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1.
Microb Biotechnol ; 17(3): e14448, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38498302

RESUMO

Pseudomonas putida is a soil bacterium with multiple uses in fermentation and biotransformation processes. P. putida ATCC 12633 can biotransform benzaldehyde and other aldehydes into valuable α-hydroxyketones, such as (S)-2-hydroxypropiophenone. However, poor tolerance of this strain toward chaotropic aldehydes hampers efficient biotransformation processes. To circumvent this problem, we expressed the gene encoding the global regulator PprI from Deinococcus radiodurans, an inducer of pleiotropic proteins promoting DNA repair, in P. putida. Fine-tuned gene expression was achieved using an expression plasmid under the control of the LacIQ /Ptrc system, and the cross-protective role of PprI was assessed against multiple stress treatments. Moreover, the stress-tolerant P. putida strain was tested for 2-hydroxypropiophenone production using whole resting cells in the presence of relevant aldehyde substrates. P. putida cells harbouring the global transcriptional regulator exhibited high tolerance toward benzaldehyde, acetaldehyde, ethanol, butanol, NaCl, H2 O2 and thermal stress, thereby reflecting the multistress protection profile conferred by PprI. Additionally, the engineered cells converted aldehydes to 2-hydroxypropiophenone more efficiently than the parental P. putida strain. 2-Hydroxypropiophenone concentration reached 1.6 g L-1 upon a 3-h incubation under optimized conditions, at a cell concentration of 0.033 g wet cell weight mL-1 in the presence of 20 mM benzaldehyde and 600 mM acetaldehyde. Product yield and productivity were 0.74 g 2-HPP g-1 benzaldehyde and 0.089 g 2-HPP g cell dry weight-1 h-1 , respectively, 35% higher than the control experiments. Taken together, these results demonstrate that introducing PprI from D. radiodurans enhances chaotrope tolerance and 2-HPP production in P. putida ATCC 12633.


Assuntos
Deinococcus , Hidroxipropiofenona , Pseudomonas putida , Benzaldeídos/metabolismo , Pseudomonas putida/genética , Pseudomonas putida/metabolismo , Deinococcus/genética , Acetaldeído/metabolismo
2.
J Forensic Leg Med ; 102: 102653, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38422828

RESUMO

OBJECTIVE: To study the characteristics of postmortem ethanol production and its relation with alcohol congeners in postmortem rat liver and muscle tissues. METHOD: Postmortem liver and muscle tissues in Sprague-Dawley rats, from postmortem time interval (PMI) day 0-20, were analyzed via headspace gas chromatograph flame ionization detection to observe production of postmortem ethanol and 5 selected alcohol congeners. RESULT: 1. Putrid ethanol production increased gradually to a peak and then decreased with the prolongation of PMI; 2. Acetaldehyde, 1-propanol, and 3-methyl-butyraldehyde were produced along with postmortem ethanol; 1-butanol was only detected from day 11-20; 3. The concentrations of acetaldehyde, 1-propanol and 3-methyl-butyraldehyde was related with ethanol production. Fifteen mathematical models were constructed for putrid ethanol production based on acetaldehyde, 1-propanol, and 3-methyl-butyraldehyde. CONCLUSION: A peak in postmortem ethanol production was identified. The production trends of acetaldehyde, 1-propanol, and 3-methyl-butyraldehyde in the liver, and of 1-propanol in muscle, were consistent with those of ethanol, and could potentially to be used as biomarkers of postmortem ethanol production. Further human samples and data analysis are needed to verify this.


Assuntos
1-Propanol , Aldeídos , Etanol , Ratos , Humanos , Animais , Ratos Sprague-Dawley , Acetaldeído , Fígado , Músculos , Mudanças Depois da Morte
3.
Food Res Int ; 180: 114057, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38395574

RESUMO

The inhibitory effects of amino acids and their combinations on the formation of heterocyclic amines were investigated in this study. The great potential in the inhibition of HAs was observed in amino acid combinations compared with that of single agents. At a mass ratio of 1:1, a His-Pro combination achieved a maximum inhibitory rate of 80 %, and the total HAs content decreased to 4.70 ± 0.18 ng/g relative to the control (24.49 ± 2.18 ng/g). However, the inhibitory rate of triple combinations showed no obvious increase compared with the binary combinations. Benzaldehyde, phenylacetaldehyde, methylglyoxal, and glyoxal were positively correlated with HAs formation, and His-Pro combination (1:4) led to a significant reduction of benzaldehyde and phenylacetaldehyde at scavenging rates of 79 % and 92 %. Thus, the synergistic inhibition was achieved by simultaneously scavenging these aldehyde intermediates, and other inhibitory target, such as competition with precursors and elimination of final products can serve as supporting factors. These results provide a new perspective for approaches to enhance the suppression of HAs and control the formation of flavor compounds.


Assuntos
Acetaldeído/análogos & derivados , Aminoácidos , Compostos Heterocíclicos , Animais , Bovinos , Benzaldeídos , Aminas/química
4.
Environ Pollut ; 344: 123419, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38253164

RESUMO

Different amounts of glyoxal and paraformaldehyde were used to synthesize phenol-glyoxal (PG) and phenol-paraformaldehyde (PPF) resins, which were compared with conventional phenol-formaldehyde (PF) resins. Glyoxal oxidation leads to a pH value of 9.83 for PG 2.2. With the addition of polyformaldehyde, PPF 2.2 exhibited the highest viscosity at 17333.33 mPa s. The PPF 2.0 plywood has a maximum bonding strength of 1.94 MPa. The formaldehyde emission of PG 1.8 plywood is found to have a minimum value of 0.025 mg/m3, reaching the ENF limit (≤0.025 mg/m3). Acetaldehyde is found only in volatile organic compound (VOC) emissions from PG plywood and is associated with increased glyoxal. PPF plywood emitted more aromatic and total VOC (TVOC) than the other two plywood types. The measured TVOC for PPF 2.2 is 196.07 µg/m3. The results showed that the total cancer risk (TCR) values of PPF 1.8, PPF 2.0, and PG 1.8 were above the threshold of 1.00E-4, indicating a definite carcinogenic risk. Acetaldehyde in the PG plywood exceeded the safety threshold for noncarcinogenic risk. The use of paraformaldehyde in the wood-based panel production is been considered a possible means of improving the bonding strength of plywood. Glyoxal has also been shown to be a viable method for lowering the formaldehyde emissions from plywood. The VOC emissions from plywood changed significantly depending on the aldehyde used. Limiting VOCs that present high health hazards is crucial for reducing the negative impact of plywood on both indoor environments and human health.


Assuntos
Aldeídos , Polímeros , Compostos Orgânicos Voláteis , Humanos , Formaldeído , Fenóis , Fenol , Glioxal , Acetaldeído
5.
Artigo em Inglês | MEDLINE | ID: mdl-38248538

RESUMO

Accurate determination of the concentration of alcohols and their metabolites is important in forensics and in several life science areas. A new headspace gas chromatography-mass spectrometry method has been developed to quantify alcohols and their oxidative products using isotope-labeled internal standards. The limit of detection (LOD) of the analytes in the developed method was 0.211 µg/mL for methanol, 0.158 µg/mL for ethanol, 0.157 µg/mL for isopropanol, 0.010 µg/mL for n-propanol, 0.157 µg/mL for acetone, and 0.209 µg/mL for acetaldehyde. The precision and accuracy of the method were evaluated, and the relative standard deviation percentages were found to be less than 3%. This work demonstrates the application of this method, specifically in quantifying the concentration of oxidative products of alcohol and other minor alcohols found in hand sanitizers, which have become an essential household item since the COVID-19 pandemic. Apart from the major components, the minor alcohols found in hand sanitizers include methanol, isopropanol, and n-propanol. The concentration range of these minor alcohols found in ethanol-based hand sanitizer samples was as follows: methanol, 0.000921-0.0151 mg/mL; isopropanol, 0.454-13.8 mg/mL; and n-propanol, 0.00474-0.152 mg/mL. In ethanol-based hand sanitizers, a significant amount of acetaldehyde (0.00623-0.231 mg/mL) was observed as an oxidation product, while in the isopropanol-based hand sanitizer, acetone (0.697 mg/mL) was observed as an oxidation product. The concentration of acetaldehyde in ethanol-based hand sanitizers significantly increased with storage time and temperature, whereas no such increase in acetone concentration was observed in isopropanol-based hand sanitizers with storage time and temperature. In two of the selected hand sanitizers, the acetaldehyde levels increased by almost 200% within a week when stored at room temperature. Additionally, exposing the hand sanitizers to a temperature of 45 °C for 24 h resulted in a 100% increase in acetaldehyde concentration. On the contrary, the acetone level remained constant upon the change in storage time and temperature.


Assuntos
Higienizadores de Mão , Metanol , Humanos , Acetaldeído , Acetona , 2-Propanol , 1-Propanol , Temperatura , Cromatografia Gasosa-Espectrometria de Massas , Pandemias , Etanol
6.
Int J Mol Sci ; 25(2)2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38256150

RESUMO

Aldehyde:ferredoxin oxidoreductases (AORs) have been isolated and biochemically-characterized from a handful of anaerobic or facultative aerobic archaea and bacteria. They catalyze the ferredoxin (Fd)-dependent oxidation of aldehydes to acids. Recently, the involvement of AOR in the reduction of organic acids to alcohols with electrons derived from sugar or synthesis gas was demonstrated, with alcohol dehydrogenases (ADHs) carrying out the reduction of the aldehyde to the alcohol (AOR-ADH pathway). Here, we describe the biochemical characterization of an AOR of the thermophilic fermentative bacterium Thermoanaerobacter sp. strain X514 (AORX514). The putative aor gene (Teth514_1380) including a 6x-His-tag was introduced into the genome of the genetically-accessible, related species Thermoanaerobacter kivui. The protein was purified to apparent homogeneity, and indeed revealed AOR activity, as measured by acetaldehyde-dependent ferredoxin reduction. AORX514 was active over a wide temperature (10 to 95 °C) and pH (5.5 to 11.5) range, utilized a wide variety of aldehydes (short and branched-chained, aliphatic, aromatic) and resembles archaeal sensu stricto AORs, as the protein is active in a homodimeric form. The successful, recombinant production of AORX514 in a related, well-characterized and likewise strict anaerobe paves the road towards structure-function analyses of this enzyme and possibly similar oxygen-sensitive or W/Mo-dependent proteins in the future.


Assuntos
Aldeídos , Ferredoxinas , Ferredoxinas/genética , Thermoanaerobacter/genética , Acetaldeído , Álcool Desidrogenase , Archaea , DNA Topoisomerases Tipo I
7.
Pestic Biochem Physiol ; 198: 105716, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38225073

RESUMO

Land snails are the most harmful pests in agricultural fields. Eobania vermiculata is a widespread snail species that causes massive damage to all agricultural crops. Thus, the molluscicidal activity of calcium borate nanoparticles (CB-NPs) against Eobania vermiculata was evaluated and compared with metaldehyde (Gastrotox® E 5% G). The amorphous phase of CB-NPs was obtained after thermal treatment at a low temperature (500 °C) which conformed by X-ray diffraction (XRD) analysis. CB-NPs are composed of aggregated nano-sheets with an average thickness of 54 nm which enhanced their molluscicidal activity. These nano-sheets displayed meso-porous network architecture with pore diameters of 13.65 nm, and a 9.46 m2/g specific surface area. CB-NPs and metaldehyde (Gastrotox® E 5% G) exhibited molluscicidal effects on Eobania vermiculata snails with median lethal concentrations LC50 of 175.3 and 60.5 mg/l, respectively, after 72 h of exposure. The results also showed significant reductions of Eobania vermiculata snails hemocytes' mean total number, the levels of Testosterone (T) and Estrogen (E), alkaline phosphatase, acid phosphatase, albumin, and protein concentrations, succinate dehydrogenase, glucose, triglycerides and phospholipids levels, while significant increases in the phagocytic index and mortality index, both transaminases (ALT and AST) and glycogen phosphorylase concentration were observed after the exposure to LC50 of CB-NPs or metaldehyde (Gastrotox® E 5% G) compared to the control group. Therefore, CB-NPs could be used as an alternative molluscicide for controlling Eobania vermiculata, but further studies are needed to assess their effects on non-target organisms.


Assuntos
Acetaldeído/análogos & derivados , Boratos , Moluscocidas , Caramujos , Animais , Compostos de Cálcio/metabolismo , Compostos de Cálcio/farmacologia , Moluscocidas/farmacologia , Flores
8.
Biochim Biophys Acta Gen Subj ; 1868(2): 130527, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38043915

RESUMO

Acetaldehyde can be found in human cells as a byproduct of various metabolic pathways, including oxidative processes such as lipid peroxidation. This secondary product of lipid peroxidation plays a role in various pathological processes, leading to various types of civilization diseases. In this study, the formation of free acetaldehyde induced by oxygen-centred radicals was studied in monocyte-like cell line U937. Exposure of U937 cells to peroxyl/alkoxyl radicals induced by azocompound resulted in the formation of free acetaldehyde. Acetaldehyde is formed by the cleavage of fatty acids, which represents the breakdown of fatty acids into smaller fragments initiated by the cyclization of lipid peroxyl radical and ß-scission of lipid alkoxyl radical. The cleavage of fatty acids alters the integrity of the plasma and nuclear membrane, leading to the loss of cell viability. Understanding the pathological processes of acetaldehyde formation is an active area of research with potential implications for preventing and treating various diseases associated with oxidative stress.


Assuntos
Acetaldeído , Monócitos , Humanos , Peroxidação de Lipídeos , Radicais Livres/metabolismo , Células U937 , Monócitos/metabolismo , Ácidos Graxos/metabolismo , Espécies Reativas de Oxigênio
9.
J Am Coll Surg ; 238(3): 272-279, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38063669

RESUMO

BACKGROUND: Surgical smoke is an occupational health problem and is increasingly recognized as a potential source of virus transmission. Dedicated smoke evacuators are used to protect against surgical smoke exposure. We tested the hypothesis that using smoke evacuators would reduce volatile organic compounds and the number of particles in surgical smoke during the laparotomy procedure. STUDY DESIGN: A randomized, double-blind clinical trial was conducted in patients undergoing laparotomy from June 11, 2021, to March 30, 2022, to compare the effectiveness of smoke evacuators with a control (registration, UMIN000044250). The primary outcome was a change in the acetaldehyde level. Secondary outcomes were changes in the formaldehyde level and particle count assessed by the particle size of 0.3, 0.5, 1.0, and 5.0 nm. RESULTS: A total of 42 patients were randomized and assessed (smoke evacuator group, n = 22 vs control group, n = 20). The acetaldehyde level was significantly lower in the smoke evacuator group than in the control group: mean (95% CI), 10.6 (3.7 to 17.5) vs 47.2 (19.9 to 74.5) µg/m 3 , p < 0.001. Similarly, the formaldehyde level was 72.2% lower in the smoke evacuator group than in the control group. Particle counts by each particle size category were 80% to 95% lower in the smoke evacuator group than in the control group (all, p < 0.001). CONCLUSIONS: Dedicated smoke evacuators reduced the level of acetaldehyde and formaldehyde, and the number of particles in surgical smoke, minimizing the potential exposure to volatile organic compounds and particle matters during surgery.


Assuntos
Doenças Profissionais , Compostos Orgânicos Voláteis , Humanos , Fumaça/prevenção & controle , Compostos Orgânicos Voláteis/análise , Laparotomia , Acetaldeído , Formaldeído
10.
Carcinogenesis ; 45(1-2): 95-106, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-37978873

RESUMO

The alcohol metabolite acetaldehyde is a potent human carcinogen linked to esophageal squamous cell carcinoma (ESCC) initiation and development. Aldehyde dehydrogenase 2 (ALDH2) is the primary enzyme that detoxifies acetaldehyde in the mitochondria. Acetaldehyde accumulation causes genotoxic stress in cells expressing the dysfunctional ALDH2E487K dominant negative mutant protein linked to ALDH2*2, the single nucleotide polymorphism highly prevalent among East Asians. Heterozygous ALDH2*2 increases the risk for the development of ESCC and other alcohol-related cancers. Despite its prevalence and link to malignant transformation, how ALDH2 dysfunction influences ESCC pathobiology is incompletely understood. Herein, we characterize how ESCC and preneoplastic cells respond to alcohol exposure using cell lines, three-dimensional organoids and xenograft models. We find that alcohol exposure and ALDH2*2 cooperate to increase putative ESCC cancer stem cells with high CD44 expression (CD44H cells) linked to tumor initiation, repopulation and therapy resistance. Concurrently, ALHD2*2 augmented alcohol-induced reactive oxygen species and DNA damage to promote apoptosis in the non-CD44H cell population. Pharmacological activation of ALDH2 by Alda-1 inhibits this phenotype, suggesting that acetaldehyde is the primary driver of these changes. Additionally, we find that Aldh2 dysfunction affects the response to cisplatin, a chemotherapeutic commonly used for the treatment of ESCC. Aldh2 dysfunction facilitated enrichment of CD44H cells following cisplatin-induced oxidative stress and cell death in murine organoids, highlighting a potential mechanism driving cisplatin resistance. Together, these data provide evidence that ALDH2 dysfunction accelerates ESCC pathogenesis through enrichment of CD44H cells in response to genotoxic stressors such as environmental carcinogens and chemotherapeutic agents.


Assuntos
Neoplasias Esofágicas , Carcinoma de Células Escamosas do Esôfago , Humanos , Camundongos , Animais , Carcinoma de Células Escamosas do Esôfago/genética , Aldeído Desidrogenase/genética , Aldeído Desidrogenase/metabolismo , Neoplasias Esofágicas/patologia , Fatores de Risco , Consumo de Bebidas Alcoólicas/genética , Cisplatino/farmacologia , Aldeído-Desidrogenase Mitocondrial/genética , Etanol/metabolismo , Acetaldeído/metabolismo , Transformação Celular Neoplásica , Células-Tronco Neoplásicas/patologia , Álcool Desidrogenase/genética
11.
Alcohol Alcohol ; 59(1)2024 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-37950904

RESUMO

Ethanol metabolism plays an essential role in how the body perceives and experiences alcohol consumption, and evidence suggests that modulation of ethanol metabolism can alter the risk for alcohol use disorder (AUD). In this review, we explore how ethanol metabolism, mainly via alcohol dehydrogenase and aldehyde dehydrogenase 2 (ALDH2), contributes to drinking behaviors by integrating preclinical and clinical findings. We discuss how alcohol dehydrogenase and ALDH2 polymorphisms change the risk for AUD, and whether we can harness that knowledge to design interventions for AUD that alter ethanol metabolism. We detail the use of disulfiram, RNAi strategies, and kudzu/isoflavones to inhibit ALDH2 and increase acetaldehyde, ideally leading to decreases in drinking behavior. In addition, we cover recent preclinical evidence suggesting that strategies other than increasing acetaldehyde-mediated aversion can decrease ethanol consumption, providing other potential metabolism-centric therapeutic targets. However, modulating ethanol metabolism has inherent risks, and we point out some of the key areas in which more data are needed to mitigate these potential adverse effects. Finally, we present our opinions on the future of treating AUD by the modulation of ethanol metabolism.


Assuntos
Alcoolismo , Humanos , Alcoolismo/tratamento farmacológico , Alcoolismo/metabolismo , Etanol/efeitos adversos , Aldeído-Desidrogenase Mitocondrial/genética , Aldeído Desidrogenase/metabolismo , Álcool Desidrogenase , Consumo de Bebidas Alcoólicas/efeitos adversos , Acetaldeído/metabolismo
12.
Luminescence ; 39(1): e4609, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37880857

RESUMO

The new drug linagliptin belongs to the class of dipeptidyl peptidase-4 enzyme inhibitors. Linagliptin is used to treat type 2 diabetes and is taken orally either alone or in combination with other drugs. In this instance, a new, simple, and economical technique for analyzing linagliptin was developed by the effective use of a pyrrolidone derivative. The primary amine group of linagliptin permits its condensation with ninhydrin (0.14% w/v) to produce a fluorescent product in the presence of phenylacetaldehyde (0.02% v/v). All experimental parameters were carefully examined and adjusted in order to monitor the generation of the pyrrolidone derivative at excitation and emission wavelengths of 385 and 475 nm, respectively. The calibration graph was made by plotting the intensity of the fluorescence in relation to linagliptin concentration. A significant linearity was found for values ranging from 20 to 460 ng/mL. The process's validity has been verified by a thorough assessment of the instructions provided by the International Conference on Harmonization (ICH). The results indicate excellent uniformity with a reference method, showing that there is no substantial difference in precision and accuracy. The proposed approach was utilized for determining linagliptin in real rat plasma successfully owing to its high sensitivity. Additionally, the proposed approach was evaluated using the Eco-Scale evaluation tool and showed a high degree of eco-friendliness (86/100).


Assuntos
Acetaldeído/análogos & derivados , Diabetes Mellitus Tipo 2 , Linagliptina , Animais , Ratos , Diabetes Mellitus Tipo 2/tratamento farmacológico , Ninidrina/química , Pirrolidinonas
13.
J Biochem Mol Toxicol ; 38(1): e23518, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37638564

RESUMO

Aldehyde dehydrogenase 2 (ALDH2) deficiency caused by   genetic variant is present in more than 560 million people of East Asian descent, which can be identified by apparent facial flushing from acetaldehyde accumulation after consuming alcohol. Recent findings indicated that ALDH2 also played a critical role in detoxification of formaldehyde (FA). Our previous studies showed that FA could enhance macrophagic inflammatory responses through the induction of HIF-1α-dependent glycolysis. In the present study, pro-inflammatory responses and glycolysis promoted by 0.5 mg/m3 FA were found in mice with Aldh2 gene knockout, which was confirmed in the primary macrophages isolated from Aldh2 gene knockout mice treated with 50 µM FA. FA at 50 and 100 µM also induced stronger dose-dependent increases of pro-inflammatory responses and glycolysis in RAW264.7 murine macrophages with knock-down of ALDH2, and the enhanced effects induced by 50 µM FA was alleviated by inhibition of HIF-1α in RAW264.7 macrophages with ALDH2 knock-down. Collectively, these results clearly demonstrated that ALDH2 deficiency reinforced pro-inflammatory responses and glycolysis in macrophages potentiated by environmentally relevant concentration of FA, which may increase the susceptibility to inflammation and immunotoxicity induced by environmental FA exposure.


Assuntos
Acetaldeído , Etanol , Humanos , Camundongos , Animais , Aldeído-Desidrogenase Mitocondrial/genética , Etanol/toxicidade , Acetaldeído/toxicidade , Formaldeído/toxicidade , Camundongos Knockout , Macrófagos
14.
Int J Biol Macromol ; 259(Pt 1): 129080, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38161018

RESUMO

Volatile aldehydes have an adverse impact on both human health and the environment, therefore, a fast, straightforward, highly accurate detection technique for the simultaneous detection and removal of several aldehydes is eagerly anticipated. Herein, novel APGF@ZIF-8 and APOF@ZIF-8 sensing materials were developed by coating fluorescent alginate-modified surfactants (APGF and APOF) into the ZIF-8 MOFs to produce quite porous fluorescent sensors (SBET up to 1519 m2/g). The detection capacity of the prepared sensors for benzaldehyde, glyoxal, formaldehyde, and acetaldehyde has been examined. The detection mechanism was suggested as hydrogen bonding formation between the sensors and volatile aldehydes as confirmed by Gaussian calculations. All the fluorescence spectra of aldehydes display remarkable linear detection relationships in the range of 0.05-200 µM with the limits of detection (LOD) values in the range of 0.001-0.18 µM (0.106-10.44 ppb). These sensors were utilized successfully to detect multiple volatile aldehydes in river water samples with satisfactory recoveries of 96-107 %. Interestingly, fluorescent APGF@ZIF-8/CS and APOF@ZIF-8/CS films as portable disposable removal techniques for benzaldehyde, glyoxal, formaldehyde, and acetaldehyde from water were fabricated. APOF@ZIF-8/CS exhibited an excellent formaldehyde adsorption capacity of 58.30 mg/g and an adsorption removal efficiency of 93.5 %. The adsorption process of biosorbent on various aldehydes was fitted by Freundlich adsorption isotherm. The adsorption kinetics followed Pseudo-second-order kinetic model.


Assuntos
Estruturas Metalorgânicas , Poluentes Químicos da Água , Humanos , Aldeídos , Benzaldeídos , Água , Adsorção , Alginatos , Poluentes Químicos da Água/análise , Corantes , Formaldeído , Acetaldeído , Glioxal
15.
J Environ Sci (China) ; 139: 377-388, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38105063

RESUMO

Atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter, for which the reason have not been clearly elucidated. Here we measured carbonyl compounds and other trace gasses together with PM2.5 over urban Jinan in North China Plain during the winter. Markedly higher carbonyl concentrations (average: 14.63 ± 4.21 ppbv) were found during wintertime haze pollution, about one to three-times relative to those on non-haze days, with slight difference in chemical composition except formaldehyde (HCHO). HCHO (3.68 ppbv), acetone (3.17 ppbv), and acetaldehyde (CH3CHO) (2.83 ppbv) were the three most abundant species, accounting for ∼75% of the total carbonylson both haze and non-haze days. Results from observational-based model (OBM) with atmospheric oxidation capacity (AOC) indicated that AOC significantly increased with the increasing carbonyls during the winter haze events. Carbonyl photolysis have supplied key oxidants such as RO2 and HO2, and thereby enhancing the formation of fine particles and secondary organic aerosols, elucidating the observed haze-carbonyls inter-correlation. Diurnal variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources. 1-butene was further confirmed to be the major precursor for HCHO. This study confirms the great contribution of carbonyls to AOC, and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.


Assuntos
Poluentes Atmosféricos , Poluentes Atmosféricos/análise , China , Material Particulado/análise , Estações do Ano , Acetaldeído/análise , Monitoramento Ambiental , Aerossóis/análise
16.
J Agric Food Chem ; 72(1): 461-474, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38153324

RESUMO

l-threo-p-methylsulfonylphenylserine (compound 1b) is the main intermediate of florfenicol, and its efficient synthesis has been the subject of current research. Herein, Burkholderia diffusa l-threonine transaldolase (BuLTTA) was rationally designed based on the sequence-structure-function relationship. A mutant M4 (Asn35Ser/Thr352Asn) could produce 35.5 mM 1b with 88.8% conversion and 93.8% diastereoselectivity, 314 and 129% of the values observed for wild-type BuLTTA. Molecular dynamics simulations indicated that the shortened distance between key active site residues and the transition state (PLP-1b) and the improved hydrogen bond force enhanced the catalytic performance of the M4 variant. Then, the mutant M4 was combined with K. kurtzmanii alcohol dehydrogenase (KkADH) to eliminate the BuLTTA-inhibiting byproduct acetaldehyde, and a cosubstrate was added to regenerate the ADH cofactor NADH. Under optimized conditions, the yield of 1b reached 115.2 mM with a conversion of 96% and a diastereoselectivity of 95.5%. This work provides a new strategy for the efficient and sustainable production of 1b.


Assuntos
Tianfenicol , Treonina , Transaldolase , Acetaldeído
17.
Chem Biol Interact ; 388: 110853, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38151107

RESUMO

Alcohol dehydrogenase catalyzes the reversible transfer of a hydride directly from an alcohol to the nicotinamide ring of NAD+ to form an aldehyde and NADH, and the proton from the alcohol probably is transferred through a hydrogen-bonded system to the imidazole of His-48. Studies of the pH dependencies, and solvent and substrate isotope effects on the wild-type and the enzyme with His-48 substituted with Gln-48 were used to demonstrate a role for the proton relay system. The H48Q substitution increases affinities for NAD+ and NADH by ∼2-fold, suggesting that the overall protein structure is maintained. In contrast, catalytic efficiencies (V/Km) on ethanol and acetaldehyde and affinity for 2,2,2-trifluoroethanol are decreased by about 10-fold. The pH dependencies for catalytic efficiencies on ethanol and acetaldehyde (log V/Km versus pH), show pK values of about 7.5 for wild-type enzyme, but ethanol oxidation by H48Q ADH is essentially linear over the pH range from 5.5 to 9.2 with a slope of 0.47. Steady-state kinetics and substrate isotope effects suggest that the kinetic mechanism of H48Q ADH has become partly random for oxidation of ethanol. Both wild-type and H48Q ADHs have pH-independent isotope effects for oxidation (V1/Kb) of 1-butanol/1-butanol-d9 of 4, suggesting that hydride transfer is a major rate-limiting step. The pH dependence for butanol oxidation by wild type ADH shows a wavy profile over the pH range from pH 6 to 10, with a ∼2.3-fold larger V1/Kb in D2O than in H2O, an "inverse" isotope effect. The substrate isotope effect of 4 is not altered by the solvent isotope effect, suggesting concerted proton/hydride transfer. The solvent isotope effect can be explained by a ground state with a water bound to the catalytic zinc in the enzyme-NAD+ complex, and a transition state that resembles a complex with NADH and aldehyde. In contrast, the H48Q enzyme has a diminished inverse solvent isotope effect of ∼1.3 and an essentially linear pH dependence with a slope of log V1/Kb against pH of 0.49 for oxidation of 1-butanol, which together are consistent with a transition state where hydroxide ion directly accepts a proton from the 2'-hydroxyl group of the nicotinamide ribose in the proton relay system in the enzyme-NAD+-alcohol complex. The results support a catalytic role for His-48 in the proton relay system.


Assuntos
Álcool Desidrogenase , Prótons , Álcool Desidrogenase/metabolismo , NAD/metabolismo , Solventes , 1-Butanol , Mutagênese , Etanol , Isótopos , Aldeídos , Concentração de Íons de Hidrogênio , Acetaldeído , Cinética
18.
RMD Open ; 9(4)2023 12 01.
Artigo em Inglês | MEDLINE | ID: mdl-38053459

RESUMO

OBJECTIVE: In rheumatoid arthritis (RA) around two-thirds of patients are autoantibody positive for rheumatoid factor, anti-citrullinated protein antibodies and/or anti-carbamylated protein antibodies. The remaining seronegative subgroup of patients is clinically heterogeneous and thus far, biomarkers predicting the disease course are lacking. Therefore, we analysed the value of other autoantibodies in RA directed against malondialdehyde-acetaldehyde adducts (MAA) and advanced glycation end-products (AGE). METHODS: In sera of 648 patients with RA and 538 patients without RA from the Leiden Early Arthritis Clinic, anti-MAA and anti-AGE IgG antibody levels were measured using ELISA. Associations between genetic risk factors, acute phase reactants, radiological joint damage, remission and anti-PTM positivity were investigated using regression, correlation and survival analyses. RESULTS: Anti-AGE and anti-MAA were most prevalent in RA (44.6% and 46.1% respectively) but were also present in non-RA arthritis patients (32.9% and 30.3% respectively). Anti-AGE and anti-MAA antibodies were associated with HLA-DRB1*03 within seronegative RA (OR=1.98, p=0.003, and OR=2.37, p<0.001, respectively) and, for anti-AGE also in non-RA arthritis patients (OR=2.34, p<0.001). Presence of anti-MAA antibodies was associated significantly with markers of inflammation, erythrocyte sedimentation rate and C reactive protein, in all groups independent of anti-AGE. Interestingly, the presence of anti-AGE and anti-MAA antibodies was associated with radiological progression in patients with seronegative RA, but not evidently with sustained drug-free remission. CONCLUSIONS: Anti-AGE and anti-MAA were present in around 45% of RA patients and 30% of non-RA arthritis patients, and although not specific for RA, their presence associated with HLA, inflammation and, for RA, with clinical outcomes especially in patients with seronegative RA.


Assuntos
Acetaldeído , Artrite Reumatoide , Humanos , Malondialdeído , Reação de Maillard , Autoanticorpos , Fenótipo , Inflamação
19.
Environ Sci Technol ; 57(50): 21235-21248, 2023 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-38051783

RESUMO

Due in part to climate change, wildfire activity is increasing, with the potential for greater public health impact from smoke in downwind communities. Studies examining the health effects of wildfire smoke have focused primarily on fine particulate matter (PM2.5), but there is a need to better characterize other constituents, such as hazardous air pollutants (HAPs). HAPs are chemicals known or suspected to cause cancer or other serious health effects that are regulated by the United States (US) Environmental Protection Agency. Here, we analyzed concentrations of 21 HAPs in wildfire smoke from 2006 to 2020 at 309 monitors across the western US. Additionally, we examined HAP concentrations measured in a major population center (San Jose, CA) affected by multiple fires from 2017 to 2020. We found that concentrations of select HAPs, namely acetaldehyde, acrolein, chloroform, formaldehyde, manganese, and tetrachloroethylene, were all significantly elevated on smoke-impacted versus nonsmoke days (P < 0.05). The largest median increase on smoke-impacted days was observed for formaldehyde, 1.3 µg/m3 (43%) higher than that on nonsmoke days. Acetaldehyde increased 0.73 µg/m3 (36%), and acrolein increased 0.14 µg/m3 (34%). By better characterizing these chemicals in wildfire smoke, we anticipate that this research will aid efforts to reduce exposures in downwind communities.


Assuntos
Poluentes Atmosféricos , Incêndios Florestais , Acetaldeído , Acroleína , Poluentes Atmosféricos/efeitos adversos , Poluentes Atmosféricos/análise , Exposição Ambiental , Formaldeído , Material Particulado/análise , Fumaça/efeitos adversos , Estados Unidos
20.
Artigo em Inglês | MEDLINE | ID: mdl-38082983

RESUMO

The breakdown of ethanol, the active chemical in alcohol, is tightly regulated by the body, yet alcohol intoxication occurs in thousands of Americans annually. Many factors contribute to the concentration of ethanol in the bloodstream and the tolerance an individual has, including body size, previous drinking experience, and liver functionality. We propose a model that estimates both the blood alcohol concentration and the concentration of acetaldehyde (the toxic intermediate during catabolism) in the liver over time to quantify organ damage for an average person. From the current literature, we derived ordinary differential equations that govern the absorption of ethanol in the body and extended it with the metabolic enzyme mechanisms. We also altered the parameters of our system in order to show the effects of Asian flush, which impairs the body's processing of acetaldehyde. We demonstrated the accumulation of acetaldehyde in Asian flush patients was about 660 times higher compared to those without the disease.Clinical relevance-With further improvements and personalization, our model would be able to quantitatively describe the effects of alcohol consumption without having volunteers go through repetitive trials with extensive exposure to alcohol. Liver damage can also be estimated with the acetaldehyde buildup predicted by the model.


Assuntos
Intoxicação Alcoólica , Concentração Alcoólica no Sangue , Humanos , Etanol/metabolismo , Acetaldeído/metabolismo , Fígado
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