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1.
J Appl Microbiol ; 135(4)2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38573833

RESUMO

In the 1940s and 1950s, researchers seeking safe and novel ways to eliminate airborne pathogens from enclosed spaces, investigated glycol vapours as a method of disinfection. More recently, the COVID-19 pandemic highlighted the need for a non-toxic aerial disinfectant that can be used in the presence of people. This scoping review is intended to analyse the early and more recent literature on glycol disinfection, scrutinizing the methodologies used, and to determine if the use of glycols as modern-day disinfectants is justified PRISMA-ScR guidelines were used to assess the 749 articles retrieved from the Web of Science platform, with 46 articles retained after the search strategy was applied. Early studies generally demonstrated good disinfection capabilities against airborne bacteria and viruses, particularly with propylene glycol (PG) vapour. Vapour pressure, relative humidity, and glycol concentration were found to be important factors affecting the efficacy of glycol vapours. Contact times depended mainly on the glycol application method (i.e. aerosolization or liquid formulation), although information on how glycol efficacy is impacted by contact time is limited. Triethylene glycol (TEG) is deemed to have low toxicity, carcinogenicity, and mutagenicity and is registered for use in air sanitization and deodorization by the US Environmental Protection Agency. Glycols are also used in liquid formulations for their antimicrobial activity against a wide range of microorganisms, although when used as a non-active excipient in products, their contribution to antimicrobial efficacy is rarely assessed. The appropriate use of liquid glycol-containing formulations was found to positively impact the antimicrobial capabilities of disinfectants when used at temperatures <0, food preservatives, and dental medicaments. Providing modern delivery technology can accurately control environmental conditions, the use of aerosolized glycol formulations should lead to successful disinfection, aiding infection prevention, and control regimens.


Assuntos
Anti-Infecciosos , Desinfetantes , Humanos , Pandemias/prevenção & controle , Desinfetantes/farmacologia , Desinfecção/métodos , Anti-Infecciosos/farmacologia , Propilenoglicol/farmacologia , Gases
2.
Environ Sci Technol ; 58(15): 6704-6715, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-38574268

RESUMO

The transformation of toxic arsine (AsH3) gas into valuable elemental arsenic (As0) from industrial exhaust gases is important for achieving sustainable development goals. Although advanced arsenic removal catalysts can improve the removal efficiency of AsH3, toxic arsenic oxides generated during this process have not received adequate attention. In light of this, a novel approach for obtaining stable As0 products was proposed by performing controlled moderate oxidation. We designed a tailored Ni-based catalyst through an acid etching approach to alter interactions between Ni and NaY. As a result, the 1Ni/NaY-H catalyst yielded an unprecedented proportion of As0 as the major product (65%), which is superior to those of other reported catalysts that only produced arsenic oxides. Density functional theory calculations clarified that Ni species changed the electronic structure of oxygen atoms, and the formed [NiIII-OH (µ-O)] active centers facilitated the adsorption of AsH2*, AsH*, and As* reaction intermediates for As-H bond cleavage, thereby decreasing the direct reactivity of oxygen with the arsenic intermediates. This work presents pioneering insights into inhibiting excessive oxidation during AsH3 removal, demonstrating potential environmental applications for recovery of As0 from toxic AsH3.


Assuntos
Arsênio , Zeolitas , Níquel/química , Elétrons , Oxigênio , Gases
3.
Luminescence ; 39(4): e4731, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38566570

RESUMO

Nerve agents are becoming serious issues for the healthy and sustainable environment of modern civilization. Therefore, its detection and degradation are of paramount importance to the scientific community. In the present contribution, we have introduced a chromo-fluorogenic pyrene-based  probe, (E)-2-methoxy-3-(pyren-1-ylimino)-3,8a-dihydro-2H-chromen-4-ol (PMCO) to detect sarin stimulant diethylchlorophosphate (DCP) in solution and gaseous phases. On inserting DCP in PMCO solution, a visual colorimetric change from yellow to clear colourless in daylight and highly intensified blue fluorescence was observed instantly under a 365 nm portable UV lamp light. PMCO has outstanding selectivity and high sensitivity with a limit of detection of 1.32 µM in dimethyl sulfoxide (DMSO) medium and 77.5 nM in 20% H2O-DMSO. A handy strained paper strip-based experiment was demonstrated to recognize DCP in a mixture of similar toxic analytes. A dip-stick experiment was performed to identify DCP vapour, and may be used as an effective photonic tool. We also demonstrated real sample analysis utilizing different DCP-spiked water samples and validating DCP detection even in various types of soils such as sand, field, and mud. Therefore, this present study provides an effective chemosensor for instant and on-site detection of toxic nerve agents in dangerous circumstances.


Assuntos
Agentes Neurotóxicos , Compostos Organofosforados , Sarina , Sarina/análise , Agentes Neurotóxicos/análise , Corantes Fluorescentes , Dimetil Sulfóxido , Gases
4.
Plant Mol Biol ; 114(2): 35, 2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38587705

RESUMO

Fixing atmospheric nitrogen for use as fertilizer is a crucial process in promoting plant growth and enhancing crop yields in agricultural production. Currently, the chemical production of nitrogen fertilizer from atmospheric N2 relies on the energy-intensive Haber-Bosch process. Therefore, developing a low-cost and easily applicable method for fixing nitrogen from the air would provide a beneficial alternative. In this study, we tested the utilization of dinitrogen pentoxide (N2O5) gas, generated from oxygen and nitrogen present in ambient air with the help of a portable plasma device, as a nitrogen source for the model plant Arabidopsis thaliana. Nitrogen-deficient plants supplied with medium treated with N2O5, were able to overcome nitrogen deficiency, similar to those provided with medium containing a conventional nitrogen source. However, prolonged direct exposure of plants to N2O5 gas adversely affected their growth. Short-time exposure of plants to N2O5 gas mitigated its toxicity and was able to support growth. Moreover, when the exposure of N2O5 and the contact with plants were physically separated, plants cultured under nitrogen deficiency were able to grow. This study shows that N2O5 gas generated from atmospheric nitrogen can be used as an effective nutrient for plants, indicating its potential to serve as an alternative nitrogen fertilization method for promoting plant growth.


Assuntos
Arabidopsis , Gases , Nitrogênio , Fertilizantes , Oxigênio , Agricultura
5.
J Environ Manage ; 357: 120809, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38583382

RESUMO

Aerobic composting has been considered as a pragmatic technique to convert food waste digestate into high-quality biofertiliser. Nevertheless, massive gaseous emission and immature product remain the primary challenges in food waste digestate composting. Thus, the performance of multi-stage aeration regimes to improve gaseous emissions and organic humification during food waste digestate composting was investigated in this study. In addition to continuous aeration with a constant intensity of 0.3 L kg·dry mass (DM)-1·min-1, two multi-stage decreased aeration regimes were designed as "0.3-0.2-0.1" and "0.3-0.1-0.1" L·kg·DM-1·min-1 from the thermophilic to cooling and then mature stages, respectively. Results showed that the decreased aeration regimes could alleviate nitrous oxide (N2O) and ammonia (NH3) emission and slightly enhance humification during composting. The alleviated N2O and NH3 emission were mainly contributed by abiotically reducing gaseous release potential as well as biotically inactivating denitrifers (Pusillimonas and Pseudidiomarina) and proliferating Atopobium to reduce nitrate availability under lower aeration supply. The "0.3-0.2-0.1 L kg·DM-1·min-1" regime exhibited a more excellent performance to alleviate N2O and NH3 emission by 27.5% and 16.3%, respectively. Moreover, the decreased aeration regimes also favored the enrichment of functional bacteria (Caldicoprobacter and Syntrophomonas) to accelerate lignocellulosic biodegradation and thus humic acid synthesis by 6.5%-11.2%. Given its better performance to improve gaseous emissions and humification, the aeration regime of "0.3-0.2-0.1 L kg·DM-1·min-1" are recommended in food waste digestate composting in practice.


Assuntos
Compostagem , Eliminação de Resíduos , Eliminação de Resíduos/métodos , 60659 , Alimentos , Solo , Gases
6.
J Environ Manage ; 357: 120830, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38583383

RESUMO

Greenhouse gases (GHGs) emissions due to increasing energy demand have raised the need to identify effective solutions to produce clean and renewable energy. Biotechnologies are an effective platform to attain green transition objectives, especially when synergically integrated to promote health and environmental protection. In this context, microalgae-based biotechnologies are considered among the most effective tools for treating gaseous effluents and simultaneously capturing carbon sources for further biomass valorisation. The production of biodiesel is regarded as a promising avenue for harnessing value from residual algal biomass. Nonetheless, the existing techniques for extracting lipids still face certain limitations, primarily centred around the cost-effectiveness of the process.This study is dedicated to developing and optimising an innovative and cost-efficient technique for extracting lipids from algal biomass produced during gaseous emissions treatment based on algal-bacterial biotechnology. This integrated treatment technology combines a bio-scrubber for degrading gaseous contaminants and a photobioreactor for capturing the produced CO2 within valuable algal biomass. The cultivated biomass is then processed with the process newly designed to extract lipids simultaneously transesterificated in fatty acid methyl esters (FAME) via In Situ Transesterification (IST) with a Kumagawa-type extractor. The results of this study demonstrated the potential application of the optimised method to overcome the gap to green transition. Energy production was obtained from residuals produced during the necessary treatment of gaseous emissions. Using hexane-methanol (v/v = 19:1) mixture in the presence KOH in Kumagawa extractor lipids were extracted with extraction yield higher than 12% and converted in fatty acid methyl esters. The process showed the enhanced extraction of lipids converted in bio-sourced fuels with circular economy approach, broadening the applicability of biotechnologies as sustainable tools for energy source diversification.


Assuntos
Lipídeos , Microalgas , Biocombustíveis , Promoção da Saúde , Ácidos Graxos , Gases , Biomassa , Ésteres
7.
Int. microbiol ; 27(2): 607-614, Abr. 2024. ilus
Artigo em Inglês | IBECS | ID: ibc-232305

RESUMO

Wetlands are the main natural sources of methane emissions, which make up a significant portion of greenhouse gas emissions. Such wetland patches serve as rich habitats for aerobic methanotrophs. Limited knowledge of methanotrophs from tropical wetlands widens the scope of study from these habitats. In the present study, a freshwater wetland in a tropical region in India was sampled and serially diluted to obtain methanotrophs in culture. This was followed by the isolation of methanotrophs on agarose-containing plates, incubated under methane: air atmosphere. Methanotrophs are difficult to cultivate, and very few cultures of methanotrophs are available from tropical wetlands. Our current study reports the cultivation of a diverse community of methanotrophs from six genera, namely, Methylomonas, Methylococcus, Methylomagnum, Methylocucumis (type I methanotrophs) along with Methylocystis, Methylosinus (type II methanotrophs). A high abundance of methanotrophs (106–1010 methanotrophs/g fresh weight) was observed in the samples. A Methylococcus strain could represent a putative novel species that was also isolated. Cultures of Methylomagnum and Methylocucumis, two newly described type I methanotrophs exclusively found in rice fields, were obtained. A large number of Methylomonas koyamae strains were cultured. Our study is pioneering in the documentation of culturable methanotrophs from a typical tropical wetland patch. The isolated methanotrophs can act as models for studying methanotroph-based methane mitigation from wetland habitats and can be used for various mitigation and valorization applications. (AU)


Assuntos
Áreas Alagadas , Metano , Efeito Estufa , Gases , Ecossistema , Água Doce
8.
ACS Appl Mater Interfaces ; 16(15): 18564-18573, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38567738

RESUMO

Replicating the sense of smell presents an ongoing challenge in the development of biomimetic devices. Olfactory receptors exhibit remarkable discriminatory abilities, including the enantioselective detection of individual odorant molecules. Graphene has emerged as a promising material for biomimetic electronic devices due to its unique electrical properties and exceptional sensitivity. However, the efficient detection of nonpolar odor molecules using transistor-based graphene sensors in a gas phase in environmental conditions remains challenging due to high sensitivity to water vapor. This limitation has impeded the practical development of gas-phase graphene odor sensors capable of selective detection, particularly in humid environments. In this study, we address this challenge by introducing peptide-functionalized graphene sensors that effectively mitigate undesired responses to changes in humidity. Additionally, we demonstrate the significant role of humidity in facilitating the selective detection of odorant molecules by the peptides. These peptides, designed to mimic a fruit fly olfactory receptor, spontaneously assemble into a monomolecular layer on graphene, enabling precise and specific odorant detection. The developed sensors exhibit notable enantioselectivity, achieving a remarkable 35-fold signal contrast between d- and l-limonene. Furthermore, these sensors display distinct responses to various other biogenic volatile organic compounds, demonstrating their versatility as robust tools for odor detection. By acting as both a bioprobe and an electrical signal amplifier, the peptide layer represents a novel and effective strategy to achieve selective odorant detection under normal atmospheric conditions using graphene sensors. This study offers valuable insights into the development of practical odor-sensing technologies with potential applications in diverse fields.


Assuntos
Técnicas Biossensoriais , Grafite , Receptores Odorantes , Odorantes , Grafite/química , Gases , Estereoisomerismo , Receptores Odorantes/química , Peptídeos
9.
Sci Rep ; 14(1): 8756, 2024 04 16.
Artigo em Inglês | MEDLINE | ID: mdl-38627517

RESUMO

Although several occupational exposures have been linked to the risk of COPD; limited data exists on sex-specific differences. This study aimed to identify at-risk occupations and sex differences for COPD risk. Cases were identified in a large surveillance system established through the linkage of former compensation claimants' data (non-COPD claims) to physician visits, ambulatory care data, and hospital inpatient data (1983-2020). Cox proportional hazard models were used to estimate hazard ratios (HRs) and corresponding 95% confidence intervals (CI) for occupation groups (occupation at time of claim), stratified by sex. HRs were indirectly adjusted for cigarette smoking using another population dataset. A total of 29,445 male and 14,693 female incident cases of COPD were identified. Increased risks were observed in both sexes for construction (HRmale 1.15, 95% CI 1.12-1.19; HRfemale 1.54, 95% CI 1.29-1.83) transport/equipment operating (HRmale 1.32, 95% CI 1.28-1.37; HRfemale 1.53, 95% CI 1.40-1.68) farming (HRmale 1.23, 95% CI 1.15-1.32; HRfemale 1.19, 95% CI 1.04-1.37) and janitors/cleaners (HRmale 1.31, 95% CI 1.24-1.37; HRfemale 1.40, 95% CI 1.31-1.49). Increased risks were observed for females employed as chefs and cooks (HR 1.44, 95% CI 1.31-1.58), bartenders (HR 1.38, 95% CI 1.05-1.81), and those working in food/beverage preparation (HR 1.34, 95% CI 1.24-1.45) among other occupations. This study demonstrates elevated risk of COPD among both male and female workers potentially exposed to vapours, gases, dusts, and fumes, highlighting the need for occupational surveillance of COPD.


Assuntos
Doenças Profissionais , Exposição Ocupacional , Doença Pulmonar Obstrutiva Crônica , Humanos , Masculino , Feminino , Ontário/epidemiologia , Doenças Profissionais/epidemiologia , Doenças Profissionais/etiologia , Ocupações , Doença Pulmonar Obstrutiva Crônica/epidemiologia , Doença Pulmonar Obstrutiva Crônica/etiologia , Exposição Ocupacional/efeitos adversos , Gases , Fatores de Risco
10.
Molecules ; 29(7)2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38611786

RESUMO

Membrane-based sensors (MePSs) exhibit remarkable precision and sensitivity in detecting pressure changes. MePSs are commonly used to monitor catalytic reactions in solution, generating gas products crucial for signal amplification in bioassays. They also allow for catalyst quantification by indirectly measuring the pressure generated by the gaseous products. This is particularly interesting for detecting enzymes in biofluids associated with disease onset. To enhance the performance of a MePS, various structural factors influence membrane flexibility and response time, ultimately dictating the device's pressure sensitivity. In this study, we fabricated MePSs using polydimethylsiloxane (PDMS) and investigated how structural modifications affect the Young's modulus (E) and residual stress (σ0) of the membranes. These modifications have a direct impact on the sensors' sensitivity to pressure variations, observed as a function of the volume of the chamber (Σ) or of the mechanical properties of the membrane itself (S). MePSs exhibiting the highest sensitivities were then employed to detect catalyst quantities inducing the dismutation of hydrogen peroxide, producing dioxygen as a gaseous product. As a result, a catalase enzyme was successfully detected using these optimized MePSs, achieving a remarkable sensitivity of (22.7 ± 1.2) µm/nM and a limit of detection (LoD) of 396 pM.


Assuntos
Bioensaio , Gases , Catalase , Membranas , Catálise , Módulo de Elasticidade
11.
Sci Data ; 11(1): 329, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38570477

RESUMO

To achieve resource efficiency, and carbon neutrality, it is vital to evaluate nutrient supply and gaseous pollutant emissions associated with field management of bio-straw resources. Previous straw yield estimates have typically relied on a constant grain-to-straw yield ratio without accounting for grain yield levels in a given region. Addressing this high-resolution data gap, our study introduces a novel empirical model for quantifying grain-to-straw yield, which has been used to gauge wheat straw field management practices at the city level during 2011-2015. Utilizing both statistical review and GIS-based methods, average nitrogen (N), phosphorus (P), and potassium (K) supplies from straw field management stood at 1510, 1229, and 61700 tons, respectively. Average emissions of PM2.5, SO2, NOx, NH3, CH4, and CO2 due to straw burning were 367, 41, 160, 18, 165, and 70,644 tons, respectively. We also reported uncertainty from Monte Carlo model as the 5th-95th percentiles of estimated nutrient supply and gaseous pollutant. These insights will provide foundational support for the sustainable and environmentally friendly management of wheat straw in China.


Assuntos
Poluentes Atmosféricos , Poluentes Ambientais , Agricultura/métodos , Poluentes Atmosféricos/análise , China , Gases/análise , Solo , Triticum
12.
Waste Manag ; 178: 371-384, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38432182

RESUMO

As an important source of malodor, the odor gases emitted from public toilet significantly interfered the air quality of living surroundings, resulting in environmental problem which received little attention before. Thus, this paper explored the odor release pattern of latrine feces and deodorization effect with composited microbial agent in Chengdu, China. The odor release rules were investigated in sealed installations with a working volume of 9 L for 20 days. The odor units (OU), ammonia (NH3), hydrogen sulfide (H2S) and total volatile organic compounds (TVOC) were selected to assess the release of malodorous gases under different temperature and humidity, while the highest malodor release was observed under 45℃, with OU and TVOC concentration was 643.91 ± 2.49 and 7767.33 ± 33.50 mg/m3, respectively. Microbes with deodorization ability were screened and mixed into an agent, which composited of Bacillus amyloliquefaciens, Lactobacillus plantarum, Enterococcus faecalis and Pichia fermentans. The addition of microbial deodorant could significantly suppress the release of malodor gas during a 20-day trial, and the removal efficiency of NH3, H2S, TVOC and OU was 81.50 %, 38.31 %, 64.38 %, and 76.86 %, respectively. The analysis of microbial community structure showed that temperature was the main environmental factor driving the microbial variations in latrine feces, while Firmicutes, Actinobacteria, Proteobacteria and Bacteroidetes were the main bacteria phyla involved in the formation and emission of malodorous gases. However, after adding the deodorant, the abundance of Bacteroidetes, Proteobacteria and Actinobacteria were decreased, while the abundance of Firmicutes was increased. Furthermore, P. fermentans successfully colonized in fecal substrates and became the dominant fungus after deodorization. These results expanded the understanding of the odor release from latrine feces, and the composited microbial deodorant provided a valuable basis to the management of odor pollution.


Assuntos
Desodorantes , Sulfeto de Hidrogênio , Odorantes , Toaletes , Gases
13.
Waste Manag ; 178: 385-394, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38442668

RESUMO

The standing pouch, a packaging material made of multiple layers of plastic and metal, presents a significant challenge for full recycling. Gasification shows promise as a method to recover aluminum from this type of waste and convert it into energy. This study aims to evaluate the efficiency of gasification in treating aluminum-containing plastic packages, and recovering aluminum while identifying the optimal combinations of temperature and equivalence ratio (ER) to achieve the best outcomes. The study achieved a conversion rate of 43.06 wt% to 69.42 wt% of the original waste mass into syngas, with aluminum recovery rates ranging from 35.2 % to 65.3 %. Temperature and ER alterations affected the product distribution, aluminum recovery rate, and aluminum partitioning in the products. The results indicated that the combination of 700 °C, ER = 0.4 would provide the largest amount of syngas about 69.42 %, which is the main product of the gasification process, and therefore, this combination is the most optimal for syngas-yielding purposes. Under the reclaiming aluminum is more prioritized, the combination of 800 °C, ER = 0.6 would be the most optimal condition, the majority of Al in fuel was found in char and fly ash were 67.5 % and 4.81 %, respectively. The study focused on the partitioning of aluminum during the gasification process, which was observed to mainly exist in the form of Al2O3(s), with gaseous species including AlCl3(g), AlH(g), and Al2O(g) due to their medium volatility. As the ER increased, the amount of O2 also increased, leading to more Al2O3(s) formation. In conclusion, this research provides a foundation for further exploration of gasification as a means of energy conversion and metal recovery.


Assuntos
Eliminação de Resíduos , Eliminação de Resíduos/métodos , Alumínio , Gases , Temperatura , Metais
14.
Sci Rep ; 14(1): 6646, 2024 03 19.
Artigo em Inglês | MEDLINE | ID: mdl-38503831

RESUMO

Nicotine use is a leading cause of preventable deaths worldwide, and most of those who attempt to quit will relapse. While electronic cigarettes and other electronic nicotine delivery systems (ENDS) were presented as a safer alternative to traditional cigarettes and promoted as devices to help traditional tobacco smokers reduce or quit smoking, they have instead contributed to increasing nicotine use among youths. Despite this, ENDS also represent a useful tool to create novel preclinical animal models of nicotine exposure that more accurately represent human nicotine use. In this study, we validated a chronic, intermittent, ENDS-based passive vapor exposure model in mice, and then measured changes in multiple behaviors related to nicotine abstinence. First, we performed a behavioral dose curve to investigate the effects of different nicotine inter-vape intervals on various measures including body weight, locomotor activity, and pain hypersensitivity. Next, we performed a pharmacokinetic study to measure plasma levels of nicotine and cotinine following chronic exposure for each inter-vape interval. Finally, we utilized a behavior test battery at a single dosing regimen that produces blood levels equivalent to human smokers in order to characterize the effects of chronic nicotine, vehicle, or passive airflow and identified nicotine-induced impairments in cognitive behavior.


Assuntos
Sistemas Eletrônicos de Liberação de Nicotina , Nicotina , Adolescente , Masculino , Humanos , Camundongos , Animais , Fumar , Cotinina , Gases , Cognição
15.
J Chromatogr A ; 1720: 464798, 2024 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-38502990

RESUMO

We present a new chromatogram decomposition method for Gas Chromatography (GC) which represents a chromatogram as a sum of template functions inspired by the analytic solution of mass balance equation. The proposed method starts by approximating GC response of a single gas by these template functions. Consequently, it utilizes the temporal translation and dilation of this approximate response to approximate GC responses of other gases of interest. The results are demonstrated on lab data using calibration bottles containing mixtures of C1-C5. Correlation of the amplitudes of the decomposed responses and injected concentrations indicates linear calibration curves are sufficient to estimate C1-C5 concentrations. The performance of the method is demonstrated by a ratio test where a calibration bottle with C1 concentration 300 times larger than C2 and C3 concentrations is injected into GC.


Assuntos
Gases , Calibragem , Cromatografia Gasosa/métodos , Gases/análise
16.
Nat Commun ; 15(1): 2732, 2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38548760

RESUMO

Fe‒S cluster-harboring enzymes, such as carbon monoxide dehydrogenases (CODH), employ sophisticated artificial electron mediators like viologens to serve as potent biocatalysts capable of cleaning-up industrial off-gases at stunning reaction rates. Unraveling the interplay between these enzymes and their associated mediators is essential for improving the efficiency of CODHs. Here we show the electron mediator-interaction site on ChCODHs (Ch, Carboxydothermus hydrogenoformans) using a systematic approach that leverages the viologen-reactive characteristics of superficial aromatic residues. By enhancing mediator-interaction (R57G/N59L) near the D-cluster, the strategically tailored variants exhibit a ten-fold increase in ethyl viologen affinity relative to the wild-type without sacrificing the turn-over rate (kcat). Viologen-complexed structures reveal the pivotal positions of surface phenylalanine residues, serving as external conduits for the D-cluster to/from viologen. One variant (R57G/N59L/A559W) can treat a broad spectrum of waste gases (from steel-process and plastic-gasification) containing O2. Decoding mediator interactions will facilitate the development of industrially high-efficient biocatalysts encompassing gas-utilizing enzymes.


Assuntos
Elétrons , Complexos Multienzimáticos , Complexos Multienzimáticos/química , Aldeído Oxirredutases/genética , Aldeído Oxirredutases/química , Gases , Viologênios , Monóxido de Carbono/química
17.
J Am Soc Mass Spectrom ; 35(4): 784-792, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38489759

RESUMO

We previously discovered that electron attachment to gaseous peptide anions can occur within a relatively narrow electron energy range. The resulting charge-increased radical ions undergo dissociation analogous to conventional cation electron capture/transfer dissociation (ECD/ETD), thus enabling a novel tandem mass spectrometry (MS/MS) technique that we termed negative ion electron capture dissociation (niECD). We proposed that gaseous zwitterionic structures are required for niECD with electron capture either occurring at or being directed by a positively charged site. Here, we further evaluate this zwitterion mechanism by performing niECD of peptides derivatized to alter their ability to form zwitterionic gaseous structures. Introduction of a fixed positive charge tag, a highly basic guanidino group, or a highly acidic sulfonate group to promote zwitterionic structures in singly charged anions, rescued the niECD ability of a peptide refractory to niECD in its unmodified form. We also performed a systematic study of five sets of synthetic peptides with decreasing zwitterion propensity and found that niECD efficiency decreased accordingly, further supporting the zwitterion mechanism. However, traveling-wave ion mobility-mass spectrometry experiments, performed to gain further insight into the gas-phase structures of peptides showing high niECD efficiency, exhibited an inverse correlation between the orientationally averaged collision cross sections and niECD efficiency. These results indicate that compact salt-bridged structures are also a requirement for effective niECD.


Assuntos
Gases , Espectrometria de Massas em Tandem , Gases/química , Espectrometria de Massas em Tandem/métodos , Elétrons , Ânions/química , Peptídeos/química , Cátions , Cloreto de Sódio
18.
Bioresour Technol ; 399: 130557, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38460561

RESUMO

A novel cascade pyrolysis upgrading process for acid hydrolysis lignin (AHL), consisting of pyrolysis, catalytic upgrading of pyrolysis vapors, and pyrolysis char, was developed to improve the yield of value-added products (monophenolic chemicals and carbon materials). Pyrolysis of AHL at 450 °C and subsequent catalytic upgrading of pyrolysis vapors over Ni/H-ZSM-5 boosted the concentration of monophenolic chemicals in pyrolysis liquids by 58%. The carbon material prepared from pyrolysis char using KOH as activating agent exhibited a large specific surface area of 2902.5 m2/g and a large total pore volume of 1.45 cm3/g, thus affording good adsorption capacity for methylene blue (824.87 mg/g) and iodine (2333.17 mg/g). Moreover, the cascade pyrolysis upgrading of AHL achieved a yield of 68.52% desired products, which was much higher than the reported results (single production of monophenols and pyrolysis char). In summary, this work provides a potential reference for efficient utilization of lignin in large-scale applications.


Assuntos
Carbono , Lignina , Pirólise , Adsorção , Hidrólise , Gases , Ácidos
19.
Astrobiology ; 24(4): 343-370, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38452176

RESUMO

Long-standing unexplained Venus atmosphere observations and chemical anomalies point to unknown chemistry but also leave room for the possibility of life. The unexplained observations include several gases out of thermodynamic equilibrium (e.g., tens of ppm O2, the possible presence of PH3 and NH3, SO2 and H2O vertical abundance profiles), an unknown composition of large, lower cloud particles, and the "unknown absorber(s)." Here we first review relevant properties of the venusian atmosphere and then describe the atmospheric chemical anomalies and how they motivate future astrobiology missions to Venus.


Assuntos
Vênus , Exobiologia , Meio Ambiente Extraterreno , Gases/química , Atmosfera/química
20.
Sensors (Basel) ; 24(5)2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38475164

RESUMO

In areas where livestock are bred, there is a demand for accurate, real-time, and stable monitoring of ammonia concentration in the breeding environment. However, existing electronic nose systems have slow response times and limited detection accuracy. In this study, we introduce a novel solution: the bionic chamber construction of the electronic nose is optimized, and the sensor response data in the chamber are analyzed using an intelligent algorithm. We analyze the structure of the biomimetic chamber and the surface airflow of the sensor array to determine the sensing units of the system. The system employs an electronic nose to detect ammonia and ethanol gases in a circulating airflow within a closed box. The captured signals are processed, followed by the application of classification and regression models for data prediction. Our results suggest that the system, leveraging the biomimetic chamber, offers rapid gas detection response times. A high classification prediction accuracy, with a determination coefficient R2 value of 0.99 for single-output regression and over 0.98 for multi-output regression predictions, is achieved by incorporating a backpropagation (BP) neural network algorithm. These outcomes demonstrate the effectiveness of the electronic nose, based on an optimized bionic chamber combined with a BP neural network algorithm, in accurately detecting ammonia emitted during livestock excreta fermentation, satisfying the ammonia detection requirements of breeding farms.


Assuntos
Amônia , Gado , Animais , Biônica , Nariz Eletrônico , Fermentação , Gases
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