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1.
Biomaterials ; 313: 122764, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39190941

RESUMO

Currently, mitochondrial dysfunction caused by oxidative stress is a growing concern in degenerative diseases, notably intervertebral disc degeneration (IVDD). Dysregulation of the balance of mitochondrial quality control (MQC) has been considered the key contributor, while it's still challenging to effectively harmonize different MQC components in a simple and biologically safe way. Hydrogen gas (H2) is a promising mitochondrial therapeutic molecule due to its bio-reductivity and diffusibility across cellular membranes, yet its relationship with MQC regulation remains unknown. Herein, we propose a mitochondrial 'Birth-Death' coordinator achieved by an intelligent hydrogen nanogenerator (Fe@HP-OD), which can sustainably release H2 in response to the unique microenvironment in degenerated IVDs. Both in vitro and in vivo results prove alleviation of cellular oxidative stress and restoration of nucleus pulposus cells function, thereby facilitating successful IVD regeneration. Significantly, this study for the first time proposes the mitochondrial 'Birth-Death' coordination mechanism: 1) attenuation of overactivated mitochondrial 'Death' process (UPRmt and unselective mitophagy); and 2) activation of Adenosine 5'-monophosphate-activated protein kinase (AMPK) signaling pathway for mitochondrial 'Birth-Death' balance (mitochondrial biogenesis and controlled mitophagy). These pioneering findings can fill in the gaps in molecular mechanisms for H2 regulation on MQC homeostasis, and pave the way for future strategies towards restoring equilibrium of MQC system against degenerative diseases.


Assuntos
Hidrogênio , Degeneração do Disco Intervertebral , Mitocôndrias , Estresse Oxidativo , Hidrogênio/química , Animais , Mitocôndrias/metabolismo , Mitocôndrias/efeitos dos fármacos , Estresse Oxidativo/efeitos dos fármacos , Regeneração/efeitos dos fármacos , Disco Intervertebral/efeitos dos fármacos , Humanos , Mitofagia/efeitos dos fármacos , Ratos Sprague-Dawley , Masculino , Núcleo Pulposo/metabolismo , Ratos
2.
J Environ Sci (China) ; 148: 274-282, 2025 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-39095164

RESUMO

Developing cost-effective and high-performance catalyst systems for dry reforming of methane (DRM) is crucial for producing hydrogen (H2) sustainably. Herein, we investigate using iron (Fe) as a promoter and major alumina support in Ni-based catalysts to improve their DRM performance. The addition of iron as a promotor was found to add reducible iron species along with reducible NiO species, enhance the basicity and induce the deposition of oxidizable carbon. By incorporating 1 wt.% Fe into a 5Ni/10ZrAl catalyst, a higher CO2 interaction and formation of reducible "NiO-species having strong interaction with support" was observed, which led to an ∼80% H2 yield in 420 min of Time on Stream (TOS). Further increasing the Fe content to 2wt% led to the formation of additional reducible iron oxide species and a noticeable rise in H2 yield up to 84%. Despite the severe weight loss on Fe-promoted catalysts, high H2 yield was maintained due to the proper balance between the rate of CH4 decomposition and the rate of carbon deposit diffusion. Finally, incorporating 3 wt.% Fe into the 5Ni/10ZrAl catalyst resulted in the highest CO2 interaction, wide presence of reducible NiO-species, minimum graphitic deposit and an 87% H2 yield. Our findings suggest that iron-promoted zirconia-alumina-supported Ni catalysts can be a cheap and excellent catalytic system for H2 production via DRM.


Assuntos
Óxido de Alumínio , Hidrogênio , Ferro , Metano , Níquel , Zircônio , Metano/química , Zircônio/química , Catálise , Ferro/química , Hidrogênio/química , Óxido de Alumínio/química , Níquel/química
3.
J Environ Sci (China) ; 149: 535-550, 2025 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-39181665

RESUMO

Li6ZnO4 was chemically modified by nickel addition, in order to develop different compositions of the solid solution Li6Zn1-xNixO4. These materials were evaluated bifunctionally; analyzing their CO2 capture performances, as well as on their catalytic properties for H2 production via dry reforming of methane (DRM). The crystal structures of Li6Zn1-xNixO4 solid solution samples were determined through X-ray diffraction, which confirmed the integration of nickel ions up to a concentration around 20 mol%, meanwhile beyond this value, a secondary phase was detected. These results were supported by XPS and TEM analyses. Then, dynamic and isothermal thermogravimetric analyses of CO2 capture revealed that Li6Zn1-xNixO4 solid solution samples exhibited good CO2 chemisorption efficiencies, similarly to the pristine Li6ZnO4 chemisorption trends observed. Moreover, a kinetic analysis of CO2 isothermal chemisorptions, using the Avrami-Erofeev model, evidenced an increment of the constant rates as a function of the Ni content. Since Ni2+ ions incorporation did not reduce the CO2 capture efficiency and kinetics, the catalytic properties of these materials were evaluated in the DRM process. Results demonstrated that nickel ions favored hydrogen (H2) production over the pristine Li6ZnO4 phase, despite a second H2 production reaction was determined, methane decomposition. Thereby, Li6Zn1-xNixO4 ceramics can be employed as bifunctional materials.


Assuntos
Dióxido de Carbono , Hidrogênio , Metano , Hidrogênio/química , Metano/química , Dióxido de Carbono/química , Níquel/química , Catálise , Modelos Químicos
4.
Bioresour Technol ; 412: 131432, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-39236909

RESUMO

In this study, the effect of modulating fulvic acid (FA) concentrations (0, 25 and 50 mg/L) on nitrogen removal in a bioelectrochemical hydrogen autotrophic denitrification system (BHDS) was investigated. Results showed that FA increased the nitrate (NO3--N) removal rate of the BHDSs from 37.8 to 46.2 and 45.2 mg N/(L·d) with a current intensity of 40 mA. The metagenomic analysis revealed that R2 (25 mg/L) was predominantly populated by autotrophic denitrifying microorganisms, which enhanced denitrification performance by facilitating electron transfer. Conversely, R3 (50 mg/L) exhibited an increase in genes related to the heterotrophic process, which improved the denitrification performance through the collaborative action of both autotrophic and heterotrophic denitrification pathways. Besides, the study also identified a potential for nitrogen removal in Serpentinimonas, which have been rarely studied. The interesting set of findings provide valuable reference for optimizing BHDS for nitrogen removal and promoting specific denitrifying genera within the system.


Assuntos
Processos Autotróficos , Benzopiranos , Desnitrificação , Hidrogênio , Hidrogênio/metabolismo , Nitratos/metabolismo , Nitrogênio , Bactérias/metabolismo , Técnicas Eletroquímicas/métodos
5.
Sci Rep ; 14(1): 21425, 2024 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-39271809

RESUMO

Oxidative stress in adipose tissue may alter the secretion pattern of adipocytokines and potentially promote atherosclerosis. However, the therapeutic role of hydrogen in adipose tissue under oxidative stress remains unclear. In this study, subcutaneous adipose tissue (SCAT) was collected from the mid-thoracic wounds of 12 patients who underwent open-heart surgery with a mid-thoracic incision. The adipose tissue was then immersed in a culture medium dissolved with hydrogen, which was generated using a hydrogen-generating device. The weight of the adipose tissue was measured before and after hydrogenation, and the tissue was immunostained for nuclear factor erythroid 2-related factor 2 (Nrf2), heme oxygenase-1 (HO-1), and superoxide dismutase (SOD), which are markers of oxidative stress. The immunostaining results showed that HO-1 and Nrf2 expression levels were significantly decreased in the hydrogenated group, whereas SOD expression levels increased, but did not attain statistical significance. Image analysis of adipose tissue revealed that a reduction in adipocyte size. Furthermore, hydrogenated adipose tissue showed a trend toward increased gene expression levels of adiponectin and decreased gene expression levels of chemerin, an adipocytokine involved in adipogenesis. These results demonstrated the therapeutic potential of hydrogen gas for oxidative stress in adipose tissue and for reducing adipocyte size.


Assuntos
Tecido Adiposo , Hidrogênio , Estresse Oxidativo , Estresse Oxidativo/efeitos dos fármacos , Humanos , Hidrogênio/farmacologia , Hidrogênio/metabolismo , Masculino , Feminino , Tecido Adiposo/metabolismo , Tecido Adiposo/efeitos dos fármacos , Pessoa de Meia-Idade , Superóxido Dismutase/metabolismo , Heme Oxigenase-1/metabolismo , Heme Oxigenase-1/genética , Idoso , Adiponectina/metabolismo , Adiponectina/genética , Adipócitos/metabolismo , Adipócitos/efeitos dos fármacos , Gordura Subcutânea/metabolismo , Gordura Subcutânea/efeitos dos fármacos , Fator 2 Relacionado a NF-E2
6.
Microbiome ; 12(1): 170, 2024 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-39252128

RESUMO

BACKGROUND: Clean energy hydrogen (H2) produced from abundant lignocellulose is an alternative to fossil energy. As an essential influencing factor, there is a lack of comparison between constant temperatures (35, 55 and 65 °C) and gradient heating temperature (35 to 65 °C) on the H2 production regulation potential from lignocellulose-rich straw via high-solid anaerobic digestion (HS-AD). More importantly, the microbial mechanism of temperature regulating H2 accumulation needs to be investigated. RESULTS: Constant 65 °C led to the lowest lignin residue (1.93%) and the maximum release of cellulose and hemicellulose, and the highest H2 production (26.01 mL/g VS). H2 production at 35 and 55 °C was only 14.56 and 24.13 mL/g VS, respectively. In order to further explore the potential of ultra-high temperature (65 °C), HS-AD was performed by gradient heating conditions (35 to 65 °C). However, compared to constant 65 °C, gradient heating conditions led to higher lignin residue (2.49%) and lower H2 production (13.53 mL/g VS) than gradient heating conditions (47.98%). In addition, metagenomic analysis showed the cellulose/hemicellulose hydrolyzing bacteria and genes (mainly Thermoclostridium, and xynA, xynB, abfA, bglB and xynD), H2-producing bacteria and related genes (mainly Thermoclostridium, and nifD, nifH and nifK), and microbial movement and metabolic functions were enriched at 65 °C. However, the enrichment of two-component systems under gradient heating conditions resulted in a lack of highly-enriched ultra-high-temperature cellulose/hemicellulose hydrolyzing genera and related genes but rather enriched H2 consumption genera and genes (mainly Acetivibrio, and hyaB and hyaA) resulting in a weaker H2 production. CONCLUSIONS: The lignin degradation process does not directly determine H2 accumulation, which was actually regulated by bacteria/genes contributing to H2 production/consumption. In addition, it is temperature that enhances the hydrolysis process of lignin rather than lignin-degrading enzymes, bacteria and genes by promoting microbial material transfer and metabolism. In terms of temperature, one of the key parameters of HS-AD for H2 production, we developed an important regulatory strategy, enriched the theoretical basis of temperature regulation for H2 production to further expanded the research horizon in this field. Video Abstract.


Assuntos
Hidrogênio , Lignina , Hidrogênio/metabolismo , Lignina/metabolismo , Anaerobiose , Temperatura Alta , Celulose/metabolismo , Polissacarídeos/metabolismo , Metagenômica/métodos , Temperatura , Bactérias/metabolismo , Bactérias/classificação , Bactérias/genética
7.
Microb Cell Fact ; 23(1): 247, 2024 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-39261831

RESUMO

Biofuel can be generated by different organisms using various substrates. The green alga Chlorococcum humicola OQ934050 exhibited the capability to photosynthesize carbonate carbon, maybe via the activity of carbonic anhydrase enzymes. The optimum treatment is C:N ratio of 1:1 (0.2 mmoles sodium carbonate and 0.2 mmoles sodium nitrate) as it induced the highest dry mass (more than 0.5 mg.mL-1). At this combination, biomass were about 0.2 mg/mL-1 carbohydrates, 0.085 mg/mL-1 proteins, and 0.16 mg/mL-1 oil of this dry weight. The C/N ratios of 1:1 or 10:1 induced up to 30% of the Chlorococcum humicola dry mass as oils. Growth and dry matter content were hindered at 50:1 C/N and oil content was reduced as a result. The fatty acid profile was strongly altered by the applied C.N ratios. The defatted leftovers of the grown alga, after oil extraction, were fermented by a newly isolated heterotrophic bacterium, identified as Bacillus coagulans OQ053202, to evolve hydrogen content as gas. The highest cumulative hydrogen production and reducing sugar (70 ml H2/g biomass and 0.128 mg/ml; respectively) were found at the C/N ratio of 10:1 with the highest hydrogen evolution efficiency (HEE) of 22.8 ml H2/ mg reducing sugar. The optimum treatment applied to the Chlorococcum humicola is C:N ratio of 1:1 for the highest dry mass, up to 30% dry mass as oils. Some fatty acids were induced while others disappeared, depending on the C/N ratios. The highest cumulative hydrogen production and reducing sugar were found at the C/N ratio of 10:1.


Assuntos
Bacillus , Biocombustíveis , Biomassa , Carbonatos , Hidrogênio , Nitratos , Hidrogênio/metabolismo , Bacillus/metabolismo , Nitratos/metabolismo , Carbonatos/metabolismo , Fermentação , Clorófitas/metabolismo , Clorófitas/crescimento & desenvolvimento , Fotossíntese , Ácidos Graxos/metabolismo
8.
Yakugaku Zasshi ; 144(9): 877-886, 2024.
Artigo em Japonês | MEDLINE | ID: mdl-39218655

RESUMO

Nucleosides with a substituent at the 4'-position have received much attention as antiviral drugs and as raw materials for oligonucleotide therapeutics. 4'-Modified nucleosides are generally synthesized using ionic reactions through the introduction of electrophilic or nucleophilic substituents at the 4'-position. However, their synthetic methods have some drawbacks; e.g., (i) it is difficult to control stereoselectivity at the 4'-position; (ii) complex protection-deprotection processes are required; (iii) the range of electrophiles and nucleophiles is limited. With this background, we considered that a carbon radical generated at the 4'-position would be a useful intermediate for the synthesis of 4'-modified nucleosides. In this review, two novel methods for the generation of 4'-carbon radicals are summarized. The first utilizes radical deformylation involving ß-fragmentation of a hydroxymethyl group at the 4'-position. The other utilizes radical decarboxylation and 1,5-hydrogen atom transfer (1,5-HAT), which enables the generation of 4'-carbon radicals while retaining the hydroxymethyl group at the 4'-position. These methods enable the rapid and facile generation of 4'-carbon radicals and provide various 4'-modified nucleosides including 2',4'-bridged structures.


Assuntos
Antivirais , Carbono , Nucleosídeos , Nucleosídeos/síntese química , Nucleosídeos/química , Carbono/química , Radicais Livres/química , Radicais Livres/síntese química , Antivirais/síntese química , Antivirais/química , Técnicas de Química Sintética/métodos , Hidrogênio/química
9.
Bioresour Technol ; 412: 131414, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-39226941

RESUMO

Anaerobic electrochemical digestion (AED) is an effective system for recovering biogas from organic wastes. However, the effects of different anode potentials on anaerobic activated sludge remain unclear. This study confirmed that biofilms exhibited the best electroactivity at -0.2 V (vs. Ag/AgCl) compared to -0.4 V and 0 V. Gas was further regulated, with the highest hydrogen content (47 ± 7 %) observed at -0.2 V. The 0 V system produced the largest amount of methane (70 ± 8 %) and exhibited the greatest presence of hydrogen-utilizing microorganisms. The gas yield at -0.4 V was the lowest, with no hydrogen detected. Excess bioelectrohydrogen at -0.2 V and 0 V caused the co-enrichment of Methanobacterium and Acetoanaerobium, establishing a thermodynamically feasible current-acetate-hydrogen electron cycle to improve electrogenesis. These results provide insights into the regulatory strategies of MEC technology during anaerobic digestion, which play a decisive role in determining the composition of biogas.


Assuntos
Eletrodos , Hidrogênio , Metano , Microbiota , Anaerobiose , Hidrogênio/metabolismo , Metano/metabolismo , Microbiota/fisiologia , Gases , Esgotos/microbiologia , Biocombustíveis , Técnicas Eletroquímicas/métodos , Biofilmes
10.
CNS Neurosci Ther ; 30(9): e70021, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39258790

RESUMO

BACKGROUND: Sepsis-associated encephalopathy (SAE) is a neuronal injury with poor prognosis. Mitochondrial dysfunction is critical in SAE development, and hydrogen gas (H2) has a protective effect on septic mice. This study aimed to investigate the effect of high concentration (67%) of H2 on SAE and whether it is related to mitochondrial biogenesis and mitochondrial dynamics. METHODS: A mouse sepsis model was induced by cecal ligation and puncture. The mice inhalated 67% H2 for 1 h at 1 and 6 h post-surgery, respectively. The 7-day survival rate was recorded. Cognitive function was assessed using the Y-maze test and Morris water maze test. Serum inflammatory factors, antioxidant enzymes, as well as mitochondrial function indexes including mitochondrial membrane potential (MMP) and ATP in the hippocampal tissue were evaluated 24 h after surgery. Mitochondrial dynamic proteins (DRP1 and MFN2) and biosynthetic proteins (PGC-1α, NRF2, and TFAM) in the hippocampal tissue were detected. Moreover, the morphology of mitochondria was observed by transmission electron microscopy. RESULTS: Inhalation of 67% H2 improved the 7-day survival rates and recognition memory function of septic mice, alleviated brain antioxidant enzyme activity (SOD and CAT), and reduced serum proinflammatory cytokine levels. H2 inhalation also enhanced the expression of MFN2 and mitochondrial biogenesis-related factors (PGC-1α, NRF2, and TFAM) and decreased the expression of fission protein (DRP1), leading to improvement in mitochondrial function, as evidenced by MMP and ATP levels. CONCLUSIONS: Inhalation of high concentration (67%) of H2 in septic mice improved the survival rate and reduced neuronal injury. Its mechanism might be mediated by enhancing mitochondrial biogenesis and mitochondrial dynamics.


Assuntos
Hidrogênio , Dinâmica Mitocondrial , Encefalopatia Associada a Sepse , Animais , Encefalopatia Associada a Sepse/tratamento farmacológico , Camundongos , Hidrogênio/farmacologia , Hidrogênio/administração & dosagem , Hidrogênio/uso terapêutico , Dinâmica Mitocondrial/efeitos dos fármacos , Masculino , Administração por Inalação , Hipocampo/efeitos dos fármacos , Hipocampo/metabolismo , Mitocôndrias/efeitos dos fármacos , Mitocôndrias/metabolismo , Sepse/complicações , Sepse/tratamento farmacológico , Sepse/metabolismo , Camundongos Endogâmicos C57BL , Potencial da Membrana Mitocondrial/efeitos dos fármacos , Aprendizagem em Labirinto/efeitos dos fármacos
11.
Crit Care Med ; 52(10): 1567-1576, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39133068

RESUMO

OBJECTIVE: The Efficacy of Inhaled Hydrogen on Neurologic Outcome Following Brain Ischemia During Post-Cardiac Arrest Care (HYBRID) II trial (jRCTs031180352) suggested that hydrogen inhalation may reduce post-cardiac arrest brain injury (PCABI). However, the combination of hypothermic target temperature management (TTM) and hydrogen inhalation on outcomes is unclear. The aim of this study was to investigate the combined effect of hydrogen inhalation and hypothermic TTM on outcomes after out-of-hospital cardiac arrest (OHCA). DESIGN: Post hoc analysis of a multicenter, randomized, controlled trial. SETTING: Fifteen Japanese ICUs. PATIENTS: Cardiogenic OHCA enrolled in the HYBRID II trial. INTERVENTIONS: Hydrogen mixed oxygen (hydrogen group) versus oxygen alone (control group). MEASUREMENTS AND MAIN RESULTS: TTM was performed at a target temperature of 32-34°C (TTM32-TTM34) or 35-36°C (TTM35-TTM36) per the institutional protocol. The association between hydrogen + TTM32-TTM34 and 90-day good neurologic outcomes was analyzed using generalized estimating equations. The 90-day survival was compared between the hydrogen and control groups under TTM32-TTM34 and TTM35-TTM36, respectively. The analysis included 72 patients (hydrogen [ n = 39] and control [ n = 33] groups) with outcome data. TTM32-TTM34 was implemented in 25 (64%) and 24 (73%) patients in the hydrogen and control groups, respectively ( p = 0.46). Under TTM32-TTM34, 17 (68%) and 9 (38%) patients achieved good neurologic outcomes in the hydrogen and control groups, respectively (relative risk: 1.81 [95% CI, 1.05-3.66], p < 0.05). Hydrogen + TTM32-TTM34 was independently associated with good neurologic outcomes (adjusted odds ratio 16.10 [95% CI, 1.88-138.17], p = 0.01). However, hydrogen + TTM32-TTM34 did not improve survival compared with TTM32-TTM34 alone (adjusted hazard ratio: 0.22 [95% CI, 0.05-1.06], p = 0.06). CONCLUSIONS: Hydrogen + TTM32-TTM34 was associated with improved neurologic outcomes after cardiogenic OHCA compared with TTM32-TTM34 monotherapy. Hydrogen inhalation is a promising treatment option for reducing PCABI when combined with TTM32-TTM34.


Assuntos
Isquemia Encefálica , Hidrogênio , Hipotermia Induzida , Parada Cardíaca Extra-Hospitalar , Humanos , Parada Cardíaca Extra-Hospitalar/terapia , Parada Cardíaca Extra-Hospitalar/tratamento farmacológico , Parada Cardíaca Extra-Hospitalar/mortalidade , Hidrogênio/administração & dosagem , Hidrogênio/uso terapêutico , Hipotermia Induzida/métodos , Masculino , Feminino , Administração por Inalação , Pessoa de Meia-Idade , Idoso , Isquemia Encefálica/prevenção & controle , Isquemia Encefálica/tratamento farmacológico , Terapia Combinada
12.
Sci Total Environ ; 951: 175673, 2024 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-39168318

RESUMO

The misuse and continues discharge of antibiotics can cause serious pollution, which is urgent to take steps to remit the environment pollution. In this study, anaerobic bacteria isolated from the aeration tank of a local sewage treatment plant were employed to investigate hydrogen production and tetracycline (TC) degradation during anaerobic fermentation. Results indicate that low concentrations of TC enhanced hydrogen production, increasing from 366 mL to a maximum of 480 mL. This increase is attributed to stimulated hydrolysis and acidogenesis, coupled with significant inhibition of homoacetogenesis. Furthermore, the removal of TC, facilitated by adsorption and biodegradation, exceeded 90 %. During the fermentation process, twenty-one by-products were identified, leading to the proposal of four potential degradation pathways. Analysis of the microbial community revealed shifts in diversity and a decrease in the abundance of hydrogen-producing bacteria, whereas bacteria harboring tetracycline resistance genes became more prevalent. This study provides a possibility to treat tetracycline-contaminated wastewater and to produce clean energy simultaneously by anaerobic fermentation.


Assuntos
Biodegradação Ambiental , Fermentação , Hidrogênio , Tetraciclina , Eliminação de Resíduos Líquidos , Poluentes Químicos da Água , Hidrogênio/metabolismo , Anaerobiose , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/metabolismo , Poluentes Químicos da Água/análise , Águas Residuárias , Antibacterianos/metabolismo , Microbiota , Bactérias/metabolismo
13.
Bioresour Technol ; 411: 131330, 2024 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-39182797

RESUMO

Biomethanation converts carbon dioxide (CO2) emissions into renewable natural gas (RNG) using mixed microbial cultures enriched with hydrogenotrophic archaea. This study examines the performance of a single methanogenic archaeon converting biogas with added hydrogen (H2) into methane (CH4) using a trickle-bed bioreactor with enhanced gas-liquid mass transport. The process in continuous operation followed the theoretical reaction of hydrogenotrophic methanogenesis (CO2 + 4 H2 â†’ CH4 + 2 H2O), producing RNG with over 99 % CH4 and more than 0.9 H2 conversion efficiency. The Monod constants of H2 uptake were experimentally determined using kinetic modelling. Also, a dimensionless parameter was used to quantify the ratio between the H2 mass transfer rate and the maximum attainable H2 consumption rate. Single-culture biomethanation averts the formation of secondary metabolites and bicarbonate buffer interferences, resulting in lower demands for H2 than mixed-culture biomethanation.


Assuntos
Biocombustíveis , Reatores Biológicos , Hidrogênio , Metano , Gás Natural , Metano/metabolismo , Biocombustíveis/microbiologia , Hidrogênio/metabolismo , Reatores Biológicos/microbiologia , Cinética , Dióxido de Carbono/metabolismo
14.
Waste Manag ; 187: 306-316, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39089146

RESUMO

Plastic waste poses a critical environmental challenge for the world. The proliferation of waste plastic coffee pods exacerbates this issue. Traditional disposal methods such as incineration and landfills are environmentally unfriendly, necessitating the exploration of alternative management strategies. One promising avenue is the pyrolysis in-line reforming process, which converts plastic waste into hydrogen. However, traditional pyrolysis methods are costly due to inefficiencies and heat losses. To address this, for the first time, our study investigates the use of microwave to enhance the pyrolysis process. We explored microwave pyrolysis for polypropylene (PP), high-density polypropylene (HDPE), and waste coffee pods, with the latter primarily comprising polypropylene. Additionally, catalytic ex-situ pyrolysis of coffee pod pyrolysis over a nickel-based catalyst was investigated to convert the evolved gas into hydrogen. The single-stage microwave pyrolysis results revealed the highest gas yield at 500 °C for HDPE, and 41 % and 58 % (by mass) for waste coffee pods and polypropylene at 700 °C, respectively. Polypropylene exhibited the highest gaseous yield, suggesting its readiness for pyrolytic degradation. Waste coffee pods uniquely produced carbon dioxide and carbon monoxide gases because of the oxygen present in their structure. Catalytic reforming of evolved gas from waste coffee pods using a 5 % nickel loaded activated carbon catalyst, yielded 76 % (by volume) hydrogen at 900 °C. These observed results were supported by elemental balance analysis. These findings highlight that two-stage microwave and catalysis assisted pyrolysis could be a promising method for the efficient management of waste coffee pods, particularly for producing clean energy.


Assuntos
Café , Hidrogênio , Micro-Ondas , Polietileno , Polipropilenos , Pirólise , Polipropilenos/química , Hidrogênio/química , Café/química , Catálise , Polietileno/química , Eliminação de Resíduos/métodos
15.
Chemosphere ; 363: 142996, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39097105

RESUMO

Photocatalytic degradation of pollutants coupled with hydrogen (H2) evolution has emerged as a promising solution for environmental and energy crises. However, the fast recombination of photoexcited electrons and holes limits photocatalytic activities. Herein, an S-scheme heterojunction carbon doped-TiO2/ZnIn2S4 (C-TiO2/ZnIn2S4) was designed by substituting oxygen sites within C-TiO2 by ZnIn2S4. Under visible light irradiation, the optimal C-TiO2/ZnIn2S4 exhibits a higher degradation efficiency (88.6%) of microcystin-LR (MC-LR), compared to pristine C-TiO2 (72.9%) and ZnIn2S4 (66.8%). Furthermore, the H2 yield of the C-TiO2/ZnIn2S4 reaches 1526.9 µmol g-1 h-1, which is 3.83 times and 2.87 times that of the C-TiO2 and ZnIn2S4, respectively. Experimental and theoretical investigations reveal that an internal electric field (IEF) informed in the C-TiO2/ZnIn2S4 heterojunction, accelerates the separation of photogenerated charge pairs, thereby enhancing photocatalytic efficiency of MC-LR degradation and H2 production. This work highlights a new perspective on the development of high-performance photocatalysts for wastewater treatment and H2 generation.


Assuntos
Carbono , Hidrogênio , Toxinas Marinhas , Microcistinas , Titânio , Microcistinas/química , Titânio/química , Toxinas Marinhas/química , Catálise , Hidrogênio/química , Carbono/química , Fotólise , Poluentes Químicos da Água/química , Águas Residuárias/química , Luz , Processos Fotoquímicos , Zinco/química
16.
Environ Sci Technol ; 58(33): 14675-14686, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39102504

RESUMO

The escalating levels of plastic waste and energy crises underscore the urgent need for effective waste-to-energy strategies. This study focused on converting polypropylene wastes into high-value products employing various iron-based catalysts and microwave radiative thermal processing. The Al-Fe catalysts exhibited exceptional performance, achieving a hydrogen utilization efficiency of 97.65% and a yield of 44.07 mmol/g PP. The gas yields increased from 19.99 to 94.21 wt % compared to noncatalytic experiments. Furthermore, this catalytic system produced high-value bamboo-shaped carbon nanotubes that were absent in other catalysts. The mechanism analysis on catalytic properties and product yields highlighted the significance of oxygen vacancies in selecting high-value products through two adsorption pathways. Moreover, the investigation examined the variations in product distribution mechanisms between conventional and microwave pyrolysis, in which microwave conditions resulted in 4 times higher hydrogen yields. The technoeconomic assessment and Monte Carlo risk analysis further compared the disparity. The microwave technique had a remarkable internal rate of return (IRR) of 39%, leading to an income of $577/t of plastic with a short payback period of 2.5 years. This research offered sustainable solutions for the plastic crisis, validating the potential applicability of commercializing the research outcomes in real-world scenarios.


Assuntos
Hidrogênio , Micro-Ondas , Nanotubos de Carbono , Plásticos , Nanotubos de Carbono/química , Hidrogênio/química , Catálise
17.
Environ Sci Technol ; 58(33): 14940-14948, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39105779

RESUMO

Low concentrations of nitrate (NO3-) widely exist in wastewater, post-treated wastewater, and natural environments; its further disposal is a challenge but meaningful for its discharge goals. Electroreduction of NO3- is a promising method that allows to eliminate NO3- and even generate higher-value NH3. However, the massive side reaction of hydrogen evolution has raised great obstacles in the electroreduction of low concentrations of NO3-. Herein, we present an efficient electroreduction method for low or even ultralow concentrations of NO3- via NO3- self-enrichment and active hydrogen (H*) inducement on the Ce(IV)-Co3O4 cathode. The key mechanism is that the strong oxytropism of Ce(IV) in Co3O4 resulted in two changes in structures, including loose nanoporous structures with copious dual adsorption sites of Ce-Co showing strong self-enrichment of NO3- and abundant oxygen vacancies (Ovs) inducing substantial H*. Ultimately, the bifunctional role synergistically promoted the selective conversion of NH3 rather than H2. As a result, Ce(IV)-Co3O4 demonstrated a NO3- self-enrichment with a 4.3-fold up-adsorption, a 7.5-fold enhancement of NH3 Faradic efficiency, and a 93.1% diminution of energy consumption when compared to Co3O4, substantially exceeding other reported electroreduction cathodes for NO3- concentrations lower than 100 mg·L-1. This work provides an effective treatment method for low or even ultralow concentrations of NO3-.


Assuntos
Eletrodos , Nitratos , Nitratos/química , Hidrogênio/química , Cério/química
18.
Bioresour Technol ; 408: 131196, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39094961

RESUMO

Hydrogen-ethanol co-production can significantly improve the energy conversion efficiency of corn stalk (CS). In this study, with CS as the raw material, the co-production characteristics of one-step and two-step photo-fermentation hydrogen production (PFHP) and ethanol production were investigated. In addition, the gas and liquid characteristics of the experiment were analyzed. The kinetics of hydrogen-ethanol co-production was calculated, and the economics of hydrogen and ethanol were analyzed. Results of the experiments indicated that the two-step hydrogen-ethanol co-production had the best hydrogen production performance when the concentration of CS was 25 g/L. The total hydrogen production was 350.08 mL, and the hydrogen yield was 70.02 mL/g, which was 2.45 times higher than that of the one-step method. The efficiency of hydrogen-ethanol co-production was 17.79 %, which was 2.76 times more efficient than hydrogen compared to fermentation with hydrogen. The result provides technical reference for the high-quality utilization of CS.


Assuntos
Biocombustíveis , Etanol , Fermentação , Hidrogênio , Zea mays , Hidrogênio/metabolismo , Zea mays/química , Zea mays/metabolismo , Etanol/metabolismo , Cinética , Biotecnologia/métodos , Luz
19.
Bioresour Technol ; 408: 131225, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39111397

RESUMO

Biomethanation represents a promising approach for biomethane production, with biofilm-based processes like trickle bed reactors (TBRs) being among the most efficient solutions. However, maintaining stable performance can be challenging, and both pure and mixed culture approaches have been applied to address this. In this study, inocula enriched with hydrogenotrophic methanogens were introduced to to TBRs as bioaugmentation strategy to assess their impacts on the process performance and microbial community dynamics. Metagenomic analysis revealed a metagenome-assembled genome belonging to the hydrogenotrophic genus Methanobacterium, which became dominant during enrichment and successfully colonized the TBR biofilm after bioaugmentation. The TBRs achieved a biogas production with > 96 % methane. The bioaugmented reactor consumed additional H2. This may be due to microbial species utilizing CO2 and H2 via various CO2 reduction pathways. Overall, implementing bioaugmentation in TBRs showed potential for establishing targeted species, although challenges remain in managing H2 consumption and optimizing microbial interactions.


Assuntos
Reatores Biológicos , Dióxido de Carbono , Hidrogênio , Metano , Hidrogênio/metabolismo , Reatores Biológicos/microbiologia , Dióxido de Carbono/metabolismo , Metano/metabolismo , Biocombustíveis/microbiologia , Biofilmes , Methanobacterium/metabolismo
20.
J Chromatogr A ; 1732: 465220, 2024 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-39106664

RESUMO

Partial least squares (PLS) regression is a valuable chemometric tool for property prediction when coupled with gas chromatography (GC). Since the separation run time and stationary phase selection are crucial for effective PLS modeling, we study these GC parameters on the prediction of viscosity, density and hydrogen content for 50 aerospace fuels. Due to the diversity of compounds in the fuels (primarily alkanes, cycloalkanes, and aromatics), we explore both polar and non-polar stationary phase columns. The robustness for the PLS models was evaluated by their normalized root mean square error of cross-validation (NRMSECV). PLS models built for viscosity across 1-min, 3-min, 7-min, and 10-min time window (TW) high-speed GC separations produced nearly the same NRMSECV with the polar column data with an average (standard deviation) of 4.41 % (0.34 %) versus the non-polar column data of 4.69 % (0.15 %). In contrast, while the NRMSECV of density modeling with the polar column data varied more than the viscosity models, averaging 7.54 % (0.67 %), the non-polar column data produced a significantly higher average NRMSECV of 10.06 % (0.35 %). Similarly, for hydrogen content, the NRMSECV with the polar column data averaged 9.50 % (0.87 %), which was significantly lower than the NRMSECV with the non-polar column data averaging 12.10 % (0.88 %). We also investigated the impact of smoothing the GC data on the corresponding PLS models. By applying varying degrees of smoothing, we can effectively obtain similar chromatographic peak patterns in a shorter TW. For example, a 10-min smoothed chromatogram appears like the 1-min separation with no smoothing but resulted in nearly the same NRMSECV. Overall, the fast separation with a 1-min TW produced robust PLS models for viscosity with either stationary phase column, whereas for density and hydrogen content the polar stationary phase column produced superior PLS models, thus with proper stationary phase selection, a fast separation run time could be readily applied with optimal PLS property modeling results.


Assuntos
Hidrogênio , Análise dos Mínimos Quadrados , Cromatografia Gasosa/métodos , Viscosidade , Hidrogênio/química , Hidrogênio/análise , Modelos Químicos , Alcanos/análise , Alcanos/química
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