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3.
ACS Appl Mater Interfaces ; 14(34): 38905-38920, 2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-35973160

RESUMO

Designing new materials for selective Fischer-Tropsch synthesis (FTS) is an elegant way to enhance local feedstock utilization like biomass and waste. In this approach, we have designed a thermally and chemically stable bimetallic PtCo/NC hybrid nanocomposite catalyst derived from a zeolitic imidazolate framework (ZIF-67, which contains cobalt as a metal center) through carbonization for low-temperature (413-473 K) aqueous-phase Fischer-Tropsch synthesis (AFTS). The selectivity of the desired range of hydrocarbons is adjusted using a highly dispersed PtCo bimetallic alloy, which facilitates extraordinary reduction of a metal oxide to active species by the synergic effect under the AFTS reaction conditions. The ZIF-derived catalyst tested in this study exhibited the highest activity to date for very low temperatures (433 K) in aqueous-phase Fischer-Tropsch synthesis with CO conversion rates between 0.61 and 1.20 molCO·molCo-1·h-1. Insights of the remarkable catalyst activity were examined by in situ X-ray photoelectron spectroscopy (XPS) studies corroborated by density functional theory (DFT) calculation. The bimetallic Co3Pt (111) surface was found to be highly active for the C-C coupling reaction between surface-adsorbed C and CO, forming a CCO intermediate with a very low activation barrier (Ea = 0.37 eV), in comparison to the C-C coupling activation barrier obtained over the Co (111) surface (Ea = 0.87 eV). This unique approach and observations create a new path for developing next-generation advanced catalyst systems and processes for selective low-temperature FTS.

4.
Polymers (Basel) ; 14(21)2022 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-36365679

RESUMO

Solid-state NMR is a nondestructive and noninvasive technique used to study the chemical structure and dynamics of starch-based materials and to bridge the gap between structure-function relationships and industrial applications. The study of crystallinity, chemical modification, product blending, molecular packing, amylose-amylopectin ratio, end chain motion, and solvent-matrix interactions is essential for tailoring starch product properties to various applications. This article aims to provide a comprehensive and critical review of research characterizing starch-based materials using solid-state NMR, and to briefly introduce the most advanced and promising NMR strategies and hardware designs used to overcome the sensitivity and resolution issues involved in structure-function relationships.

5.
Mol Microbiol ; 69(5): 1153-64, 2008 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-18573179

RESUMO

Low Molecular Weight Tyrosine Phosphatases (LMWTP) are widespread in prokaryotes; however, understanding of the signalling cascades controlled by these enzymes is still emerging. Porphyromonas gingivalis, an opportunistic oral pathogen, expresses a LMWTP, Ltp1, that is differentially regulated in biofilm communities. Here we characterize the enzymatic activity of Ltp1 and, through the use of mutants that lack Ltp1 or expresses catalytically defective Ltp1, show that tyrosine phosphatase activity constrains both monospecies biofilm development and community development with the antecedent oral biofilm constituent Streptococcus gordonii. Exopolysaccharide production is downregulated by Ltp1 through transcriptional regulation of multiple genes involved in biosynthesis and transport. Furthermore, Ltp1 regulates transcriptional activity of luxS and thus impacts AI-2-dependent signalling in biofilm communities. In the absence of Ltp1 transcription across the hmu haemin uptake locus is reduced, and consequently uptake of haemin is impaired in the Ltp1 mutant. The gingipain proteinases Kgp and RgpA/B remain phosphorylated in the Ltp1 mutant. Phosphorylated Rgps are poorly secreted, whereas cell surface activity of phosphorylated Kgp is enhanced. By controlling the activity of several virulence-associated properties, Ltp1 may restrain the pathogenic potential of P. gingivalis and maintain a commensal interaction with the host.


Assuntos
Proteínas de Bactérias/metabolismo , Infecções por Bacteroidaceae/microbiologia , Regulação Bacteriana da Expressão Gênica , Doenças Periodontais/microbiologia , Porphyromonas gingivalis/enzimologia , Porphyromonas gingivalis/patogenicidade , Proteínas Tirosina Fosfatases/metabolismo , Proteínas de Bactérias/química , Proteínas de Bactérias/genética , Biofilmes/crescimento & desenvolvimento , Liases de Carbono-Enxofre/genética , Liases de Carbono-Enxofre/metabolismo , Heme/metabolismo , Humanos , Peptídeo Hidrolases/genética , Peptídeo Hidrolases/metabolismo , Polissacarídeos Bacterianos/genética , Polissacarídeos Bacterianos/metabolismo , Porphyromonas gingivalis/genética , Porphyromonas gingivalis/fisiologia , Proteínas Tirosina Fosfatases/química , Proteínas Tirosina Fosfatases/genética , Streptococcus gordonii/genética , Streptococcus gordonii/fisiologia , Especificidade por Substrato , Virulência , Fatores de Virulência/genética , Fatores de Virulência/metabolismo
6.
Infect Immun ; 74(11): 6419-28, 2006 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-16923784

RESUMO

Porphyromonas gingivalis, one of the causative agents of adult periodontitis, develops biofilm microcolonies on substrata of Streptococcus gordonii but not on Streptococcus mutans. P. gingivalis genome microarrays were used to identify genes differentially regulated during accretion of P. gingivalis in heterotypic biofilms with S. gordonii. Thirty-three genes showed up- or downregulation by array analysis, and differential expression was confirmed by quantitative reverse transcription-PCR. The functions of the regulated genes were predominantly related to metabolism and energy production. In addition, many of the genes have no current known function. The roles of two upregulated genes, ftsH (PG0047) encoding an ATP-dependent zinc metallopeptidase and ptpA (PG1641) encoding a putative tyrosine phosphatase, were investigated further by mutational analysis. Strains with mutations in these genes developed more abundant biofilms with S. gordonii than the parental strain developed. ftsH and ptpA may thus participate in a regulatory network that constrains P. gingivalis accumulation in heterotypic biofilms. This study provided a global analysis of P. gingivalis transcriptional responses in an oral microbial community and also provided insight into the regulation of heterotypic biofilm development.


Assuntos
Regulação Bacteriana da Expressão Gênica , Porphyromonas gingivalis/genética , Streptococcus/genética , Proteases Dependentes de ATP/genética , Proteases Dependentes de ATP/metabolismo , Biofilmes/crescimento & desenvolvimento , Perfilação da Expressão Gênica , Regulação Bacteriana da Expressão Gênica/imunologia , Genoma Bacteriano , Fosfoproteínas Fosfatases/genética , Fosfoproteínas Fosfatases/metabolismo , Porphyromonas gingivalis/enzimologia , Porphyromonas gingivalis/fisiologia , RNA Mensageiro/metabolismo , Streptococcus/enzimologia , Streptococcus/fisiologia , Transcrição Gênica/imunologia
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