. Taken together, by suppressing the formation and function of RANKL-induced osteoclast, Car, may be a therapeutic supplementary in the prevention or the treatment of osteolysis.


Assuntos
Abietanos/uso terapêutico , Osteogênese , Osteólise/induzido quimicamente , Osteólise/tratamento farmacológico , Ligante RANK/farmacologia , Titânio/efeitos adversos , Abietanos/farmacologia , Animais , Reabsorção Óssea/complicações , Reabsorção Óssea/genética , Reabsorção Óssea/patologia , Sinalização do Cálcio/efeitos dos fármacos , Feminino , Regulação da Expressão Gênica/efeitos dos fármacos , Sistema de Sinalização das MAP Quinases/efeitos dos fármacos , Masculino , Camundongos Endogâmicos C57BL , Modelos Biológicos , Inibidor de NF-kappaB alfa/metabolismo , NF-kappa B/metabolismo , Fatores de Transcrição NFATC/metabolismo , Osteoclastos/efeitos dos fármacos , Osteoclastos/metabolismo , Osteoclastos/patologia , Osteogênese/efeitos dos fármacos , Osteogênese/genética , Osteólise/genética , Osteólise/patologia , Proteólise/efeitos dos fármacos , Crânio/efeitos dos fármacos , Crânio/patologia
15.
Zootaxa ; 4768(4): zootaxa.4768.4.4, 2020 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-33055637

RESUMO

A taxonomic review of the genus Hechinoschema is presented. A new genus, Propedicellus gen. nov., is described, and two new species Propedicellus guoliangi sp. nov. and Propedicellus qiului sp. nov. are described from China. A new combination Propedicellus vitalisi (Pic, 1925) comb. nov. is proposed. A key to species of Propedicellus is presented.


Assuntos
Besouros , Distribuição Animal , Estruturas Animais , Animais , Tamanho Corporal , Tamanho do Órgão
16.
Angew Chem Int Ed Engl ; 59(48): 21510-21514, 2020 11 23.
Artigo em Inglês | MEDLINE | ID: mdl-32779357

RESUMO

The fusion and fission behaviors of exosomes are essential for the cell-to-cell communication. Developing exosome-mimetic vesicles with such behaviors is of vital importance, but still remains a big challenge. Presented herein is an artificial supramolecular vesicle that exhibits redox-modulated reversible fusion-fission functions. These vesicles tend to fuse together and form large-sized vesicles upon oxidation, undergo a fission process and then return to small-sized vesicles through reduction. Noteworthy, the aggregation-induced emission (AIE) characteristics of the supramolecular building blocks enable the molecular configuration during vesicular transformation to be monitored by fluorescence technology. Moreover, the presented vesicles are excellent nanocarrier candidates to transfer siRNA into cancer cells.


Assuntos
Exossomos/metabolismo , Compostos de Ferro/metabolismo , Neoplasias do Colo do Útero/metabolismo , Antineoplásicos/química , Antineoplásicos/metabolismo , Antineoplásicos/farmacologia , Comunicação Celular/efeitos dos fármacos , Sobrevivência Celular/efeitos dos fármacos , Portadores de Fármacos/química , Portadores de Fármacos/metabolismo , Portadores de Fármacos/farmacologia , Exossomos/química , Feminino , Células HeLa , Humanos , Compostos de Ferro/química , Compostos de Ferro/farmacologia , Substâncias Macromoleculares/química , Substâncias Macromoleculares/metabolismo , Substâncias Macromoleculares/farmacologia , Estrutura Molecular , Oxirredução , Tamanho da Partícula , RNA Interferente Pequeno/química , RNA Interferente Pequeno/metabolismo , RNA Interferente Pequeno/farmacologia , Propriedades de Superfície , Neoplasias do Colo do Útero/tratamento farmacológico , Neoplasias do Colo do Útero/patologia
17.
ACS Appl Mater Interfaces ; 12(35): 39578-39585, 2020 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-32805932

RESUMO

Anticounterfeiting paintings are usually with limited colors and easy blurring and need to be dispersed in an environmentally unfriendly organic solvent. We report a set of water-based polyion micellar inks to solve all these problems. Upon complexation of reversible coordination polymers formed with rare earth metal ions Eu3+ and Tb3+ and the aggregation-induced emission ligand tetraphenylethylene-L2EO4 with oppositely charged block polyelectrolyte P2MVP29-b-PEO205, we are able to generate polyion micelles displaying three elementary emission colors of red (R) (ΦEu3+ = 24%), green (G) (ΦTb3+ = 7%), and blue (B) (ΦTPE = 9%). Full-spectrum emission and white light emission (0.34, 0.34) become possible by simply mixing the R, G, and B micelles at the desired fraction. Strikingly, the micellar inks remain stable even after soaking in water or organic solvents (ethyl acetate, ethanol, etc.) for 24 h. We envision that polyion micelles would open a new paradigm in the field of anticounterfeiting.

18.
ACS Appl Mater Interfaces ; 12(26): 29641-29649, 2020 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-32500997

RESUMO

Modifying different functional moieties into one platform is a conventional strategy for constructing theranostic systems. However, this strategy usually suffers from the unsatisfied efficiency of each individual function. Herein, a programmed self-assembly strategy is presented to fabricate theranostic nanoparticles, which significantly exhibit a dual-modality imaging function involving fluorescence imaging and magnetic resource imaging (MRI), and an efficient targeted therapy to cancer cells. Fluorescent vesicles are first self-assembled by aggregation-induced emission (AIE)-active molecules. Gd3+, serving as an MRI agent, is subsequently bound to the vesicles to provide highly positive charges, which have been realized to be anticancer active. Thereafter, transferrin (Tf) protein is introduced onto the surface of Gd3+ coordinated vesicles, shielding the positive charges and making the nanoparticles nontoxic to cells. With the assistance of Tf protein, the constructed nanoparticles are specifically targeted to cancer cells. Moreover, Tf proteins further peel off from nanoparticles in lysosomes due to their charge reversion, resulting in highly positive charges and heavy toxicity of nanoparticles to kill cancer cells. In the nanoparticles, each of the functional components acts as double-sided adhesive tape to glue the next layer, so that the abilities of functional components are not compromised. This strategy holds great potential for theranostic nanomedicine.


Assuntos
Nanopartículas/química , Neoplasias/diagnóstico por imagem , Nanomedicina Teranóstica/métodos , Linhagem Celular Tumoral , Humanos , Imageamento por Ressonância Magnética , Transferrina/química
19.
Cell Death Dis ; 11(3): 159, 2020 03 02.
Artigo em Inglês | MEDLINE | ID: mdl-32123165

RESUMO

Hereditary distal renal tubular acidosis (dRTA) is a rare disease of H+ excretion defect of α-intercalated cells in renal collecting duct, caused by decreased V-ATPase function due to mutations in the ATP6V1B1 or ATP6V0A4 genes. In the present study, a genetic family with 5 members of the complete dRTA phenotype were found with distal tubule H+ secretion disorder, hypokalemia, osteoporosis, and kidney stones. A variant NM_020632.2:c.1631C > T (p.Ser544Leu) in exon 16 on an ATP6V0A4 gene associated with dRTA was detected by next generation sequencing target region capture technique and verified by Sanger sequencing, which suggested that except for one of the patients who did not receive the test, the other four patients all carried the p.S544L heterozygote. In transfected HEK293T cells, cells carrying p.S544L-mut showed early weaker ATPase activity and a slower Phi recovery rate after rapid acidification. By immunofluorescence localization, it was observed that the expression level of p.S544L-mut on the cell membrane increased and the distribution was uneven. Co-immunoprecipitation showed the a4 subunit of ATP6V0A4/p.S544L-mut could not bind to the B1 subunit, which might affect the correct assembly of V-ATPase. The present study of dRTA family suggests that the p.S544L variant may be inherited in a dominant manner.


Assuntos
Acidose Tubular Renal/genética , Mutação/genética , ATPases Vacuolares Próton-Translocadoras/genética , Acidose Tubular Renal/complicações , Acidose Tubular Renal/diagnóstico , Éxons , Feminino , Perda Auditiva Neurossensorial/genética , Heterozigoto , Humanos , Rim/metabolismo , Masculino
20.
Angew Chem Int Ed Engl ; 59(25): 10081-10086, 2020 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-31633871

RESUMO

Hydration water greatly impacts the color of inorganic crystals, but it is still unknown whether hydration water can be utilized to systematically manipulate the emission color of organic luminescent groups. Now, metal ions with different hydration ability allow fine-tuning the emission color of a fluorescent group displaying aggregation induced emission (AIE). Because the hydration water can be removed easily by gentle heating or mechanical grinding and re-gained by solvent fuming, rewritable materials can be fabricated both in the hot-writing and cold-writing modes. This hydration-facilitated strategy will open up a new vista in fine-tuning the emission color of AIE molecules based on one synthesis and in the design of smart luminescent devices.

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