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1.
Environ Sci Technol ; 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39291786

RESUMO

Exposure to the indoor airborne microbiome is closely related to the air that individuals breathe. However, the floor dust-borne microbiome is commonly used as a proxy for indoor airborne microbiome, and the spatial distribution of indoor airborne microbiome is less well understood. This study aimed to characterize indoor airborne microorganisms at varying heights and compare them with those in floor dust. An assembly of three horizontally and three vertically positioned Petri dishes coated with mineral oil was applied for passive air sampling continuously at three heights without interruption. The airborne microbiomes at the three different heights showed slight stratification and differed significantly from those found in the floor dust. Based on the apportionment results from the fast expectation-maximization algorithm (FEAST), shoe sole dust contributed approximately 4% to indoor airborne bacteria and 14% to airborne fungi, a contribution that is comparable to that from the floor dust-borne microbiome. The results indicated that floor dust may not be a reliable proxy for indoor airborne microbiome. Moreover, the study highlights the need for height-resolved studies of indoor airborne microbiomes among humans in different activity modes and life states. Additionally, shoe sole-dust-associated microorganisms could potentially be a source to "re-wild" the indoor microbiota.

3.
Environ Sci Technol ; 58(32): 14329-14337, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39088742

RESUMO

A series of Mn and Fe metal oxide catalysts loaded onto USY, as well as single metal oxides, were prepared and characterized. The effects of interactions between the catalytic components and the introduction of gas phase NO on the catalytic ozonation of toluene were investigated. Characterization showed that there existed strong interactions between MnOx, FeOx, and USY, which enhanced the content of oxygen vacancies and acid sites of the catalysts and thus boosted the generation of reactive oxygen species and the adsorption of toluene. The MnFeOx-USY catalyst with MnOx and FeOx dimetallic oxides exhibited the most excellent performance of catalytic ozonation of toluene. On the other hand, the presence of NOx in reaction gas mixtures significantly promoted both toluene conversion and mineralization, which was attributed to the formation of nitrate species on the catalysts surface and thus the increase of both acid sites and toluene oxidation sites. Meanwhile, the reaction mechanism between O3 and C7H8 was modified in which the strong interactions between MnOx, FeOx, and USY accelerated the reaction progress based on the L-H route. In addition, the formation of the surface nitrate species not only promoted reaction progress following the L-H route but also resulted in the occurrence of the reaction via the E-R route.


Assuntos
Ozônio , Tolueno , Tolueno/química , Catálise , Ozônio/química , Compostos Férricos/química , Manganês/química , Gases/química , Óxidos/química , Óxidos de Nitrogênio/química , Oxirredução
4.
Environ Sci Technol ; 58(27): 12091-12100, 2024 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-38916160

RESUMO

The widespread ozone (O3) pollution is extremely hazardous to human health and ecosystems. Catalytic decomposition into O2 is the most promising method to eliminate ambient O3, while the fast deactivation of catalysts under humid conditions remains the primary challenge for their application. Herein, we elaborately developed a splendidly active and stable Mn-based catalyst with double hydrophobic protection of active carbon (AC) and CeO2 (CeMn@AC), which possessed abundant interfacial oxygen vacancies and excellent desorption of peroxide intermediates (O22-). Under extremely humid (RH = 90%) conditions and a high space velocity of 1200 L h-1 g-1, the optimized CeMn@AC achieved nearly 100% O3 conversion (140 h) at 5 ppm, showing unprecedented catalytic activity and moisture resistance toward O3 decomposition. In situ DRIFTS and theory calculations confirmed that the exceptional moisture resistance of CeMn@AC was ascribed to the double protection effect of AC and CeO2, which cooperatively prevented the competitive adsorption of H2O molecules and their accumulation on the active sites of MnO2. AC provided a hydrophobic reaction environment, and CeO2 further alleviated moisture deterioration of the MnO2 particles exposed on the catalyst surface via the moisture-resistant oxygen vacancies of MnO2-CeO2 crystal boundaries. This work offers a simple and efficient strategy for designing moisture-resistant materials and facilitates the practical application of the O3 decomposition catalysts in various environments.


Assuntos
Ozônio , Ozônio/química , Catálise , Carbono/química , Compostos de Manganês/química , Cério/química , Óxidos/química
5.
Nat Commun ; 15(1): 3592, 2024 Apr 27.
Artigo em Inglês | MEDLINE | ID: mdl-38678057

RESUMO

Supported nanoclusters (SNCs) with distinct geometric and electronic structures have garnered significant attention in the field of heterogeneous catalysis. However, their directed synthesis remains a challenge due to limited efficient approaches. This study presents a plasma-assisted treatment strategy to achieve supported metal oxide nanoclusters from a rapid transformation of monomeric dispersed metal oxides. As a case study, oligomeric vanadia-dominated surface sites were derived from the classic supported V2O5-WO3/TiO2 (VWT) catalyst and showed nearly an order of magnitude increase in turnover frequency (TOF) value via an H2-plasma treatment for selective catalytic reduction of NO with NH3. Such oligomeric surface VOx sites were not only successfully observed and firstly distinguished from WOx and TiO2 by advanced electron microscopy, but also facilitated the generation of surface amide and nitrates intermediates that enable barrier-less steps in the SCR reaction as observed by modulation excitation spectroscopy technologies and predicted DFT calculations.

6.
Andrology ; 2024 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-38436126

RESUMO

BACKGROUND: Since the outbreak of coronavirus disease 2019, it has had a serious impact on people's physical and mental health. However, in our clinical work, we have found that the erectile function of coronavirus disease 2019 patients with neurological decline was often seriously affected. OBJECTIVES: To further explore the relationship between erectile dysfunction and neurological dysfunction caused by coronavirus disease 2019. MATERIALS AND METHODS: We conducted a survey from August 2022 to February 2023 at the First Affiliated Hospital of Anhui Medical University and the Third People's Hospital of Linyi City. A total of 251 subjects with a history of coronavirus disease 2019 infection were included. Symptoms and changes in erectile function after the coronavirus disease 2019 infection were collected and assessed using the International Index of Erectile Function-5 scale and several targeted questions. RESULTS: In this study, we found that in patients infected with novel coronavirus, the proportion of erectile dysfunction was higher in those with neurological manifestations such as olfactory and taste impairment or psychological symptoms such as anxiety. DISCUSSION: We found that neurological decline and psychological factors were independent and significant risk factors for erectile dysfunction caused by coronavirus disease 2019. CONCLUSION: Patients with neurological damage or psychiatric symptoms are more likely to have erectile dysfunction, suggesting that the 2019 novel coronavirus may affect erectile function by damaging nerves. This provides a new insight into the mechanism of erectile dysfunction.

7.
World J Mens Health ; 2024 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-38311371

RESUMO

PURPOSE: Explore the causal relationship between the gut microbiota and erectile dysfunction (ED) at phylum, class, order, family, and genus levels, and identify specific pathogenic bacteria that may be associated with the onset and progression of ED. MATERIALS AND METHODS: The genetic variation data of 196 human gut microbiota incorporated in our study came from the human gut microbiome Genome Wide Association Studies (GWAS) dataset released by the MiBioGen Consortium. The GWAS statistics for ED were extracted from one study by Bovijn et al., which included 223,805 participants of European ancestry, of whom 6,175 were diagnosed with ED. Subsequently, Mendelian randomization (MR) analysis was carried out to explore whether a causal relationship exists between the gut microbiota and ED. Additionally, bidirectional MR analysis was performed to examine the directionality of the causal relationship. RESULTS: Through MR analysis, we found that family Lachnospiraceae (odds ratio [OR]: 1.27, 95% confidence interval [CI]: 1.05-1.52, p=0.01) and its subclass genus LachnospiraceaeNC2004 group (OR: 1.17, 95% CI: 1.01-1.37, p=0.04) are associated with a higher risk of ED. In addition, genus Oscillibacter (OR: 1.17, 95% CI: 1.02-1.35, p=0.03), genus Senegalimassilia (OR: 1.32, 95% CI: 1.06-1.64, p=0.01) and genus Tyzzerella3 (OR: 1.14, 95% CI: 1.02-1.27, p=0.02) also increase the risk of ED. In contrast, the inverse variance weighted estimate of genus RuminococcaceaeUCG013 (OR: 0.77, 95% CI: 0.61-0.96, p=0.02) suggests that it has a protective effect against the occurrence of ED. CONCLUSIONS: This study preliminarily identified 6 bacterial taxa that may have a causal relationship with ED, including family Lachnospiraceae, genus Lachnospiraceae NC2004 group, Oscillibacter, Senegalimassilia, Tyzzerella 3 and Ruminococcaceae UCG013. These identified important bacterial taxa may serve as candidates for microbiome intervention in future ED clinical trials.

8.
Environ Sci Technol ; 57(48): 20053-20063, 2023 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-37936384

RESUMO

Modulating oxygen vacancies of catalysts through crystal facet engineering is an innovative strategy for boosting the activity for ozonation of catalytic volatile organic compounds (VOCs). In this work, three kinds of facet-engineered monoclinic NiO catalysts were successfully prepared and utilized for catalytic toluene ozonation (CTO). Density functional theory calculations revealed that Ni vacancies were more likely to form preferentially than O vacancies on the (110), (100), and (111) facets of monoclinic NiO due to the stronger Ni-vacancy formation ability, further affecting O-vacancy formation. Extensive characterizations demonstrated that Ni vacancies significantly promoted the formation of O vacancies and thus reactive oxygen species in the (111) facet of monoclinic NiO, among the three facets. The performance evaluation showed that the monoclinic NiO catalyst with a dominant (111) facet exhibits excellent performance for CTO, achieving a toluene conversion of ∼100% at 30 °C after reaction for 120 min under 30 ppm toluene, 210 ppm ozone, 45% relative humidity, and a space velocity of 120 000 h-1. This outperformed the previously reported noble/non-noble metal oxide catalysts used for CTO at room temperature. This study provided novel insight into the development of highly efficient facet-engineered catalysts for the elimination of catalytic VOCs.


Assuntos
Ozônio , Compostos Orgânicos Voláteis , Tolueno/química , Óxidos , Oxigênio , Catálise
9.
Angew Chem Int Ed Engl ; 62(43): e202313099, 2023 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-37694769

RESUMO

The development of practical materials for (de)hydrogenation reactions is a prerequisite for the launch of a sustainable hydrogen economy. Herein, we present the design and construction of an atomically dispersed dual-metal site Co/Cu-N-C catalyst allowing significantly improved dehydrogenation of formic acid, which is available from carbon dioxide and green hydrogen. The active catalyst centers consist of specific CoCuN6 moieties with double-N-bridged adjacent metal-N4 clusters decorated on a nitrogen-doped carbon support. At optimal conditions the dehydrogenation performance of the nanostructured material (mass activity 77.7 L ⋅ gmetal -1 ⋅ h-1 ) is up to 40 times higher compared to commercial 5 % Pd/C. In situ spectroscopic and kinetic isotope effect experiments indicate that Co/Cu-N-C promoted formic acid dehydrogenation follows the so-called formate pathway with the C-H dissociation of HCOO* as the rate-determining step. Theoretical calculations reveal that Cu in the CoCuN6 moiety synergistically contributes to the adsorption of intermediate HCOO* and raises the d-band center of Co to favor HCOO* activation and thereby lower the reaction energy barrier.

10.
Basic Clin Androl ; 33(1): 7, 2023 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-37046205

RESUMO

BACKGROUND: We investigated the association between premature ejaculation (PE) and the quality of residential environment from a new perspective to explore the influencing factors of PE, especially in four PE subtypes. We selected 499 adult males to participate in this study from September 2021 to September 2022. The satisfaction of residential environment was assessed by the Perceived Residential Environment Quality Indicators (PREQIs) scale, the control ability over ejaculation was assessed using the premature ejaculation diagnostic tool (PEDT), and their depression was assessed using the self-rating depression scale (SDS). RESULTS: The Architectural and Town-planning Spaces (ATS), Green Spaces (GS), and Commercial Services (CS) of PE patients (N = 346) were compared with those of control group (N = 153), showed a significant difference (p < .05), for PE patients, the score of ATS was 44.30 ± 12.38, the score of GS was 18.60 ± 6.24, and the score of CS was 20.82 ± 8.20; for control group, which were 40.46 ± 16.21, 20.69 ± 5.71 and 22.90 ± 7.03 respectively. After age was taken into account, ATS had a positive correlation with PEDT score (r = 0.76), whereas GS and CS had a negative correlation (r = -0.87, -0.90); ATS had a positive correlation with SDS (r = 0.96), whereas GS and CS had a negative correlation (r = -0.74, -0.81). CONCLUSIONS: We discovered that PE patients more likely resided in high-density areas with little green space and subpar commercial services, which might have an adverse effect on their mental health. This study offered a new viewpoint about the influence of residential environment on PE.


RéSUMé: CONTEXTE: Nous avons étudié l'association entre éjaculation précoce (PE) et qualité de l'environnement résidentiel sous un nouvel angle pour explorer les facteurs d'influence de la PE, en particulier dans quatre sous-types de PE. Nous avons sélectionné 499 hommes adultes pour participer à cette étude de septembre 2021 à septembre 2022. La satisfaction de l'environnement résidentiel a été évaluée par l'échelle des indicateurs de qualité perçue de l'environnement résidentiel (PREQI), la capacité de contrôle de l'éjaculation a été évaluée à l'aide de l'outil de diagnostic de la PE (PEDT) et leur dépression à l'aide de l'échelle d'auto-évaluation de la dépression (SDS). RéSULTATS: Les espaces architecturaux et urbanistiques (ATS), les espaces verts (GS) et les services commerciaux (CS) des patients atteints de PE (n = 346) ont été comparés à ceux du groupe témoin (n = 153). Ils ont montré une différence significative (p<,05) ; pour les patients PE, le score de l'ATS était de 44,30±12,38, le score de GS de 18,60±6,24 et le score de CS de 20,82±8,20 ; pour le groupe témoin, ces scores étaient respectivement de 40,46±16,21, 20,69±5,71 et 22,90±7,03. Une fois l'âge pris en compte, l'ATS avait une corrélation positive avec le score PEDT (r = 0,76), tandis que GS et CS avaient une corrélation négative (r = -0,87, -0,90) ; l'ATS avait une corrélation positive avec SDS (r = 0,96), tandis que GS et CS avaient une corrélation négative (r = -0,74, -0,81). CONCLUSIONS: Nous avons découvert que les patients atteints de PE résidaient plutôt dans des zones à forte densité avec peu d'espaces verts et des services commerciaux médiocres, ce qui pourrait avoir un effet néfaste sur leur santé mentale. Cette étude a offert un nouveau point de vue sur l'influence de l'environnement résidentiel sur la PE.

11.
Andrology ; 11(6): 1175-1187, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-36746766

RESUMO

BACKGROUND: Recently, dapoxetine has been widely accepted to treat premature ejaculation by fast-inhibiting 5-hydroxytryptamine reuptake. However, dapoxetine is not suitable for all premature ejaculation patients in clinical treatment. We need to investigate and reveal the mechanism deeply to solve this problem. OBJECTIVES: To investigate and reveal the function of dopamine D4 receptor in dapoxetine medicated premature ejaculation treatment. MATERIALS AND METHODS: A rat model was used to screen rapid ejaculators. The molecular mechanisms of histone serotonylation-mediated regulation of dopamine D4 receptor were demonstrated by chromatin immunoprecipitation, DNA pull-down, mass spectrometry analysis, and coimmunoprecipitation experiments. The biological function of dopamine D4 receptor was investigated through in vivo experiments by intrathecal injection of shDRD4 to knockdown dopamine D4 receptor. RESULTS: In this study, we found that dapoxetine increased expression of 5-hydroxytryptamine and dopamine D4 receptor. We demonstrated that dapoxetine increased levels of 5-hydroxytryptamine, which promoted histone serotonylation (H3K4me3Q5ser) and transcription factor myeloid zinc-finger 1 complex binding on the dopamine D4 receptor promoter, upregulated the expression of dopamine D4 receptor and thus delayed ejaculation. DISCUSSION: In this study, we demonstrated that dapoxetine increased the levels of 5-hydroxytryptamine, which promoted histone serotonylation and myeloid zinc-finger 1 complex binding to the dopamine D4 receptor promoter and upregulated the expression of dopamine D4 receptor, thus delaying ejaculation. CONCLUSION: It is a novel mechanism that dapoxetine take effect of premature ejaculation treatment through upregulating the dopamine D4 receptor, which indicated that upregulated dopamine D4 receptor would enhance the dapoxetine effect in premature ejaculation treatment. This may lead to the development of novel therapeutic interventions for premature ejaculation.


Assuntos
Ejaculação Precoce , Masculino , Humanos , Ratos , Animais , Ejaculação Precoce/tratamento farmacológico , Histonas , Receptores de Dopamina D4/genética , Serotonina , Inibidores Seletivos de Recaptação de Serotonina/farmacologia , Inibidores Seletivos de Recaptação de Serotonina/uso terapêutico , Resultado do Tratamento , Ejaculação , Benzilaminas/farmacologia , Benzilaminas/uso terapêutico , Zinco/farmacologia , Zinco/uso terapêutico
12.
J Hazard Mater ; 448: 130900, 2023 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36731324

RESUMO

Although free hydroxyl radical (·OH) generated on OMS-2-based catalysts during the catalytic ozonation process have been shown as important reactive oxygen species (ROSs) for toluene degradation, improvement of surface ·OH formation ability remains challenging. Here, Na, K, Rb, and Cs-OMS-2-SO42-/ZSM-5 catalysts were prepared, characterized and evaluated for catalytic ozonation of toluene. Both characterizations and DFT calculations showed that the appropriate alkali metal introduction made the catalyst possess with appropriate crystalline, reducibility, and acidity, which was favorable for catalytic ozonation of toluene. Characterizations also showed that alkali metal introduction resulted in water molecule adsorption on Brönsted acid sites of the catalysts, which made water molecule activation by ozone to form ·OH more easily. The introduction of K+ content of ∼ 5.9 wt% yielded K-OMS-2-SO42-/ZSM-5 catalyst with the highest Brönsted acid sites and thus formed the most ·OH among the five prepared catalysts. As a result, the catalyst exhibited excellent toluene conversion and COx selectivity for catalytic ozonation of toluene at room temperature and ambient humidity. Furthermore, the catalytic activity of deactivated K-OMS-2-SO42-/ZSM-5 catalyst was recovered after regeneration by a combination of water washing and heat treatment. Finally, a complete mechanism for toluene catalytic ozonation, catalyst deactivation, and regeneration was proposed.

13.
Mol Biol Rep ; 50(4): 3515-3523, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36787051

RESUMO

BACKGROUND: There are several investigations that have revealed that cerebral dopamine (DA) plays a pivotal role in the occurrence of premature ejaculation (PE). Although tyrosine hydroxylase (TH) is an essential enzyme for the synthesis of DA, only few investigations have described the role of TH in regulation mechanisms for ejaculation till now. To investigate whether there is a correlation between TH expression level in the brain and different ejaculation behavior in rats. Then explore whether the TH expression in the brain will change after acute dapoxetine treatment in rats with Rapid ejaculation. METHODS AND RESULTS: Rats (male, S-D rats, 6-8 weeks) were separated into three groups based on their ejaculation frequency: Rapid, Normal, and Sluggish. Expression level of DA in the brain was determined by enzyme-linked immune sorbent assay (ELISA) kit, TH expression level in the brain was determined by immunohistochemistry and Western Blot (WB) techniques. Among the three groups, DA and TH expression level were the highest in the Rapid ejaculation group, while the lowest was the Sluggish ejaculation group. The results also showed that TH level was positively associated with ejaculation frequency (r = 0.8038, P < 0.001) and negatively associated with ejaculation latency (r=-0.6199, P = 0.018). Furthermore, acute dapoxetine therapy in rats with Rapid ejaculation downregulated TH level in the brain. CONCLUSION: Changes in ejaculation behavior were significantly linked with TH level. Upregulated TH in selected brain regions related with ejaculation could cause rapid ejaculation. The effect of dapoxetine in prolonging ejaculation could be related to TH downregulation within the brain.


Assuntos
Ejaculação Precoce , Humanos , Masculino , Ratos , Animais , Ejaculação Precoce/tratamento farmacológico , Tirosina 3-Mono-Oxigenase , Resultado do Tratamento , Inibidores Seletivos de Recaptação de Serotonina
14.
J Hazard Mater ; 441: 129894, 2023 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-36087534

RESUMO

The commercial V2O5 -WO3/TiO2 (VWTi) catalysts often suffer from a serious joint deactivation by multiple heavy metals in the flue gas for NOx removal by NH3-SCR. Herein, we report an extraordinary deactivation offset effect between Zn and As on VWTi with alleviation of the toxic effects of the heavy metals by "like cures like". With the As&Zn content of 4 wt%, VWTi-As&Zn exhibited over 97% NO conversion under a GHSV of 100,000 h-1 and good SO2/H2O tolerance (> 93% NO conversion). It's presented 85% of fresh VWTi, exceeding those of VWTi-Zn (15%) by 5.6-fold and VWTi-As (70%) by 1.2-fold. Structure analysis showed that, unlike VWTi-As and VWTi-Zn, the VO vibration and dispersion state of VOx sites over VWTi-As&Zn were hardly affected. Moreover, VWTi-As&Zn possessed both the Lewis and Brønsted acid sites while VWTi-Zn and VWTi-As had only one type of them. The operando infrared/Raman/UV-vis spectroscopy and DFT calculations verified that the less affected VOx sites mainly reflected in three aspects: 1) the electron interaction between As and Zn; 2) the active VO Lewis acid sites; 3) lower energy barrier for N - H bond breaking. The "like cures like" phenomenon may open up an innovative pathway for the control of hazardous heavy metals.

15.
Chemosphere ; 315: 137679, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36586443

RESUMO

The heat desorption of styrene from adsorbents is impracticable owing to its spontaneous polymerization under heating conditions. However, the feature also brings a potential promoting effect on styrene adsorption. Therefore, it is expected to develop the non-regenerative adsorbents with large adsorption capacity by strengthening the polymerization effect. In this work, C-Cl grafted silica gel adsorbents were prepared by introducing (Chloromethyl)dimethylchlorosilane (CMDMCS) and FeCl2 into silica gel. The C-Cl grafted silica gel exhibited excellent styrene adsorption performance, its adsorption amounts for styrene were 4.67 times and 9 times of unmodified silica gel under dry air condition and high humidity condition (RH = 80%), respectively. In addition, the adsorption of styrene on C-Cl grafted silica gel was almost unaffected by the presence of toluene. The characterization of adsorbents after styrene adsorption indicated that the improvement of adsorption capacity of C-Cl grafted silica gel for styrene can be attributed to atom transfer radical polymerization (ATRP) of styrene molecules on modified silica gel during adsorption process.


Assuntos
Estireno , Tolueno , Sílica Gel , Adsorção , Dióxido de Silício
16.
RSC Adv ; 12(41): 26834-26845, 2022 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-36320860

RESUMO

Mesoporous and dispersed MnAl-based mixed metal oxide catalysts (Mn x AlO) were fabricated via the calcination of layered double hydroxide (LDH) precursors prepared by the coprecipitation method. Their physiochemical properties were characterized and their catalytic activities for ozone decomposition were evaluated. The results indicate that the prepared Mn x AlO catalysts have excellent catalytic activity owing to their large specific surface area, abundant surface oxygen vacancies and lower average Mn oxidation states. The Mn/Al atomic ratio and calcination temperature are found to significantly affect the textural properties and catalytic activity for ozone decomposition. The Mn2AlO-400 catalyst (Mn/Al = 2, calcined at 400 °C) exhibited 84.8% ozone conversion after 8 h reaction under an initial ozone concentration of 45 ± 2 ppm, 30 ± 1 °C, a relative humidity of 50% ± 3%, and a space velocity of 550 000 h-1. The results also show that the catalytic activity of Mn2AlO-400, which was deactivated owing to the accumulation of oxygen-related intermediates, was recovered by calcination at 400 °C under a N2 atmosphere for 1 h. A possible reason for catalyst deactivation and regeneration is proposed. This work provides a facile method for fabricating Mn x AlO catalysts with excellent characteristics to achieve better catalytic activity, which are promising candidates for practical ozone decomposition.

17.
Environ Sci Technol ; 56(22): 15695-15704, 2022 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-36259958

RESUMO

Mn-based catalysts hold the promise of practical applications in catalytic ozonation of toluene at room temperature, yet improvement of toluene conversion and COx selectivity remains challenging. Here, an innovative α-MnO2/ZSM-5 catalyst modified with SO42- was successfully prepared, and both characterizations and density functional theory (DFT) calculations showed that SO42- introduction facilitated the formation of oxygen vacancies, Lewis and Brönsted acid sites, and active oxygen species and enhanced the adsorption ability of toluene on α-MnO2/ZSM-5. Characterizations also showed that SO42- introduction made the catalyst possess larger specific surface area, superior reducibility, and stronger surface acidity. As a result, α-MnO2/ZSM-5 with a S/Mn molar ratio of 0.019 exhibited the best toluene conversion and COx selectivity, 87 and 94%, respectively, after the reaction for 8 h at 30 °C under an initial concentration of 5 ppm toluene and 45 ppm ozone, relative humidity of 45%, and space velocity of 32,000 h-1, far superior to those of non-noble catalysts reported to date under comparable reaction conditions. The synergistic role of increased oxygen vacancies and acid sites of α-MnO2/ZSM-5 modified with SO42- resulted in excellent toluene conversion and COx selectivity. The findings represented a critical step toward the rational design and synthesis of highly efficient catalysts for catalytic ozonation of toluene.

18.
Environ Sci Technol ; 56(17): 12625-12634, 2022 09 06.
Artigo em Inglês | MEDLINE | ID: mdl-35947769

RESUMO

Regeneration of spent V2O5-WO3/TiO2 catalysts is highly desirable, especially for those containing hypertoxic As, which is categorized as hazardous waste. However, common solution-leaching methods suffer from the trade-off between As removal and V2O5 retention, and it would be necessary to introduce extra proceedings like ingredients reimplantation and As-bearing waste treatment after regeneration. Herein, a formic acid-mediated regeneration strategy has been developed to achieve superior catalytic activity, short timescale regeneration, and nontoxic metallic As recycling with controllable and safe conduction. The specific activity of the optimal regenerated catalyst reaches 98.3% of the fresh catalyst with 99.1% As removal and less than 1.8% V loss within 15 min. Structure characterizations reveal that the distorted VOx molecular structure, surface acidity, and redox property recover to the fresh level after regeneration. In situ investigation of the regeneration process indicates that As-OH removal together with V-OH generation occurs at the first regeneration stage, followed by the active center V═O sites over-reduction at the second stage. The retained V═O species by suitable regeneration temperature and time are essential for NH3-selective catalytic reduction (SCR) since As existence and VOx over-reduction will separately cause unstable and excessive NH3 adsorption to further suppress the reaction cycle. The developed strategy and improved understanding of active site protection would exert benefits on the development of efficient and time-saving regeneration methods for spent catalysts.


Assuntos
Venenos , Amônia/química , Catálise , Formiatos , Titânio/química
19.
J Hazard Mater ; 436: 129208, 2022 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-35739730

RESUMO

Adsorptive removal of gas phase low concentration macromolecular organic component, represented by naphthalene, from the enclosed space using ordered mesoporous carbon (OMC) has been studied by molecular simulation and experimental investigation. The simulation results indicated that both adsorption capacity and adsorption stability of the OMCs for naphthalene decreased with the increase of pore sizes from 2 nm to 8 nm. Characterizations showed that the prepared OMCs had the pore structure similar to the simulated OMCs except for the rough surface. In particular, the adsorption performance of the prepared OMCs was significantly lower than that of the simulated OMCs when pore size was 2 nm and 3 nm, which was attributed to the rough inner surface of these adsorbents, blocking the narrow pore channels and significantly reducing the pore volume. OMC with pore size of 4 nm had the highest adsorption amount for naphthalene. The co-adsorption experiments in the presence of both naphthalene and toluene, acetone or water showed the adsorption performance of OMCs for naphthalene were almost unaffected by the presence of low concentration toluene and acetone, as well as high relative humidity.

20.
Environ Sci Technol ; 56(10): 6282-6293, 2022 05 17.
Artigo em Inglês | MEDLINE | ID: mdl-35512288

RESUMO

Microorganisms residing in the human respiratory tract can be exhaled, and they constitute a part of environmental microbiotas. However, the expiratory microbiota community and its associations with environmental microbiotas remain poorly understood. Here, expiratory bacteria and fungi and the corresponding microbiotas from the living environments were characterized by DNA amplicon sequencing of residents' exhaled breath condensate (EBC) and environmental samples collected from 14 residences in Nanjing, China. The microbiotas of EBC samples, with a substantial heterogeneity, were found to be as diverse as those of skin, floor dust, and airborne microbiotas. Model fitting results demonstrated the role of stochastic processes in the assembly of the expiratory microbiota. Using a fast expectation-maximization algorithm, microbial community analysis revealed that expiratory microbiotas were differentially associated with other types of microbiotas in a type-dependent and residence-specific manner. Importantly, the expiratory bacteria showed a composition similarity with airborne bacteria in the bathroom and kitchen environments with an average of 12.60%, while the expiratory fungi showed a 53.99% composition similarity with the floor dust fungi. These differential patterns indicate different relationships between expiratory microbiotas and the airborne microbiotas and floor dust microbiotas. The results here illustrated for the first time the associations between expiratory microbiotas and indoor microbiotas, showing a potential microbial exchange between the respiratory tract and indoor environment. Thus, improved hygiene and ventilation practices can be implemented to optimize the indoor microbial exposome, especially in indoor bathrooms and kitchens.


Assuntos
Poluição do Ar em Ambientes Fechados , Microbiota , Poluição do Ar em Ambientes Fechados/análise , Bactérias/genética , Poeira/análise , Fungos , Humanos , Ventilação
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