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1.
ChemSusChem ; 16(24): e202300930, 2023 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-37589250

RESUMO

Alternative to current liquid amine technologies for post-combustion CO2 capture, new technologies such as adsorbent-based processes are developed, wherein material lifetime and degradation is important. Herein a robust method to determine degradation rates in a laboratory setup is developed, which was validated with a continuous multi-staged fluidized bed pilot plant designed to capture 1 ton CO2 per day. An amine functionalized polystyrene adsorbent showed very good agreement between the experimental 1000-hour laboratory degradation rates and 2200 hours of degradation in a pilot plant. This validates how laboratory experiments can be extrapolated for sorbent screening and for scale-up. Resulting, the oxidative degradation in the desorber at high temperatures (120 °C) and low O2 concentrations (150 ppmv) is 3 times higher compared to the adsorber at low temperatures and high O2 (56 °C, 7 vol %). Laboratory degradation experiments can hence be used to further optimize process operations to limit degradation or screen for potential new adsorbents.

2.
Bioelectrochemistry ; 148: 108254, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36122427

RESUMO

A novel membraneless ß-glucan/O2 enzymatic fuel cell was developed by combining a bioanode based on buckypaper modified with co-immobilized Agaricus meleagris pyranose dehydrogenase (AmPDH) and Rhodothermus marinus ß-glucosidase (RmBgl3B) (RmBgl3B-AmPDH/buckypaper) with a biocathode based on solid graphite modified with Myrothecium verrucaria bilirubin oxidase (MvBOx/graphite). AmPDH was connected electrochemically with the buckypaper using an osmium redox polymer in a mediated reaction, whereas MvBOx was connected with graphite in a direct electron transfer reaction. The fuel for the bioanode was produced by enzymatic hydrolysis of ß-glucan by the exoglucanase RmBgl3B into d-glucose, which in turn was enzymatically oxidised by AmPDH to generate a current response. This design allows to obtain an efficient enzymatic fuel cell, where the chemical energy converted into electrical energy is higher than the chemical energy stored in complex carbohydrate based fuel. The maximum power density of the assembled ß-glucan/O2 biofuel cell reached 26.3 ±â€¯4.6 µWcm-2 at 0.36 V in phosphate buffer containing 0.5 % (w/v) ß-glucan at 40 °C with excellent stability retaining 68.6 % of its initial performance after 5 days. The result confirms that ß-glucan can be employed as fuel in an enzymatic biofuel cell.


Assuntos
Fontes de Energia Bioelétrica , Grafite , beta-Glucanas , Agaricales , Eletrodos , Enzimas Imobilizadas , Glucose , Osmio , Fosfatos , Polímeros , Rhodothermus , beta-Glucosidase
3.
Curr Opin Biotechnol ; 73: 179-187, 2022 02.
Artigo em Inglês | MEDLINE | ID: mdl-34481244

RESUMO

Supercapacitive biofuel cells' (SBFCs) most recent advancements are herein disclosed. In conventional SBFCs the biocomponent is employed as the pseudocapacitive component, while in self-charging biodevices it also works as the biocatalyst. The performance of different types of SBFCs are summarized according to the categorization based on the biocatalyst employed: supercapacitive microbial fuel cells (s-MFCs), supercapacitive biophotovoltaics (SBPV) and supercapacitive enzymatic fuel cells (s-EFCs). SBFCs could be considered as promising 'alternative' energy devices (low-cost, environmentally friendly, and technically undemanding electric power sources etc.) being suitable for powering a new generation of miniaturized electronic applications.


Assuntos
Fontes de Energia Bioelétrica , Eletrodos
4.
J Bacteriol ; 202(7)2020 03 11.
Artigo em Inglês | MEDLINE | ID: mdl-31932308

RESUMO

Enterococcus faecalis cells are known to have ferric reductase activity and the ability to transfer electrons generated in metabolism to the external environment. We have isolated mutants defective in ferric reductase activity and studied their electron transfer properties to electrodes mediated by ferric ions and an osmium complex-modified redox polymer (OsRP). Electron transfer mediated with ferric ions and ferric reductase activity were both found to be dependent on the membrane-associated Ndh3 and EetA proteins, consistent with findings in Listeria monocytogenes In contrast, electron transfer mediated with OsRP was independent of these two proteins. Quinone in the cell membrane was required for the electron transfer with both mediators. The combined results demonstrate that extracellular electron transfer from reduced quinone to ferric ions and to OsRP occurs via different routes in the cell envelope of E. faecalisIMPORTANCE The transfer of reducing power in the form of electrons, generated in the catabolism of nutrients, from a bacterium to an extracellular acceptor appears to be common in nature. The electron acceptor can be another cell or abiotic material. Such extracellular electron transfer contributes to syntrophic metabolism and is of wide environmental, industrial, and medical importance. Electron transfer between microorganisms and electrodes is fundamental in microbial fuel cells for energy production and for electricity-driven synthesis of chemical compounds in cells. In contrast to the much-studied extracellular electron transfer mediated by cell surface exposed cytochromes, little is known about components and mechanisms for such electron transfer in organisms without these cytochromes and in Gram-positive bacteria such as E. faecalis, which is a commensal gut lactic acid bacterium and opportunistic pathogen.


Assuntos
Transporte de Elétrons , Enterococcus faecalis/fisiologia , Respiração Celular , Parede Celular/metabolismo , Espaço Extracelular/metabolismo , FMN Redutase/metabolismo , Genótipo , Mutação , Oxirredução
5.
Anal Chim Acta ; 1076: 32-47, 2019 Oct 17.
Artigo em Inglês | MEDLINE | ID: mdl-31203962

RESUMO

Electroactive microorganisms possess the unique ability to transfer electrons to or from solid phase electron conductors, e.g., electrodes or minerals, through various physiological mechanisms. The processes are commonly known as extracellular electron transfer and broadly harnessed in microbial electrochemical systems, such as microbial biosensors, microbial electrosynthesis, or microbial fuel cells. Apart from a few model microorganisms, the nature of the microbe-electrode conductive interaction is poorly understood for most of the electroactive species. The interaction determines the efficiency and a potential scaling up of bioelectrochemical systems. Gram-positive bacteria generally have a thick electron non-conductive cell wall and are believed to exhibit weak extracellular electron shuttling activity. This review highlights reported research accomplishments on electroactive Gram-positive bacteria. The use of electron-conducting polymers as mediators is considered as one promising strategy to enhance the electron transfer efficiency up to application scale. In view of the recent progress in understanding the molecular aspects of the extracellular electron transfer mechanisms of Enterococcus faecalis, the electron transfer properties of this bacterium are especially focused on. Fundamental knowledge on the nature of microbial extracellular electron transfer and its possibilities can provide insight in interspecies electron transfer and biogeochemical cycling of elements in nature. Additionally, a comprehensive understanding of cell-electrode interactions may help in overcoming insufficient electron transfer and restricted operational performance of various bioelectrochemical systems and facilitate their practical applications.


Assuntos
Elétrons , Bactérias Gram-Positivas/química , Parede Celular/química , Eletrodos , Hidrogéis/química , Proteínas de Membrana/química , Oxirredução , Polímeros/química
6.
Bioelectrochemistry ; 128: 94-99, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-30959399

RESUMO

We report on a hybrid bioelectrochemical system that integrates an energy converting part, viz. a glucose/oxygen enzymatic fuel cell, with a charge-storing component, in which the redox features of the immobilized redox protein cytochrome c (cyt c) were utilized. Bilirubin oxidase and pyrroloquinoline quinone-dependent glucose dehydrogenase (PQQ-GDH) were employed as the biocatalysts for dioxygen reduction and glucose oxidation, respectively. A bi-protein PQQ-GDH/cyt c signal chain was created that facilitates electron transfer between the enzyme and the electrode surface. The assembled supercapacitor/biofuel cell hybrid biodevice displays a 15 times higher power density tested in the pulse mode compared to the performance achieved from the continuously operating regime (4.5 and 0.3 µW cm-2, respectively) with an 80% residual activity after 50 charge/discharge pulses. This can be considered as a notable step forward in the field of glucose/oxygen membrane-free, biocompatible hybrid power sources.


Assuntos
Fontes de Energia Bioelétrica , Citocromos c/metabolismo , Enzimas Imobilizadas/metabolismo , Glucose Desidrogenase/metabolismo , Oxirredutases atuantes sobre Doadores de Grupo CH-CH/metabolismo , Técnicas Eletroquímicas/instrumentação , Eletrodos , Transporte de Elétrons , Glucose/metabolismo , Oxirredução
7.
Biochemistry ; 57(30): 4597-4603, 2018 07 31.
Artigo em Inglês | MEDLINE | ID: mdl-29989403

RESUMO

Extracellular electron transfer (EET) in microbial cells is essential for certain biotechnological applications and contributes to the biogeochemical cycling of elements and syntrophic microbial metabolism in complex natural environments. The Gram-positive lactic acid bacterium Enterococcus faecalis, an opportunistic human pathogen, is shown to be able to transfer electrons generated in fermentation metabolism to electrodes directly and indirectly via mediators. By exploiting E. faecalis wild-type and mutant cells, we demonstrate that reduced demethylmenaquinone in the respiratory chain in the bacterial cytoplasmic membrane is crucial for the EET. Heme proteins are not involved, and cytochrome bd oxidase activity was found to attenuate EET. These results are significant for the mechanistic understanding of EET in bacteria and for the design of microbial electrochemical systems. The basic findings infer that in dense microbial communities, such as in biofilm and in the large intestine, metabolism in E. faecalis and similar Gram-positive lactic acid bacteria might be electrically connected to other microbes. Such a transcellular electron transfer might confer syntrophic metabolism that promotes growth and other activities of bacteria in the microbiota of humans and animals.


Assuntos
Enterococcus faecalis/fisiologia , Infecções por Bactérias Gram-Positivas/microbiologia , Vitamina K 2/análogos & derivados , Biofilmes/crescimento & desenvolvimento , Citocromos/metabolismo , Eletricidade , Técnicas Eletroquímicas , Eletrodos , Transporte de Elétrons , Elétrons , Enterococcus faecalis/enzimologia , Enterococcus faecalis/crescimento & desenvolvimento , Fermentação , Humanos , Oxirredução , Vitamina K 2/metabolismo
8.
Mutat Res ; 791-792: 49-60, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-27648955

RESUMO

A single exposure to ionizing radiation (IR) results in an elevated cell-free DNA (cfDNA) content in the blood plasma. In this case, the cfDNA concentration can be a marker of the cell death in the organism. However, a chronic exposure to a low-dose IR enhances both the endonuclease activity and titer of antibodies to DNA in blood plasma, resulting in a decrease of the total concentration of circulating cfDNA in exposed people. In this case, the total cfDNA concentration should not be considered as a marker of the cell death in an exposed body. We assumed that a pool of the cfDNA circulating in the exposed people contains DNA fragments, which are resistant to a double-strand break formation in the environment of the elevated plasma endonuclease activity, and can be accumulated in the blood plasma. In order to test this hypothesis, we studied the content of GC-rich sequences (69%GC) of the transcribed region of human ribosomal repeat (rDNA), as well as the content of AT-rich repeat (63%AT) of satellite III (1q12) in the cfDNA samples obtained from 285 individuals. We have found that a chronic exposure to gamma-neutron radiation (N=88) and tritium ß-radiation (N=88) evokes an increase of the rDNA content (RrDNA index) and a decrease of the satellite III content (RsatIII index) in the circulating cfDNA as compared with the cfDNA of non-exposed people (N=109). Such index that simultaneously displays both the increase of rDNA content and decrease of satellite III content in the cfDNA (RrDNA/RsatIII) can be recommended as a marker of chronic processes in the body that involve the elevated cell death rate and/or increased blood plasma endonuclease activity.


Assuntos
Partículas beta/efeitos adversos , DNA Ribossômico/sangue , DNA Satélite/sangue , Raios gama/efeitos adversos , Exposição Ocupacional/efeitos adversos , Exposição à Radiação/efeitos adversos , Adolescente , Adulto , Idoso , Idoso de 80 Anos ou mais , Estudos de Coortes , Quebras de DNA de Cadeia Dupla , DNA Ribossômico/genética , DNA Satélite/genética , Relação Dose-Resposta à Radiação , Sequência Rica em GC , Humanos , Pessoa de Meia-Idade , Nêutrons , Exposição Ocupacional/análise , Doses de Radiação , Exposição à Radiação/análise , Reação em Cadeia da Polimerase em Tempo Real , Federação Russa , Sequências de Repetição em Tandem/genética , Trítio , Adulto Jovem
9.
Anal Bioanal Chem ; 408(22): 6009-17, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-27007732

RESUMO

Multiarray on a test strip (MATS) was developed for the detection of eight important potato pathogens. The proposed assay combines the rapidity of immunochromatography with the high throughput of array techniques. The test zone of the immunochromatographic strip comprises ordered rows of spots containing antibodies specific for different potato pathogens. The assay benefits from the simplicity of immunochromatography; colored immune complexes form at the corresponding spots within the test zone. The presence and intensity of the coloration are used for identification of the target pathogens. The MATS was applied to the simultaneous detection of eight priority potato pathogens, characterized by the following limits of detection: 1 ng/mL for potato virus X and the ordinary type of potato virus Y, 10 ng/mL for potato virus M, 20 ng/mL for potato leaf roll virus, 40 ng/mL for necrotic-type potato virus Y, 100 ng/mL for potato virus S, 300 ng/mL for potato virus A, and 10(4) cells/mL for Clavibacter michiganensis subsp. sepedonicus. Analysis time was 15 min. The observed sensitivity of the MATS was comparable to the traditional enzyme-linked immunosorbent assay. The developed technique was tested on potato leaf extracts, and its efficiency for on-site control of the pathogens was confirmed in 100 % by commercial LFIA test strips. Graphical abstract Location of binding zones in the developed multiarray on a test strip (MATS) for simultaneous detection of eight pathogens.


Assuntos
Cromatografia de Afinidade/métodos , Doenças das Plantas/virologia , Vírus de Plantas/isolamento & purificação , Fitas Reagentes/análise , Solanum tuberosum/virologia , Anticorpos Imobilizados/química , Cromatografia de Afinidade/economia , Cromatografia de Afinidade/instrumentação , Desenho de Equipamento , Ouro/química , Limite de Detecção , Nanopartículas Metálicas/química , Análise Serial de Proteínas/economia , Análise Serial de Proteínas/instrumentação , Análise Serial de Proteínas/métodos
10.
Mutat Res ; 779: 1-15, 2015 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-26113293

RESUMO

The blood plasma of healthy people contains cell-fee (circulating) DNA (cfDNA). Apoptotic cells are the main source of the cfDNA. The cfDNA concentration increases in case of the organism's cell death rate increase, for example in case of exposure to high-dose ionizing radiation (IR). The objects of the present research are the blood plasma and blood lymphocytes of people, who contacted occupationally with the sources of external gamma/neutron radiation or internal ß-radiation of tritium N = 176). As the controls (references), blood samples of people, who had never been occupationally subjected to the IR sources, were used (N = 109). With respect to the plasma samples of each donor there were defined: the cfDNA concentration (the cfDNA index), DNase1 activity (the DNase1 index) and titre of antibodies to DNA (the Ab DNA index). The general DNA damage in the cells was defined (using the Comet assay, the tail moment (TM) index). A chronic effect of the low-dose ionizing radiation on a human being is accompanied by the enhancement of the DNA damage in lymphocytes along with a considerable cfDNA content reduction, while the DNase1 content and concentration of antibodies to DNA (Ab DNA) increase. All the aforementioned changes were also observed in people, who had not worked with the IR sources for more than a year. The ratio cfDNA/(DNase1×Ab DNA × TM) is proposed to be used as a marker of the chronic exposure of a person to the external low-dose IR. It was formulated the assumption that the joint analysis of the cfDNA, DNase1, Ab DNA and TM values may provide the information about the human organism's cell resistivity to chronic exposure to the low-dose IR and about the development of the adaptive response in the organism that is aimed, firstly, at the effective cfDNA elimination from the blood circulation, and, secondly - at survival of the cells, including the cells with the damaged DNA.


Assuntos
Dano ao DNA/efeitos da radiação , DNA/efeitos da radiação , Linfócitos/efeitos da radiação , Exposição Ocupacional , Adulto , Idoso , Apoptose/efeitos da radiação , Partículas beta , Ensaio Cometa , DNA/sangue , Desoxirribonuclease I/metabolismo , Relação Dose-Resposta à Radiação , Feminino , Raios gama , Humanos , Masculino , Pessoa de Meia-Idade , Nêutrons , Centrais Nucleares , Federação Russa , Trítio
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