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1.
Proc Natl Acad Sci U S A ; 121(31): e2400525121, 2024 Jul 30.
Article in English | MEDLINE | ID: mdl-39042683

ABSTRACT

Per- and polyfluoroalkyl substances (PFAS), particularly the perfluorinated ones, are recalcitrant to biodegradation. By integrating an enrichment culture of reductive defluorination with biocompatible electrodes for the electrochemical process, a deeper defluorination of a C6-perfluorinated unsaturated PFAS was achieved compared to the biological or electrochemical system alone. Two synergies in the bioelectrochemical system were identified: i) The in-series microbial-electrochemical defluorination and ii) the electrochemically enabled microbial defluorination of intermediates. These synergies at the material-microbe interfaces surpassed the limitation of microbial defluorination and further turned the biotransformation end products into less fluorinated products, which could be less toxic and more biodegradable in the environment. This material-microbe hybrid system brings opportunities in the bioremediation of PFAS driven by renewable electricity and warrants future research on mechanistic understanding of defluorinating and electroactive microorganisms at the material-microbe interface for system optimizations.


Subject(s)
Biodegradation, Environmental , Anaerobiosis , Halogenation , Electrodes/microbiology , Fluorocarbons/metabolism , Fluorocarbons/chemistry , Electrochemical Techniques/methods , Bacteria/metabolism
2.
Chem Catal ; 1(3): 704-720, 2021 Aug 19.
Article in English | MEDLINE | ID: mdl-34693393

ABSTRACT

Powered by renewable electricity, biological | inorganic hybrids employ water-splitting electrocatalysis and generate H2 as reducing equivalents for microbial catalysis. The approach integrates the beauty of biocatalysis with the energy efficiency of inorganic materials for sustainable chemical production. Yet a successful integration requires delicate control of the hybrid's extracellular chemical environment. Such an argument is evident in the exemplary case of O2 because biocatalysis has a stringent requirement of O2 but the electrocatalysis may inadvertently perturb the oxidative pressure of biological moieties. Here we report the addition of perfluorocarbon (PFC) nanoemulsions promote a biocompatible O2 microenvironment in a O2-sensitive N2-fixing biological | inorganic hybrid. Langmuir-type nonspecific binding between bacteria and nanoemulsions facilitates O2 transport in bacterial microenvironment and leads to a 250% increase in efficiency for organic fertilizers within 120 hours. Controlling the biological microenvironment with nanomaterials heralds a general approach accommodating the compatibility in biological | inorganic hybrids.

3.
Anal Chem ; 88(12): 6479-84, 2016 06 21.
Article in English | MEDLINE | ID: mdl-27212711

ABSTRACT

Blood is a major contributor of evidence in investigations involving violent crimes because of the unique composition of proteins and low molecular weight compounds present in the circulatory system, which often serve as biomarkers in clinical diagnostics. It was recently shown that biomarkers present in blood can also identify characteristics of the originator, such as ethnicity and biological sex. A biocatalytic assay for on-site forensic investigations was developed to simultaneously identify the age range of the blood sample originator and the time since deposition (TSD) of the blood spot. For these two characteristics to be identified, the levels of alkaline phosphatase (ALP), a marker commonly used in clinical diagnostics corresponding to old and young originators, were monitored after deposition for up to 48 h to mimic a crime scene setting. ALP was chosen as the biomarker due to its age-dependent nature. The biocatalytic assay was used to determine the age range of the originator using human serum samples. By means of statistical tools for evaluation and the physiological levels of ALP in healthy people, the applicability of this assay in forensic science was shown for the simultaneous determination of the age of the originator and the TSD of the blood spot. The stability of ALP in serum allows for the differentiation between old and young originators up to 2 days after the sample was left under mimicked crime scene conditions.


Subject(s)
Alkaline Phosphatase/blood , Forensic Sciences/methods , Adolescent , Adult , Blood Stains , Child , Child, Preschool , Crime , Enzyme Assays/methods , Female , Humans , Infant , Male , Middle Aged , Young Adult
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