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1.
Chem Sci ; 12(37): 12407-12418, 2021 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-34603671

RESUMO

The simultaneous detection of multiple microRNAs (miRNAs) will facilitate early clinical diagnosis. Herein, we demonstrate the integration of multicolor fluorophore-encoded cascade signal amplification with single-molecule detection for simultaneous measurement of different miRNAs in lung cancer tissues. This assay involves two linear templates and two circular templates without the requirement of any fluorescent-labeled probes. The binding of target miRNAs to their corresponding linear templates initiates the cyclic strand displacement amplification, generating many triggers which can specifically hybridize with the corresponding biotin-labeled AP probes to initiate the apurinic/apyrimidic endonuclease 1-assisted cyclic cleavage reaction for the production of more biotin-labeled primers for each miRNA. The resultant two primers can react with their corresponding circular templates to initiate rolling circle amplification which enables the incorporation of Cy5-dCTP/Cy3-dGTP nucleotides, resulting in the simultaneous production of abundant biotin-/multiple Cy5/Cy3-labeled DNA products. After magnetic separation and exonuclease cleavage, the amplified products release abundant Cy5 and Cy3 fluorescent molecules which can be simply monitored by single-molecule detection, with Cy3 indicating miR-21 and Cy5 indicating miR-155. This assay involves three consecutive amplification reactions, enabling the conversion of extremely low abundant target miRNAs into large numbers of Cy5/Cy3 fluorophore-encoded DNA products which can release abundant fluorescent molecules for the generation of amplified signals. This assay exhibits high sensitivity, good selectivity, and the capability of multiplexed assay. This method can simultaneously quantify miR-155 and miR-21 in living cells and in lung cancer tissues, and it can distinguish the expression of miRNAs between non-small cell lung cancer patients and healthy persons. The accuracy and reliability of the proposed method are further validated by quantitative reverse transcription polymerase chain reaction.

2.
Anal Chem ; 2021 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-34648255

RESUMO

Biofouling has been a substantial burden on biomarker analysis in complex biological media, leading to poor sensitivity and selectivity or even malfunction of the sensing devices. In this work, an electrochemical biosensor with excellent antifouling ability and high stability was fabricated based on amyloid-like bovine serum albumin (AL-BSA) crosslinked with the conducting polymer polyaniline (PANI). Compared with the crosslinked conventional bovine serum albumin (BSA), the crosslinked AL-BSA exhibited enhanced antifouling capability, and it was able to form an effective antifouling film within a significantly short reaction time. With further immobilization of immunoglobulin M (IgM) antibodies onto the prepared AL-BSA surface via the formation of amide bonds, an electrochemical biosensor capable of assaying IgM in human serum samples with superior selectivity and sensitivity was constructed. The biosensor exhibited excellent antifouling performance even in 100% human serum, a low limit of detection down to 2.32 pg mL-1, and acceptable accuracy for real sample analysis compared with the standard enzyme-linked immunosorbent assay for IgM detection. This strategy of using AL-BSA to construct antifouling sensing interfaces provided a reliable diagnostic method for the detection of a series of protein biomarkers in complex biological media.

3.
Anal Chem ; 2021 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-34672523

RESUMO

Single-nucleotide polymorphisms (SNPs) are important hallmarks of human diseases. Herein, we develop a single quantum dot (QD)-mediated fluorescence resonance energy transfer (FRET) nanosensor with the integration of multiple primer generation rolling circle amplification (MPG-RCA) for sensitive detection of SNPs in cancer cells. This assay involves only a linear padlock probe for MPG-RCA. The presence of a mutant target facilitates the circularization of linear padlock probes to initiate RCA, producing three short single-stranded DNAs (ssDNAs) with the assistance of nicking endonuclease. The resulting ssDNAs can function as primers to induce cyclic MPG-RCA, resulting in the exponential amplification and generation of large numbers of linker probes. The linker probes can subsequently hybridize with the Cy5-labeled reporter probes and the biotinylated capture probes to obtain the sandwich hybrids. The assembly of these sandwich hybrids on the 605 nm-emission quantum dot (605QD) generates the 605QD-oligonucleotide-Cy5 nanostructures, resulting in efficient FRET from the 605QD to Cy5. This nanosensor is free from both the complicated probe design and the exogenous primers and has distinct advantages of high amplification efficiency, zero background signal, good specificity, and high sensitivity. It can detect SNPs with a large dynamic range of 8 orders of magnitude and a detection limit of 5.41 × 10-20 M. Moreover, this nanosensor can accurately distinguish as low as 0.001% mutation level from the mixtures, which cannot be achieved by previously reported methods. Furthermore, it can discriminate cancer cells from normal cells and even quantify SNP at the single-cell level.

4.
Anal Chem ; 93(40): 13555-13563, 2021 10 12.
Artigo em Inglês | MEDLINE | ID: mdl-34570974

RESUMO

A brief and universal ultralow fouling sensing platform capable of assaying targets in complex biofluids was developed based on designed antifouling peptides that could form a loop-closed structure with enhanced stability. The newly designed peptide with thiol groups in its two terminals self-assembled onto a gold nanoparticle (AuNP)-modified electrode surface to form a stable loop structure, which displayed excellent antifouling performance, outstanding stability under enzymatic hydrolysis, and satisfactory long-term antifouling capability in complex biofluids (clinical human serum). The antifouling and highly sensitive electrochemical aptasensor was constructed via one-step co-immobilization of the designed peptides and aptamers onto the electrode surface modified with electrodeposited poly(3,4-ethylenedioxythiophene) (PEDOT) and AuNPs. The developed peptide-based aptasensor exhibited a decent response for the analysis of the cancer antigen 125 (CA125), with a relatively wide linear range (0.1-1000 U mL-1) and a low limit of detection (0.027 U mL-1), and was capable of detecting CA125 in clinical serum samples with acceptable accuracy. This antifouling strategy-based self-assembled peptide with a loop-closed structure provided a potential path for the development of various low-fouling biosensors for application in complex biological fluids.


Assuntos
Aptâmeros de Nucleotídeos , Incrustação Biológica , Técnicas Biossensoriais , Nanopartículas Metálicas , Incrustação Biológica/prevenção & controle , Antígeno Ca-125 , Técnicas Eletroquímicas , Ouro , Humanos , Limite de Detecção , Peptídeos
5.
Anal Chem ; 93(36): 12329-12336, 2021 09 14.
Artigo em Inglês | MEDLINE | ID: mdl-34474564

RESUMO

"On-demand" accurate imaging of multiple intracellular miRNAs will significantly improve the detection reliability and accuracy. However, the "always-active" design of traditional multicomponent detection probes enables them to passively recognize and output signals as soon as they encounter targets, which will inevitably impair the detection accuracy and, inevitably, result in false-positive signals. To address this scientific problem, in this work, we developed a near-infrared (NIR) light-activated multicomponent detection intelligent nanoprobe for spatially and temporally controlled on-demand accurate imaging of multiple intracellular miRNAs. The proposed intelligent nanoprobe is composed of a rationally designed UV light-responsive triangular DNA nano sucker (TDS) and upconversion nanoparticles (UCNPs), named UCNPs@TDS (UTDS), which can enter cells autonomously through endocytosis and enable remote regulation of on-demand accurate imaging for multiple intracellular miRNAs using NIR light illumination at a chosen time and place. It is worth noting that the most important highlight of the UTDS we designed in this work is that it can resist nonspecific activation as well as effectively avoid false-positive signals and improve the accuracy of imaging of multiple intracellular miRNAs. Moreover, distinguishing different kinds of cell lines with different miRNA expressions levels can be also achieved through this NIR light-activated intelligent UTDS, showing feasible prospects in precise imaging and disease diagnosis.


Assuntos
MicroRNAs , Nanopartículas , DNA , Raios Infravermelhos , Reprodutibilidade dos Testes
6.
Anal Chim Acta ; 1176: 338750, 2021 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-34399893

RESUMO

Developing a highly sensitive immunoassay for tumor biomarkers is particularly important in bioanalysis and early disease diagnosis. In this work, a simple one-pot solvothermal method was developed for controllable synthesis of well-dispersed PtCo alloyed nanodendrites (PtCo NDs) by using l-carnosine as the co-structure-directing agent. The PtCo NDs had a large specific surface area and provided abundant active sites available for electrocatalytic oxygen reduction reaction (ORR). Based on the highly enhanced currents of the ORR, a novel label-free electrochemical immunosensor was fabricated for highly sensitive assay of carbohydrate antigen 15-3 (CA15-3). The sensor showed a wide linear range of 0.1-200 U mL-1 and a low limit of detection (LOD) down to 0.0114 U mL-1 (S/N = 3), in turn exploring its application to diluted human serum samples with satisfactory results. This study provides a feasible platform for monitoring other tumor markers in clinical diagnosis.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Anticorpos Imobilizados , Carboidratos , Catálise , Técnicas Eletroquímicas , Ouro , Humanos , Imunoensaio , Limite de Detecção , Oxigênio
7.
Anal Chim Acta ; 1176: 338779, 2021 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-34399895

RESUMO

A rationally designed multifunctional polydopamine (PDA)-coated metal-organic frameworks (MOFs) biosensors for detection of miRNA-122 with Zn2+-triggered aggregation-induced enhancement (AIE) and synergistic chem-photothermal therapy in vitro was developed for the first time. Further, it was successfully used for enhanced fluorescence imaging of miRNA-122 in living cells. The pH-responsive MOFs structure was decomposed under the influence of acidic environment, and a large amount of free Zn2+ was released as the trigger agent for AIE signal amplification, realizing the ultra-sensitive detection of miRNA-122 and the accurate discrimination of the cells with different expression levels of miRNA-122, with the detection limit as low as 12.5 pM. Meanwhile, ZIF-8 nanoparticles with high loading rate can effectively deliver therapeutic drugs to achieve responsive release. In addition, the modification of versatile PDA-coating provides the biosensor with a faster drug release capability and photothermal conversion performance, demonstrating its superior synergistic chem-photothermal therapy performance. It is expected to play an important role in the integration of cancer diagnosis and synergistic therapy.


Assuntos
Técnicas Biossensoriais , Hipertermia Induzida , Estruturas Metalorgânicas , MicroRNAs , Nanopartículas , Doxorrubicina , Humanos , Imagem Óptica , Fototerapia , Terapia Fototérmica
8.
Anal Chem ; 93(30): 10679-10687, 2021 08 03.
Artigo em Inglês | MEDLINE | ID: mdl-34288646

RESUMO

Herein, an electrochemiluminescence (ECL) microRNA biosensor based on anti-fouling magnetic beads (MBs) and two signal amplification strategies was developed. The newly designed anti-fouling dendritic peptide was wrapped on the surfaces of MBs to make them resistant to nonspecific adsorption of biomolecules in complex biological samples so as to realize accurate and selective target recognition. One of the amplification strategies was achieved through nucleic acid cycle amplification based on the DNAzyme on the surfaces of MBs. Then, the output DNA generated by the nucleic acid cycle amplification program stimulated the hybrid chain reaction (HCR) process on the modified electrode surface to generate the other amplification of the ECL response. Titanium dioxide nanoneedles (TiO2 NNs), as a co-reaction accelerator of the Ru(bpy)2(cpaphen)2+ and tripropylamine (TPrA) system, were wrapped with the electrodeposited polyaniline (PANI) on the electrode surface to enhance the ECL intensity of Ru(bpy)2(cpaphen)2+. The conducting polymer PANI can not only immobilize the TiO2 NNs but also improve the conductivity of the modified electrodes. The biosensor exhibited ultra-high sensitivity and excellent selectivity toward the detection of miRNA 21, with a detection limit of 0.13 fM. More importantly, with the anti-fouling MBs as a unique separation tool, this ECL biosensor was capable of assaying targets in complex biological media such as serum and cell lysate.


Assuntos
Incrustação Biológica , Técnicas Biossensoriais , MicroRNAs , Incrustação Biológica/prevenção & controle , Técnicas Eletroquímicas , Medições Luminescentes , Fenômenos Magnéticos
9.
Biosens Bioelectron ; 190: 113466, 2021 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-34214764

RESUMO

The development of antifouling biosensors capable of detecting biomarkers at low concentrations in complex bio-fluids with many interference components is of great importance in the diagnosis and treatment of diseases. Certain zwitterionic peptides composed of natural L-amino acids have been used for the construction of low fouling biosensors and demonstrated excellent antifouling performances, but they are prone to enzymatic degradation in biological media, such as serum that contains a variety of enzymes. In this work, a novel antifouling peptide with the sequence of cppPPEKEKEkek was designed, and three unnatural D-amino acids were set at both ends of the peptide to enhance its tolerance to enzymatic degradation. An electrochemical biosensor was constructed by coupling the antifouling peptide with a conducting polymer polyaniline (PANI) to achieve accurate detection of alpha-fetoprotein (AFP) in clinical samples. Owing to the presence of the designed peptide with partial D-amino acids (pD-peptide), the biosensing interface showed significantly high antifouling performance and enhanced stability in human serum. Meanwhile, the pD-peptide based biosensor exhibited high sensitivity toward the target AFP, with the linear range from 0.1 fg mL-1 to 1.0 ng mL-1 and the limit of detection of 0.03 fg mL-1 (S/N = 3). This strategy of enhancing the stability (tolerance to enzymolysis) of antifouling peptides in biological samples provided an effective way to develop antifouling biosensors for practical applications.


Assuntos
Incrustação Biológica , Técnicas Biossensoriais , Aminoácidos , Incrustação Biológica/prevenção & controle , Técnicas Eletroquímicas , Humanos , Peptídeos , alfa-Fetoproteínas
10.
Anal Chem ; 93(29): 10310-10316, 2021 07 27.
Artigo em Inglês | MEDLINE | ID: mdl-34260216

RESUMO

DNA methyltransferases may function as important biomarkers of cancers and genetic diseases. Herein, we develop a dye-sensitized and gold plasmon-enhanced cathodic photoelectrochemical (PEC) biosensor on the basis of p-type covalent organic polymers (COPs) for the signal-on measurement of M.SssI methyltransferase (M.SssI MTase). The cathodic PEC biosensor is constructed by the in situ growth of p-type COP films onto a glass coated with indium tin oxide and the subsequent assembly of biotin- and HS-labeled double-stranded DNA (dsDNA) probes onto the COP film via biotin-streptavidin interaction. The dsDNA probe contains the recognition sequence of M.SssI MTase. The COP thin films possess a porous ultrathin nanosheet structure with abundant active sites, facilitating the generation of a high photocurrent compared with the hydrothermally synthesized ones. The presence of DNA methyltransferases can prevent the digestion of restriction endonuclease HpaII, consequently inducing the introduction of gold nanoparticles (AuNPs) to the dsDNA probes via the S-Au bond and the intercalation of rhodamine B (RhB) into the DNA grooves to produce a high photocurrent due to the dye-photosensitized enhancement and AuNP-mediated surface plasmon resonance. However, in the absence of M.SssI MTase, HpaII digests the dsDNA probes, and neither AuNPs nor RhB can be introduced onto the electrode surface, leading to a low photocurrent. This cathodic PEC biosensor possesses high sensitivity and good selectivity, and it can screen the inhibitors and detect M.SssI MTase in serum as well.


Assuntos
Técnicas Biossensoriais , Nanopartículas Metálicas , Técnicas Eletroquímicas , Eletrodos , Ouro , Metiltransferases
11.
ACS Appl Mater Interfaces ; 13(24): 28782-28789, 2021 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-34106699

RESUMO

Herein, we synthesize the thiophene tetraphenylethene-based conjugated microporous polymer (ThT-CMP) using the tetraphenylethylene derivative [i.e., 1,1,2,2-tetrakis(4-bromophenyl)ethane (TPBE)] and 2,5-thiophenediboronic acid as the precursors. The aggregation of TPBE in the ThT-CMP can induce a strong dual-band bipolar electrochemiluminescence (AIECL) emission at 554 nm (anodic) and 559 nm (cathodic) with tri-n-propylamine (TPrA) and S2O82- as the coreactants, respectively. The anodic and cathodic ECL efficiencies are measured to be 11.49 and 3.82% with respect to the standard of the Ru(bpy)32+/TPrA system, respectively. We further develop a dipolar ECL sensor to sensitively detect rhodamine B (RhB) based on resonance energy transfer. This ECL sensor possesses a large dynamic range and high sensitivity. This research provides a new avenue of designing organic structures with the characteristic of bipolar AIECL for the development of luminescent devices.

13.
Anal Chem ; 93(19): 7355-7361, 2021 05 18.
Artigo em Inglês | MEDLINE | ID: mdl-33957042

RESUMO

A facile strategy for the electrochemical detection of human epidermal growth factor receptor 2 (HER2), a breast cancer biomarker, was presented via the fabrication of an antifouling sensing interface based on the conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) and a biocompatible peptide hydrogel. The peptide hydrogel prepared from a designed short peptide of Phe-Glu-Lys-Phe functionalized with a fluorene methoxycarbonyl group (Fmoc-FEKF) enabled excellent activity preservation for the immobilized biomolecules, and its good hydrophilicity facilitated effective alleviation of nonspecific adsorption or biofouling, while the PEDOT film provided a highly stable and conducting substrate. The developed biosensor was highly sensitive and selective for HER2 detection, with a wide linear response range from 0.1 ng mL-1 to 1.0 µg mL-1 and a low limit of detection of 45 pg mL-1. Moreover, the peptide hydrogel based biosensor was feasible to use for complex biological samples, and it was capable of detecting HER2 in human serum with clinically acceptable accuracy, manifesting a promising potential for practical application.


Assuntos
Incrustação Biológica , Técnicas Biossensoriais , Neoplasias da Mama , Incrustação Biológica/prevenção & controle , Biomarcadores Tumorais , Neoplasias da Mama/diagnóstico , Técnicas Eletroquímicas , Feminino , Humanos , Hidrogéis , Peptídeos , Receptor ErbB-2
14.
Anal Chem ; 93(22): 7879-7888, 2021 06 08.
Artigo em Inglês | MEDLINE | ID: mdl-34038093

RESUMO

A nanoflare, a conjugate of Au nanoparticles (NPs) and fluorescent nucleic acids, is believed to be a powerful nanoplatform for diagnosis and therapy. However, it highly suffers from the nonspecific detachment of nucleic acids from the AuNP surface because of the poor stability of Au-S linkages, thereby leading to the false-positive signal and serious side effects. To address these challenges, we report the use of covalent amide linkage and functional Au@graphene (AuG) NP to fabricate a covalent conjugate system of DNA and AuG NP, label-rcDNA-AuG. Covalent coating of abundant amino groups (-NH2) onto the graphitic shell of AuG NP efficiently facilitates the coupling with carboxyl-labeled capture DNA sequences through simple, but strong, amide bonds. Importantly, such an amide-bonded nanoflare possesses excellent stability and anti-interference capability against the biological agents (nuclease, DNA, glutathione (GSH), etc.). By accurately monitoring the intracellular miR-21 levels, this covalent nanoflare is able to identify the positive cancer cells even in a mix of cancer and normal cells. Moreover, it allows for efficient photodynamic therapy of the targeted cancer cells with minimized side effects on normal cells. This work provides a facile approach to develop a superstable nanosystem showing promising potential in clinical diagnostics and therapy.


Assuntos
Grafite , Nanopartículas Metálicas , Amidas , Glutationa , Ouro
15.
Mikrochim Acta ; 188(6): 217, 2021 05 31.
Artigo em Inglês | MEDLINE | ID: mdl-34057597

RESUMO

A flexible free-standing electrochemical biosensor to detect carcinoembryonic antigen (CEA) is described based on a conducting polypyrrole (PPy) nanocomposite film electrode. The conducting PPy composite was constructed by the sandwiched structure formed by PPy doped with pentaerythritol ethoxylate (PEE) and 2-naphthalene sulfonate (2-NS-PPy) separately via electropolymerization. Gold nanoparticles (AuNPs) were fixed on the PPy composite film by electrodeposition and then connected to CEA aptamer through self-assembly to construct a free-standing electrochemical biosensor breaking away from additional soft substrates and current collector. This PPy composite film-based electrochemical biosensor exhibits satisfying sensing performance for CEA detection, with a linear range from 10-10 g/mL to 10-6 g/mL and a detection limit of 0.033 ng/mL, good specificity and long-term sensing stability (96.8% of the original signal after 15 days). The biosensor also presents acceptable reproducibility with 1.7% relative standard deviation. Moreover, this electrochemical biosensor owns the deformation stability that could bear various deformations (twisting, folding, and knotting) without affecting device's sensing performance. It can even maintain 99.4% of the original signal under 25% strain deformation. Due to the superior sensing performance, high stability (mechanical deformation and long-term storage), and flexibility, this free-standing electrochemical biosensor proves huge potential in application of flexible and wearable electronics.

16.
Anal Chem ; 93(17): 6857-6864, 2021 05 04.
Artigo em Inglês | MEDLINE | ID: mdl-33890762

RESUMO

Aggregation-induced emission (AIE) active Pdots are attractive nanomaterials applied in electrochemiluminescence (ECL) fields, while the irreversible redox reaction of these Pdots is a prevailing problem, resulting in instability of ECL emission. Herein, we first designed and synthesized an AIE-active Pdot with reversible redox property, which contains a tetraphenylethene derivate and benzothiadiazole (BT) to achieve stable ECL emission. BT has a good rigid structure with excellent electrochemical behaviors, which is beneficial for avoiding the destruction of the conjugated structure as much as possible during the preparation of Pdots, thus maintaining good redox property. The tetraphenylethene derivate, as a typical AIE-active moiety, provides a channel for highly efficient luminescence in the aggregated states. The Pdots exhibited reversible and quasi-reversible electrochemical behaviors during cathodic and anodic scanning, respectively. The stable annihilation, reductive-oxidative, and oxidative-reductive ECL signals were observed. Subsequently, we constructed an ultrasensitive ECL biosensor based on the oxidative-reductive ECL mode for the detection of miRNA-21 with a detection limit of 32 aM. This work provides some inspiration for the future design of ECL materials featuring AIE-active property and stable ECL emission.

17.
Chem Commun (Camb) ; 57(34): 4178-4181, 2021 Apr 27.
Artigo em Inglês | MEDLINE | ID: mdl-33908489

RESUMO

The present study reports an aqueous synthesis approach towards Cu-In-Se/ZnS quantum dots with emission in the near-infrared spectral range. The photoluminescence of the dots can be effectively controlled by adjusting the sulfur source, to achieve increased quantum yields (four times higher) and red-shifted emission peaks (from 809 nm to 830 nm).

18.
Anal Chem ; 93(14): 5963-5971, 2021 04 13.
Artigo em Inglês | MEDLINE | ID: mdl-33797892

RESUMO

Biofouling caused by the accumulation of biomolecules on sensing surfaces is one of the major problems and challenges to realize the practical application of electrochemical biosensors, and an effective way to counter this problem is the construction of antifouling biosensors. Herein, an antifouling electrochemical biosensor was constructed based on electropolymerized polyaniline (PANI) nanowires and newly designed peptides for the detection of the COVID-19 N-gene. The inverted Y-shaped peptides were designed with excellent antifouling properties and two anchoring branches, and their antifouling performances against proteins and complex biological media were investigated using different approaches. Based on the biotin-streptavidin affinity system, biotin-labeled probes specific to the N-gene (nucleocapsid phosphoprotein) of COVID-19 were immobilized onto the peptide-coated PANI nanowires, forming a highly sensitive and antifouling electrochemical sensing interface for the detection of COVID-19 nucleic acid. The antifouling genosensor demonstrated a wide linear range (10-14 to 10-9 M) and an exceptional low detection limit (3.5 fM). The remarkable performance of the genosensor derives from the high peak current of PANI, which is chosen as the sensing signal, and the extraordinary antifouling properties of designed peptides, which guarantee accurate detection in complex systems. These crucial features represent essential elements for future rapid and decentralized clinical testing.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , RNA Viral/isolamento & purificação , SARS-CoV-2/genética , Humanos , Sondas Moleculares , Peptídeos
19.
Acta Biomater ; 128: 143-149, 2021 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-33930576

RESUMO

Development of photoliquefiable solid-state biomaterials at room temperature would address scientific challenges in life science. However, external stimuli-induced phase transitions are difficult for some biomacromolecules based materials, due to the high rigidity of these biomolecules. In this present work, by delicate molecule design on azobenzene-type ammonium surfactants, two new types of DNA-surfactant materials are fabricated. At room temperature, these DNA materials show photoliquefaction of ionic crystals to isotropic liquids under UV light, and fast self-assembly from isotropic liquids back to crystals after ceasing UV light, under the assistance of azobenzene isomerization. To achieve this objective, the designed solid-state DNA materials should have melting points near room temperature and an immediate liquid crystal to isotropic liquid transition process just above the melting points, which highly depends on the stoichiometric charge ratio between DNA and surfactants. As proved by the successful self-healing tests, these DNA ionic crystals are good biomaterials with potential applications in biomedicine and life science. This work would provide a new strategy for designing anhydrous functional biomaterials at room temperature by using rigid biomacromolecules. STATEMENT OF SIGNIFICANCE: At room temperature, solid-state biomaterials with photoregulated crystal⇄isotropic liquid phase transition property are attractive functional materials in life science, considering the body temperature and living environment temperature of human beings. Although several kinds of anhydrous materials achieved isothermal photoresponsive phase transitions, the photoregulated phase transition of anhydrous biomacromolecules based materials has not been achieved at room temperature, due to the high rigidity of these biomolecules. In this work, by delicate molecule design on ammonium surfactants, we synthesized two kinds of anhydrous DNA-surfactants ionic crystals. These DNA materials show fast photoliquefaction under UV light and self-assembly after ceasing light, which affords excellent self-healing biomaterials. This work would provide a new strategy for designing anhydrous photoresponsive biomaterials by using rigid biomacromolecules.


Assuntos
Cristais Líquidos , Tensoativos , Materiais Biocompatíveis , DNA , Humanos , Temperatura
20.
Bioelectrochemistry ; 140: 107802, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-33794412

RESUMO

Procalcitonin (PCT) is a sensitive and specific biomarker for sepsis diagnosis. In this study, a novel ratio-typed electrochemical immunosensor was constructed for reliable and sensitive assay of PCT based on hierarchical PtCoIr nanowires/polyethylene polyamine-grafted-ferrocene (PtCoIr HNWs/PEPA-Fc) and porous SiO2@Ag nanoparticles-toluidine blue (porous SiO2@Ag NPs-TB). Importantly, the PtCoIr HNWs/PEPA-Fc was first modified on the sensing interface, which harvested stable and strong electrochemical signals for readout of Fc due to the enriched anchoring sites created by the PtCoIr HNWs. Meanwhile, porous SiO2@Ag NPs-TB behaved as the label to conjugate with secondary antibody (Ab2), which also provided another strong detection signals originated from TB confined in such porous structures. The resulting immunosensor displayed a measurable output of procalcitonin (PCT) in the dynamic scope of 0.001 ~ 100 ng mL-1 with a low limit of detection (LOD) of 0.46 pg mL-1 (S/N = 3). Moreover, we exploited this strategy for PCT assay in a diluted human serum sample with acceptable results, exhibiting promising applications in the clinical analysis.


Assuntos
Técnicas Biossensoriais/métodos , Imunoensaio/métodos , Indóis/química , Nanopartículas Metálicas/química , Polímeros/química , Sepse/sangue , Dióxido de Silício/química , Prata/química , Biomarcadores/sangue , Eletroquímica , Compostos Ferrosos/química , Humanos , Limite de Detecção , Metalocenos/química , Nanofios/química , Porosidade
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