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1.
Small ; 20(33): e2312120, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38558528

RESUMO

The tunable properties of 2D transition-metal dichalcogenide (TMDs) materials are extensively investigated for high-performance and wavelength-tunable optoelectronic applications. However, the precise modification of large-scale systems for practical optoelectronic applications remains a challenge. In this study, a wafer-scale atomic assembly process to produce 2D multinary (binary, ternary, and quaternary) TMDs for broadband photodetection is demonstrated. The large-area growth of homogeneous MoS2, Ni0.06Mo0.26S0.68, and Ni0.1Mo0.9S1.79Se0.21 is carried out using a succinct coating of the single-source precursor and subsequent thermal decomposition combined with thermal evaporation of the chalcogen powder. The optoelectrical properties of the multinary TMDs are dependent on the combination of heteroatoms. The maximum photoresponsivity of the MoS2-, Ni0.06Mo0.26S0.68-, and Ni0.1Mo0.9S1.79Se0.21-based photodetectors is 3.51 × 10-4, 1.48, and 0.9 A W-1 for 532 nm and 0.063, 0.42, and 1.4 A W-1 for 1064 nm, respectively. The devices exhibited excellent photoelectrical properties, which is highly beneficial for visible and near-infrared (NIR) photodetection.

2.
Small ; 18(40): e2203653, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-36048144

RESUMO

High-quality lead sulfide (PbS) films are deposited on selected substrate chemistries by an H2 S-free metal-organic chemical vapor deposition (MOCVD) process using a single-source metal-organic complex (Pb(dmampS)2 ). The complex is synthesized via a salt metathesis reaction between PbCl2  and lithium 1-(dimethylamino)-2-methylpropane-2-thiolate (Li(dmampS)) in diethyl ether. Subsequent film deposition is conducted by a simple thermolysis process in the absence of H2 S, yet chemical and structural analysis confirm chemically stoichiometric and homogenous films. Mechanistic studies with electron impact mass spectroscopy (EIMS) and gas chromatography mass spectroscopy (GCMS) suggest the selective cleavage of C-S bonds in the complex as the reason for the facile PbS formation with negligible impurity incorporation. The high crystallinity, low hole concentrations, and charge transport properties comparable and in many cases superior to films produced by atomic layer deposition (ALD) testify to the quality of the films. Lastly, rigid and flexible photodetectors fabricated with the PbS films exhibit considerably high photocurrents, reliable switching characteristics, and high sensitivity over a broad spectral bandwidth, highlighting the potential for realizing practical broadband photodetectors.

3.
J Proteome Res ; 19(12): 4867-4883, 2020 12 04.
Artigo em Inglês | MEDLINE | ID: mdl-33206527

RESUMO

We previously reported that human carboxylesterase 1 (CES1), a serine esterase containing a unique N-linked glycosyl group at Asn79 (N79 CES1), is a candidate serological marker of hepatocellular carcinoma (HCC). CES1 is normally present at low-to-undetectable levels in normal human plasma, HCC tumors, and major liver cancer cell lines. To investigate the potential mechanism underlying the suppression of CES1 expression in liver cancer cells, we took advantage of the low detectability of this marker in tumors by overexpressing CES1 in multiple HCC cell lines, including stable Hep3B cells. We found that the population of CES1-overexpressing (OE) cells decreased and that their doubling time was longer compared with mock control liver cancer cells. Using interactive transcriptome, proteome, and subsequent Gene Ontology enrichment analysis of CES1-OE cells, we found substantial decreases in the expression levels of genes involved in cell cycle regulation and proliferation. This antiproliferative function of the N79 glycan of CES1 was further supported by quantitative real-time polymerase chain reaction, flow cytometry, and an apoptosis protein array assay. An analysis of the levels of key signaling target proteins via Western blotting suggested that CES1 overexpression exerted an antiproliferative effect via the PKD1/PKCµ signaling pathway. Similar results were also seen in another HCC cell line (PLC/RFP/5) after transient transfection with CES1 but not in similarly treated non-HCC cell lines (e.g., HeLa and Tera-1 cells), suggesting that CES1 likely exerts a liver cell-type-specific suppressive effect. Given that the N-linked glycosyl group at Asn79 (N79 glycan) of CES1 is known to influence CES1 enzyme activity, we hypothesized that the post-translational modification of CES1 at N79 may be linked to its antiproliferative activity. To investigate the regulatory effect of the N79 glycan on cellular growth, we mutated the single N-glycosylation site in CES1 from Asn to Gln (CES1-N79Q) via site-directed mutagenesis. Fluorescence 2-D difference gel electrophoresis protein expression analysis of cell lysates revealed an increase in cell growth and a decrease in doubling time in cells carrying the N79Q mutation. Thus our results suggest that CES1 exerts an antiproliferative effect in liver cancer cells and that the single N-linked glycosylation at Asn79 plays a potential regulatory role. These functions may underlie the undetectability of CES1 in human HCC tumors and liver cancer cell lines. Mass spectrometry data are available via ProteomeXchange under the identifier PXD021573.


Assuntos
Carcinoma Hepatocelular , Neoplasias Hepáticas , Hidrolases de Éster Carboxílico/genética , Hidrolases de Éster Carboxílico/metabolismo , Carcinoma Hepatocelular/genética , Linhagem Celular Tumoral , Proliferação de Células , Regulação Neoplásica da Expressão Gênica , Glicosilação , Humanos , Neoplasias Hepáticas/genética
4.
Nanotechnology ; 30(33): 335402, 2019 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-31026842

RESUMO

Piezoelectric materials convert external mechanical force into electrical energy, due to the breaking of the centrosymmetry of the atomic structure. Piezoelectricity-based nano-generators (PNGs) based on two-dimensional transition metal dichalcogenides (TMDs) can generate electrical energy stably by the piezoelectric effect at their nanoscale thickness. However, the commercialization of TMD-based PNGs is limited by their poor piezoelectric performance and microscale energy harvesting. Here, we present the first centimeter-scale PNGs based on molybdenum disulfide (MoS2) nanosheets with vertically grown hollow MoS2 nanoflakes (v-MoS2 NFs) obtained by chemical vapor deposition for energy harvesting from human motions. The collision of v-MoS2 NFs with a preferred odd-atomic-layer number and their 2H antiparallel phase leads to efficient electrical energy generation during the bending movement. Further, basal MoS2 films with v-MoS2 NFs are transferred onto flexible substrates via conventional polymer-assisted methods for the fabrication of attachable and wearable piezoelectric power generators.

5.
J Proteome Res ; 16(12): 4455-4467, 2017 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-28960081

RESUMO

One of the major goals of the Chromosome-Centric Human Proteome Project (C-HPP) is to fill the knowledge gaps between human genomic information and the corresponding proteomic information. These gaps are due to "missing" proteins (MPs)-predicted proteins with insufficient evidence from mass spectrometry (MS), biochemical, structural, or antibody analyses-that currently account for 2579 of the 19587 predicted human proteins (neXtProt, 2017-01). We address some of the lessons learned from the inconsistent annotations of missing proteins in databases (DB) and demonstrate a systematic proteogenomic approach designed to explore a potential new function of a known protein. To illustrate a cautious and strategic approach for characterization of novel function in vitro and in vivo, we present the case of Na(+)/H(+) exchange regulatory cofactor 1 (NHERF1/SLC9A3R1, located at chromosome 17q25.1; hereafter NHERF1), which was mistakenly labeled as an MP in one DB (Global Proteome Machine Database; GPMDB, 2011-09 release) but was well known in another public DB and in the literature. As a first step, NHERF1 was determined by MS and immunoblotting for its molecular identity. We next investigated the potential new function of NHERF1 by carrying out the quantitative MS profiling of placental trophoblasts (PXD004723) and functional study of cytotrophoblast JEG-3 cells. We found that NHERF1 was associated with trophoblast differentiation and motility. To validate this newly found cellular function of NHERF1, we used the Caenorhabditis elegans mutant of nrfl-1 (a nematode ortholog of NHERF1), which exhibits a protruding vulva (Pvl) and egg-laying-defective phenotype, and performed genetic complementation work. The nrfl-1 mutant was almost fully rescued by the transfection of the recombinant transgenic construct that contained human NHERF1. These results suggest that NHERF1 could have a previously unknown function in pregnancy and in the development of human embryos. Our study outlines a stepwise experimental platform to explore new functions of ambiguously denoted candidate proteins and scrutinizes the mandated DB search for the selection of MPs to study in the future.


Assuntos
Fosfoproteínas/fisiologia , Proteogenômica/métodos , Trocadores de Sódio-Hidrogênio/fisiologia , Animais , Caenorhabditis elegans/genética , Diferenciação Celular , Movimento Celular , Bases de Dados de Proteínas , Feminino , Humanos , Immunoblotting , Espectrometria de Massas , Reprodução , Transgenes , Trofoblastos/citologia
6.
J Proteome Res ; 15(11): 4116-4125, 2016 11 04.
Artigo em Inglês | MEDLINE | ID: mdl-27573070

RESUMO

Glycoproteins influence numerous indispensable biological functions, and changes in protein glycosylation have been observed in various diseases. The identification and characterization of glycoprotein and glycosylation sites by mass spectrometry (MS) remain challenging tasks, and great efforts have been devoted to the development of proteome informatics tools that facilitate the MS analysis of glycans and glycopeptides. Here we report on the development of gFinder, a web-based bioinformatics tool that analyzes mixtures of native N-glycopeptides that have been profiled by tandem MS. gFinder not only enables the simultaneous integration of collision-induced dissociation (CID) and high-energy collisional dissociation (HCD) fragmentation but also merges the spectra for high-throughput analysis. These merged spectra expedite the identification of both glycans and N-glycopeptide backbones in tandem MS data using the glycan database and a proteomic search tool (e.g., Mascot). These data can be used to simultaneously characterize peptide backbone sequences and possible N-glycan structures using assigned scores. gFinder also provides many convenient functions that make it easy to perform manual calculations while viewing the spectrum on-screen. We used gFinder to detect an additional protein (Q8N9B8) that was missed from the previously published data set containing N-linked glycosylation. For N-glycan analysis, we used the GlycomeDB glycan structure database, which integrates the structural and taxonomic data from all of the major carbohydrate databases available in the public domain. Thus, gFinder is a convenient, high-throughput analytical tool for interpreting the tandem mass spectra of N-glycopeptides, which can then be used for identification of potential missing proteins having glycans. gFinder is available publicly at http://gFinder.proteomix.org/ .


Assuntos
Biologia Computacional/métodos , Glicopeptídeos/análise , Internet , Software , Animais , Humanos , Polissacarídeos/análise , Proteômica , Espectrometria de Massas em Tandem
7.
J Proteome Res ; 15(12): 4146-4164, 2016 12 02.
Artigo em Inglês | MEDLINE | ID: mdl-27760464

RESUMO

Glycoprotein conformations are complex and heterogeneous. Currently, site-specific characterization of glycopeptides is a challenge. We sought to establish an efficient method of N-glycoprotein characterization using mass spectrometry (MS). Using alpha-1-acid glycoprotein (AGP) as a model N-glycoprotein, we identified its tryptic N-glycopeptides and examined the data reproducibility in seven laboratories running different LC-MS/MS platforms. We used three test samples and one blind sample to evaluate instrument performance with entire sample preparation workflow. 165 site-specific N-glycopeptides representative of all N-glycosylation sites were identified from AGP 1 and AGP 2 isoforms. The glycopeptide fragmentations by collision-induced dissociation or higher-energy collisional dissociation (HCD) varied based on the MS analyzer. Orbitrap Elite identified the greatest number of AGP N-glycopeptides, followed by Triple TOF and Q-Exactive Plus. Reproducible generation of oxonium ions, glycan-cleaved glycopeptide fragment ions, and peptide backbone fragment ions was essential for successful identification. Laboratory proficiency affected the number of identified N-glycopeptides. The relative quantities of the 10 major N-glycopeptide isoforms of AGP detected in four laboratories were compared to assess reproducibility. Quantitative analysis showed that the coefficient of variation was <25% for all test samples. Our analytical protocol yielded identification and quantification of site-specific N-glycopeptide isoforms of AGP from control and disease plasma sample.


Assuntos
Glicopeptídeos/química , Orosomucoide/química , Isoformas de Proteínas/análise , Sítios de Ligação , Coleta de Amostras Sanguíneas , Cromatografia Líquida , Glicosilação , Humanos , Reprodutibilidade dos Testes , Espectrometria de Massas em Tandem
8.
Opt Express ; 24(10): A846-55, 2016 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-27409957

RESUMO

We herein report an investigation of the device performance capabilities and impedance characteristics of solution-processed organic light-emitting devices (OLEDs) with all-water-processable triple-stacked hole-selective layers (HSLs) on an indium-tin-oxide (ITO) anode, fabricated using a simple coating technique. Highly smooth and homogeneous triple-stacked layers were deposited via horizontal-dip- (H-dip-) coating using aqueous dispersions of graphene oxide (GO), molybdenum oxide (MoO3), and poly(ethylenedioxy thiophene):poly(styrene sulfonate) ( PEDOT: PSS). From the triple-stacked GO/MoO3/ PEDOT: PSS HSLs used as hole-injection layers (HILs) in the OLEDs, which outperform a conventional single HIL of PEDOT: PSS, it was found that OLEDs with triple-stacked HILs exhibited characteristic impedance properties, including low parallel resistance with trap-free space-charge-limited conductivity. Furthermore, it was shown that the relaxation frequency of a sample OLED with triple-stacked GO/MoO3/ PEDOT: PSS HILs was much higher than that of a reference device with a single PEDOT: PSS HIL. These impedance behaviors indicate that carrier (hole) injection in the sample OLED is more efficient than that in any of the other devices tested here. The results presented here clarify that the triple-stacked GO/MoO3/ PEDOT: PSS layers can act as efficient HILs on an ITO anode, representing a remarkable advance in relation to the mass production of high-performance solution-processable OLEDs.

9.
Nanotechnology ; 27(7): 075709, 2016 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-26789982

RESUMO

Graphene-organic hybrid thin films are promising candidates for use as advanced transparent electrodes and high-performance photodetectors. In this work, we fabricated hybrid thin film structures consisting of graphene and either tetraphenyl-porphyrin (H2TPP) or metalloporphyrins such as aluminum (III) tetraphenyl-porphyrin (Al(III)TPP) and zinc tetraphenyl-porphyrin (ZnTPP). The optical and electrical characteristics of ultrathin photodetectors based on the graphene-organic hybrid layers were subsequently evaluated. A hybrid deposition system capable of both thermal evaporation and vapor phase metalation was employed to synthesize the tunable metalloporphyrin-based thin films. As a proof of concept, we successfully fabricated various graphene-based photodetectors via the simple and efficient vapor-phase metalation of porphyrin. This work may facilitate the development of new architectures for flexible graphene-organic devices.

10.
J Proteome Res ; 14(8): 3007-14, 2015 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-26148796

RESUMO

Solid-pseudopapillary neoplasm (SPN) is an uncommon pancreatic tumor with mutation in CTNNB1 and distinct clinical and pathological features. We compared the proteomic profiles of SPN to mRNA expression. Pooled SPNs and pooled non-neoplastic pancreatic tissues were examined with high-resolution mass spectrometry. We identified 329 (150 up-regulated and 179 down-regulated) differentially expressed proteins in SPN. We identified 191 proteins (58.1% of the 329 dysregulated proteins) with the same expression tendencies in SPN based on mRNA data. Many overexpressed proteins were related to signaling pathways known to be activated in SPNs. We found that several proteins involved in Wnt signaling, including DKK4 and ß-catenin, and proteins that bind ß-catenin, such as FUS and NONO, were up-regulated in SPNs. Molecules involved in glycolysis, including PKM2, ENO2, and HK1, were overexpressed in accordance to their mRNA levels. In summary, SPN showed (1) distinct protein expression changes that correlated with mRNA expression, (2) overexpression of Wnt signaling proteins and proteins that bind directly to ß-catenin, and (3) overexpression of proteins involved in metabolism. These findings may help develop early diagnostic biomarkers and molecular targets.


Assuntos
Carcinoma Papilar/metabolismo , Neoplasias Pancreáticas/metabolismo , Proteoma/metabolismo , Proteômica/métodos , Adulto , Biomarcadores Tumorais/genética , Biomarcadores Tumorais/metabolismo , Western Blotting , Carcinoma Papilar/genética , Cromatografia Líquida , Feminino , Perfilação da Expressão Gênica/métodos , Regulação Neoplásica da Expressão Gênica , Humanos , Peptídeos e Proteínas de Sinalização Intercelular/genética , Peptídeos e Proteínas de Sinalização Intercelular/metabolismo , Masculino , Pessoa de Meia-Idade , Neoplasias Pancreáticas/genética , Proteoma/genética , Reação em Cadeia da Polimerase Via Transcriptase Reversa , Espectrometria de Massas em Tandem , Via de Sinalização Wnt/genética , beta Catenina/genética , beta Catenina/metabolismo
11.
J Proteome Res ; 13(5): 2328-38, 2014 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-24628331

RESUMO

Aberrant structures of site-specific N-linked glycans are closely associated with the tumorigenesis of hepatocellular carcinoma (HCC), one of the most common fatal cancers worldwide. Vitronectin (VTN) is considered a candidate glycobiomarker of HCC. In this study, we describe a reliable and simple quantification strategy based on abundance ratios of site-specific N-linked glycopeptides of VTN to screen for potential biomarkers. A total of 14 unique N-linked glycans corresponding to 27 unique N-linked glycopeptides were characterized at three N-linked sites (Asn-86, -169, and -242) present in VTN. These glycans could be good candidate markers for HCC. Among these glycans, the abundance ratio of two representative glycoforms (fucosyl vs non-fucosyl) was significantly increased in HCC plasma relative to normal plasma. This strategy was also successfully applied to another potential HCC biomarker, haptoglobin. Furthermore, we demonstrate that our approach employing tandem mass tag (TMT) and target N-linked glycopeptides of VTN is a useful tool for quantifying specific glycans in HCC plasma relative to normal plasma. Our strategy represents a simple and potentially useful screening platform for the discovery of cancer-specific glycobiomarkers.


Assuntos
Carcinoma Hepatocelular/metabolismo , Glicopeptídeos/metabolismo , Neoplasias Hepáticas/metabolismo , Polissacarídeos/metabolismo , Adulto , Idoso , Sequência de Aminoácidos , Sítios de Ligação , Biomarcadores Tumorais/sangue , Biomarcadores Tumorais/metabolismo , Carcinoma Hepatocelular/sangue , Carcinoma Hepatocelular/patologia , Cromatografia Líquida , Glicômica/métodos , Glicopeptídeos/sangue , Glicopeptídeos/química , Humanos , Neoplasias Hepáticas/sangue , Neoplasias Hepáticas/patologia , Masculino , Pessoa de Meia-Idade , Dados de Sequência Molecular , Estadiamento de Neoplasias , Polissacarídeos/sangue , Proteômica/métodos , Reprodutibilidade dos Testes , Espectrometria de Massas em Tandem , Vitronectina/sangue , Vitronectina/metabolismo
12.
J Proteome Res ; 13(11): 4878-88, 2014 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-25057901

RESUMO

Pancreatic cancer (PC; pancreatic ductal adenocarcinoma) is characterized by significant morbidity and mortality worldwide. Although carbohydrate antigen (CA) 19-9 has been known as a PC biomarker, it is not commonly used for general screening because of its low sensitivity and specificity. Therefore, there is an urgent need to develop a new biomarker for PC diagnosis in the earlier stage of cancer. To search for a novel serologic PC biomarker, we carried out an integrated proteomic analysis for a total of 185 pooled or individual plasma from healthy donors and patients with five disease groups including chronic pancreatitis (CP), PC, and other cancers (e.g., hepatocellular carcinoma, cholangiocarcinoma, and gastric cancer) and identified complement factor b (CFB) as a candidate serologic biomarker for PC diagnosis. Immunoblot analysis of CFB revealed more than two times higher expression in plasma samples from PC patients compared with plasma from individuals without PC. Immunoprecipitation coupled to mass spectrometry analysis confirmed both molecular identity and higher expression of CFB in PC samples. CFB showed distinctly higher specificity than CA 19-9 for PC against other types of digestive cancers and in discriminating PC patients from non-PC patients (p < 0.0001). In receiver operator characteristic curve analysis, CFB showed an area under curve of 0.958 (95% CI: 0.956 to 0.959) compared with 0.833 (95% CI: 0.829 to 0.837) for CA 19-9. Furthermore, the Y-index of CFB was much higher than that of CA 19-9 (71.0 vs 50.4), suggesting that CFB outperforms CA 19-9 in discriminating PC from CP and other gastrointestinal cancers. This was further supported by immunoprecipitation and qRT-PCR assays showing higher expression of CFB in PC cell lines than in normal cell lines. A combination of CFB and CA 19-9 showed markedly improved sensitivity (90.1 vs 73.1%) over that of CFB alone in the diagnosis of PC against non-PC, with similar specificity (97.2 vs 97.9%). Thus, our results identify CFB as a novel serologic PC biomarker candidate and warrant further investigation into a large-scale validation and its role in molecular mechanism of pancreatic carcinogenesis.


Assuntos
Biomarcadores Tumorais/sangue , Carcinoma Ductal Pancreático/diagnóstico , Fator B do Complemento , Neoplasias Pancreáticas/diagnóstico , Proteômica/métodos , Área Sob a Curva , Western Blotting , Carcinoma Ductal Pancreático/sangue , Linhagem Celular Tumoral , Fator B do Complemento/metabolismo , Primers do DNA/genética , Eletroforese em Gel Bidimensional , Ensaio de Imunoadsorção Enzimática , Humanos , Processamento de Imagem Assistida por Computador , Imunoprecipitação , Neoplasias Pancreáticas/sangue , Reação em Cadeia da Polimerase em Tempo Real , Estatísticas não Paramétricas , Espectrometria de Massas em Tandem , Tripsina
13.
Nanotechnology ; 25(28): 285302, 2014 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-24971722

RESUMO

There has been considerable interest in soft lithographic patterning processing of large scale graphene sheets due to the low cost and simplicity of the patterning process along with the exceptional electrical or physical properties of graphene. These properties include an extremely high carrier mobility and excellent mechanical strength. Recently, a study has reported that single layer graphene grown via chemical vapor deposition (CVD) was patterned and transferred to a target surface by controlling the surface energy of the polydimethylsiloxane (PDMS) stamp. However, applications are limited because of the challenge of CVD-graphene functionalization for devices such as chemical or bio-sensors. In addition, graphene-based layers patterned with a micron scale width on the surface of biocompatible silk fibroin thin films, which are not suitable for conventional CMOS processes such as the patterning or etching of substrates, have yet to be reported. Herein, we developed a soft lithographic patterning process via surface energy modification for advanced graphene-based flexible devices such as transistors or chemical sensors. Using this approach, the surface of a relief-patterned elastomeric stamp was functionalized with hydrophilic dimethylsulfoxide molecules to enhance the surface energy of the stamp and to remove the graphene-based layer from the initial substrate and transfer it to a target surface. As a proof of concept using this soft lithographic patterning technique, we demonstrated a simple and efficient chemical sensor consisting of reduced graphene oxide and a metallic nanoparticle composite. A flexible graphene-based device on a biocompatible silk fibroin substrate, which is attachable to an arbitrary target surface, was also successfully fabricated. Briefly, a soft lithographic patterning process via surface energy modification was developed for advanced graphene-based flexible devices such as transistors or chemical sensors and attachable devices on a biocompatible silk fibroin substrate. Significantly, this soft lithographic patterning technique enables us to demonstrate a simple and efficient chemical sensor based on reduced graphene oxide (rGO), a metallic nanoparticle composite, and an attachable graphene-based device on a silk fibroin thin film.


Assuntos
Grafite/química , Técnicas Biossensoriais/métodos , Dimetilpolisiloxanos/química , Fibroínas/química , Nanopartículas Metálicas/química , Nanotecnologia/métodos , Óxidos/química , Seda/química , Propriedades de Superfície
14.
ACS Appl Mater Interfaces ; 16(22): 28808-28817, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38775279

RESUMO

This paper reports chemiresistive multiarray gas sensors through the synthesized ternary nanocomposites, using a one-pot method to integrate two-dimensional MXene (Ti3C2Tx) with Ti-doped WO3 (Ti-WO3/Ti3C2Tx) and Ti3C2Tx with Pd-doped SnO2 (Pd-SnO2/Ti3C2Tx). The gas sensors based on Ti-WO3/Ti3C2Tx and Pd-SnO2/Ti3C2Tx exhibit exceptional sensitivity, particularly in detecting 70% at 1 ppm acetone and 91.1% at 1 ppm of H2S. Notably, our sensors demonstrate a remarkable sensing performance in the low-ppb range for acetone and H2S. Specifically, the Ti-WO3/Ti3C2Tx sensor demonstrates a detection limit of 0.035 ppb for acetone, and the Pd-SnO2/Ti3C2Tx sensor shows 0.116 ppb for H2S. Simultaneous measurements with Ti-WO3/Ti3C2Tx- and Pd-SnO2/Ti3C2Tx-based sensors enable the evaluation of both the concentration and type of unknown target gases, such as acetone or H2S. Furthermore, density functional theory calculations are performed to clarify the role of Ti and Pd doping in enhancing the performance of Ti-WO3/Ti3C2Tx and Pd-SnO2/Ti3C2Tx nanocomposites. Theoretical simulations contribute to a deeper understanding of the doping effects, providing essential insights into the mechanisms underlying the enhanced gas response of the gas sensors. Overall, this work provides valuable insights into the gas-sensing mechanisms and introduces a novel approach for high-performance multiarray gas sensing.

15.
ACS Omega ; 9(26): 28707-28714, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38973851

RESUMO

This study describes the synthesis of germanium and tin complexes Ge(mdpaS)2 (1), Ge(edpaS)2 (2), Ge(bdpaS)2 (3), Ge(empaS)2 (4), Sn(mdpaS)2 (5), Sn(edpaS)2 (6), Sn(bdpaS)2 (7), and Sn(empaS)2 (8) (mdpaSH = (Z)-N-methoxy-2,2-dimethylpropanimidothioic acid; edpaSH = (Z)-N-ethoxy-2,2-dimethylpropanimidothioic acid; bdpaSH = (Z)-N-(tert-butoxy)-2,2-dimethylpropanimidothioic acid; empaSH = (Z)-N-ethoxy-2-methylpropanimidothioic acid), using newly designed N-alkoxy thioamide ligands as precursors for metal chalcogenide materials. All complexes were characterized using various analytical techniques, and the single-crystal structures of complexes 5 and 7 revealed a distorted seesaw geometry in the monomeric SnL2 form. Thermogravimetric (TG) curves showed differences between Ge compounds, which exhibited single-step weight losses, and Sn compounds, which exhibited multistep weight losses. As a result, we suggest that the synthesized complexes 1-8 are potential precursors for group IV metal chalcogenide materials.

16.
Adv Sci (Weinh) ; 11(23): e2308976, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38582529

RESUMO

Portable and personalized artificial intelligence (AI)-driven sensors mimicking human olfactory and gustatory systems have immense potential for the large-scale deployment and autonomous monitoring systems of Internet of Things (IoT) devices. In this study, an artificial Q-grader comprising surface-engineered zinc oxide (ZnO) thin films is developed as the artificial nose, tongue, and AI-based statistical data analysis as the artificial brain for identifying both aroma and flavor chemicals in coffee beans. A poly(vinylidene fluoride-co-hexafluoropropylene)/ZnO thin film transistor (TFT)-based liquid sensor is the artificial tongue, and an Au, Ag, or Pd nanoparticles/ZnO nanohybrid gas sensor is the artificial nose. In order to classify the flavor of coffee beans (acetic acid (sourness), ethyl butyrate and 2-furanmethanol (sweetness), caffeine (bitterness)) and the origin of coffee beans (Papua New Guinea, Brazil, Ethiopia, and Colombia-decaffeine), rational combination of TFT transfer and dynamic response curves capture the liquids and gases-dependent electrical transport behavior and principal component analysis (PCA)-assisted machine learning (ML) is implemented. A PCA-assisted ML model distinguished the four target flavors with >92% prediction accuracy. ML-based regression model predicts the flavor chemical concentrations with >99% accuracy. Also, the classification model successfully distinguished four different types of coffee-bean with 100% accuracy.


Assuntos
Nariz Eletrônico , Aprendizado de Máquina , Humanos , Inteligência Artificial , Paladar/fisiologia , Café/química , Odorantes/análise , Olfato/fisiologia , Língua/fisiologia , Óxido de Zinco/química , Análise de Componente Principal
17.
ACS Appl Mater Interfaces ; 16(23): 30264-30273, 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38832451

RESUMO

Despite the advancement of the Internet of Things (IoT) and portable devices, the development of zero-biased sensing systems for the dual detection of light and gases remains a challenge. As an emerging technology, direct energy conversion driven by intriguing physical properties of two-dimensional (2D) materials can be realized in nanodevices or a zero-biased integrated system. In this study, we unprecedentedly attempted to exploit the photostimulated pyrothermoelectric coupling of two-dimensional SnSe for use in zero-biased multimodal transducers for the dual detection of light and gases. We synthesized homogeneous, large-area 6 in SnSe multilayers via a rational synthetic route based on the thermal decomposition of a solution-processed single-source precursor. Zero-biased SnSe transducers for the dual monitoring of light and gases were realized by exploiting the synergistic coupling of the photostimulated pyroelectric and thermoelectric effects of SnSe. The extracted photoresponsivity at 532 nm and NO2 gas responsivity of the SnSe-based transducers corresponded to 1.07 × 10-6 A/W and 13263.6% at 0 V, respectively. To bring universal applicability of the zero-biased SnSe transducers, the wide operation bandwidth photoelectrical properties (visible to NIR) and dynamic current responses toward two NO2/NH3 gases were systematically evaluated.

18.
J Proteome Res ; 12(6): 2458-66, 2013 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-23362793

RESUMO

As a starting point of the Chromosome-Centric Human Proteome Project (C-HPP), we established strategies of genome-wide proteomic analysis, including protein identification, quantitation of disease-specific proteins, and assessment of post-translational modifications, using paired human placental tissues from healthy and preeclampsia patients. This analysis resulted in identification of 4239 unique proteins with high confidence (two or more unique peptides with a false discovery rate less than 1%), covering 21% of approximately 20, 059 (Ensembl v69, Oct 2012) human proteins, among which 28 proteins exhibited differentially expressed preeclampsia-specific proteins. When these proteins are assigned to all human chromosomes, the pattern of the newly identified placental protein population is proportional to that of the gene count distribution of each chromosome. We also identified 219 unique N-linked glycopeptides, 592 unique phosphopeptides, and 66 chromosome 13-specific proteins. In particular, protein evidence of 14 genes previously known to be specifically up-regulated in human placenta was verified by mass spectrometry. With respect to the functional implication of these proteins, 38 proteins were found to be involved in regulatory factor biosynthesis or the immune system in the placenta, but the molecular mechanism of these proteins during pregnancy warrants further investigation. As far as we know, this work produced the highest number of proteins identified in the placenta and will be useful for annotating and mapping all proteins encoded in the human genome.


Assuntos
Cromossomos Humanos/química , Estudo de Associação Genômica Ampla , Pré-Eclâmpsia/metabolismo , Processamento de Proteína Pós-Traducional , Proteoma/isolamento & purificação , Estudos de Casos e Controles , Feminino , Perfilação da Expressão Gênica , Regulação da Expressão Gênica , Genoma Humano , Glicosilação , Projeto Genoma Humano , Humanos , Espectrometria de Massas , Fosforilação , Placenta , Pré-Eclâmpsia/genética , Gravidez , Proteoma/genética , Proteoma/metabolismo
19.
ACS Omega ; 8(22): 19816-19821, 2023 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-37305263

RESUMO

To substitute corrosive halogen ligands, we designed and synthesized novel tungsten complexes containing amido ligands, W(DMEDA)3 (1) and W(DEEDA)3 (2) (DMEDA = N,N'-dimethylethylenediamido; DEEDA = N,N'-diethylethylenediamido). Complexes 1 and 2 were characterized by 1H NMR, 13C NMR, FT-IR, and elemental analysis. The pseudo-octahedral molecular structure of 1 was confirmed by single-crystal X-ray crystallography. The thermal properties of 1 and 2 were analyzed by thermogravimetric analysis (TGA), which confirmed that the precursors were volatile and exhibited adequate thermal stability. Additionally, the WS2 deposition test was performed using 1 in thermal chemical vapor deposition (thermal CVD). Further analysis of the surface of the thin films was conducted using Raman spectroscopy, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS).

20.
RSC Adv ; 13(19): 13128-13133, 2023 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-37124004

RESUMO

The rising importance of gas detection has prompted rigorous research on flexible and transparent high-performance gas sensors. We demonstrated a sensor for NO2 detection at room temperature, in which our device was fabricated via screen printing on a flexible substrate, and MoS2 and single-walled carbon nanotube (SWCNT) were coated on a specific area by the self-assembly method. This fabrication process is rapid, facile, and cost-effective. The proposed sensor enables precise and stable NO2 gas sensing from 50 ppb to 100 ppm. This method should also be applicable to the selective detection of other gases.

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