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1.
J Environ Sci (China) ; 148: 274-282, 2025 Feb.
Article in English | MEDLINE | ID: mdl-39095164

ABSTRACT

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.


Subject(s)
Aluminum Oxide , Hydrogen , Iron , Methane , Nickel , Zirconium , Methane/chemistry , Zirconium/chemistry , Catalysis , Iron/chemistry , Hydrogen/chemistry , Aluminum Oxide/chemistry , Nickel/chemistry
2.
J Environ Sci (China) ; 149: 535-550, 2025 Mar.
Article in English | MEDLINE | ID: mdl-39181665

ABSTRACT

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.


Subject(s)
Carbon Dioxide , Hydrogen , Methane , Hydrogen/chemistry , Methane/chemistry , Carbon Dioxide/chemistry , Nickel/chemistry , Catalysis , Models, Chemical
3.
Biomaterials ; 313: 122764, 2025 Feb.
Article in English | MEDLINE | ID: mdl-39190941

ABSTRACT

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.


Subject(s)
Hydrogen , Intervertebral Disc Degeneration , Mitochondria , Oxidative Stress , Hydrogen/chemistry , Animals , Mitochondria/metabolism , Mitochondria/drug effects , Oxidative Stress/drug effects , Regeneration/drug effects , Intervertebral Disc/drug effects , Humans , Mitophagy/drug effects , Rats, Sprague-Dawley , Male , Nucleus Pulposus/metabolism , Rats
4.
Chem Commun (Camb) ; 60(78): 10914-10917, 2024 Sep 26.
Article in English | MEDLINE | ID: mdl-39254592

ABSTRACT

[FeFe]-hydrogenases function as both H2 catalysts and sensors. While catalysis is well investigated, details regarding the H2 sensing mechanism are limited. Here, we relate protein structure changes to H2 sensing, similar to light-driven bio-sensors. Our results highlight how identical cofactors incorporated in alternative protein scaffolds serve different functions in nature.


Subject(s)
Hydrogen , Hydrogenase , Hydrogenase/chemistry , Hydrogenase/metabolism , Hydrogen/chemistry , Hydrogen/metabolism , Iron-Sulfur Proteins/chemistry , Iron-Sulfur Proteins/metabolism , Protein Structure, Secondary
5.
Water Environ Res ; 96(9): e11119, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39299908

ABSTRACT

Microbial electrolysis cell (MEC) is gaining importance not only for effectively treating wastewater but also for producing hydrogen. The up-flow microbial electrolysis cell (UPMEC) is an innovative approach to enhance the efficiency, and substrate degradation. In this study, a baffled UPMEC with an anode divided into three regions by inserting the baffle (sieve) plates at varying distances from the cathode was designed. The effect of process parameters, such as flow rate (10, 15, and 20 mL/min), electrode area (50, 100, and 150 cm2), and catholyte buffer concentration (50, 100, and 150 mM) were investigated using distillery wastewater as substrate. The experimental results showed a maximum of 0.6837 ± 0.02 mmol/L biohydrogen at 150 mM buffer, with 49 ± 1.0% COD reduction using an electrode of area 150 cm2. The maximum current density was 1335.94 mA/m2 for the flow rate of 15 mL/min and surface area of 150 cm2. The results showed that at optimized flow rate and buffer concentration, maximum hydrogen production and effective treatment of wastewater were achieved in the baffled UPMEC. PRACTITIONER POINTS: Biohydrogen production from distillery wastewater was investigated in a baffled UPMEC. Flowrate, concentration and electrode areas significantly influenced the hydrogen production. Maximum hydrogen (0.6837±0.02mmol/L.day) production and COD reduction (49±1.0%) was achieved at 15 mL/min. Highest CHR of 95.37±1.9 % and OHR of 4.6±0.09 % was observed at 150 mM buffer concentration.


Subject(s)
Bioelectric Energy Sources , Electrolysis , Hydrogen , Industrial Waste , Waste Disposal, Fluid , Wastewater , Hydrogen/metabolism , Hydrogen/chemistry , Wastewater/chemistry , Waste Disposal, Fluid/methods
6.
Int J Med Sci ; 21(12): 2390-2401, 2024.
Article in English | MEDLINE | ID: mdl-39310256

ABSTRACT

Background: Persistent inflammation over time can cause gradual harm to the body. Molecular hydrogen has the potential to specifically counteract reactive oxygen species (ROS), reduce disease severity, and enhance overall health. Investigations of the anti-inflammatory and antioxidant properties of oral solid hydrogen capsules (OSHCs) are currently limited, prompting our examination of the beneficial effects of OSHCs. Subsequently, we conducted a clinical study to assess the impact of OSHCs supplementation on individuals with chronic inflammation. Materials and methods: Initially, we evaluated the oxidative reduction potential (ORP) properties of the OSHCs solution by comparing it to hydrogen-rich water (HRW) and calcium hydride (CaH2) treated water. In our outpatient department, stable patients with chronic illnesses who were treated with varying doses of OSHCs were randomized into low-, medium-, and high-dose groups for 4 weeks. Primary outcomes included changes in the serum erythrocyte sedimentation rate (ESR) and C-reactive protein (CRP) concentrations after four weeks of OSHCs consumption. Secondary outcomes included changes in the Brief Fatigue Inventory-Taiwan (BFI-T) fatigue scale, Control Status Scale for Diabetes (CSSD70) scores, and Disease Activity Score 28 (DAS28). Results: Compared to HRW and CaH2, OSHCs demonstrated a prolonged reduction in ORP for 60 minutes in vitro and enabled a regulated release of hydrogen over 24 hours. A total of 30 participants, with 10 in each dosage (low/medium/high) group, completed the study. The average ESR120 significantly decreased from the first week to the fourth week, with a noticeable dose effect (low-dose group, p = 0.494; high-dose group, p = 0.016). Overall, the average CRP concentration showed a distinct decreasing trend after four weeks of OSHCs administration (w0 vs. w4, p = 0.077). The average DAS28 score demonstrated a significant decrease following OSHCs treatment. Furthermore, there were improvements in the BFI-T and CSSD70 scores. Conclusion: OSHCs supplementation may exert anti-inflammatory and antioxidant effects on individuals with chronic inflammation. However, further clinical studies could be investigated to explore the potential therapeutic effects of OSHCs.


Subject(s)
Dietary Supplements , Hydrogen , Inflammation , Humans , Hydrogen/administration & dosage , Pilot Projects , Male , Female , Inflammation/drug therapy , Inflammation/blood , Middle Aged , Adult , Administration, Oral , C-Reactive Protein/analysis , Antioxidants/administration & dosage , Anti-Inflammatory Agents/administration & dosage , Aged , Blood Sedimentation/drug effects , Reactive Oxygen Species/metabolism , Oxidative Stress/drug effects
7.
J Am Chem Soc ; 146(38): 26351-26359, 2024 Sep 25.
Article in English | MEDLINE | ID: mdl-39265189

ABSTRACT

The first total synthesis of the pentacyclic phenylnaphthacenoid type II polyketide antibiotic formicamycin H is described. A key feature of the synthesis involves the convergent, regioselective assembly of the tetracyclic core via ruthenium-catalyzed α-ketol-benzocyclobutenone [4 + 2] cycloaddition. Double dehydration of the diol-containing cycloadduct provides an achiral enone, which upon asymmetric nucleophilic epoxidation and further manipulations delivers the penultimate tetracyclic trichloride in enantiomerically enriched form. Subsequent chemo- and atroposelective Suzuki cross-coupling of the tetracyclic trichloride introduces the E-ring to complete the total synthesis. Single-crystal X-ray diffraction analyses of two model compounds suggest that the initially assigned stereochemistry of the axially chiral C6-C7 linkage may require revision.


Subject(s)
Anti-Bacterial Agents , Cycloaddition Reaction , Ruthenium , Ruthenium/chemistry , Catalysis , Anti-Bacterial Agents/chemical synthesis , Anti-Bacterial Agents/chemistry , Stereoisomerism , Hydrogen/chemistry , Polyketides/chemistry , Polyketides/chemical synthesis , Naphthacenes/chemistry , Naphthacenes/chemical synthesis , Molecular Structure
8.
Yakugaku Zasshi ; 144(9): 877-886, 2024.
Article in Japanese | MEDLINE | ID: mdl-39218655

ABSTRACT

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.


Subject(s)
Antiviral Agents , Carbon , Nucleosides , Nucleosides/chemical synthesis , Nucleosides/chemistry , Carbon/chemistry , Free Radicals/chemistry , Free Radicals/chemical synthesis , Antiviral Agents/chemical synthesis , Antiviral Agents/chemistry , Chemistry Techniques, Synthetic/methods , Hydrogen/chemistry
9.
Microb Cell Fact ; 23(1): 247, 2024 Sep 11.
Article in English | MEDLINE | ID: mdl-39261831

ABSTRACT

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.


Subject(s)
Bacillus , Biofuels , Biomass , Carbonates , Hydrogen , Nitrates , Hydrogen/metabolism , Bacillus/metabolism , Nitrates/metabolism , Carbonates/metabolism , Fermentation , Chlorophyta/metabolism , Chlorophyta/growth & development , Photosynthesis , Fatty Acids/metabolism
10.
Sci Rep ; 14(1): 21425, 2024 09 13.
Article in English | MEDLINE | ID: mdl-39271809

ABSTRACT

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.


Subject(s)
Adipose Tissue , Hydrogen , Oxidative Stress , Oxidative Stress/drug effects , Humans , Hydrogen/pharmacology , Hydrogen/metabolism , Male , Female , Adipose Tissue/metabolism , Adipose Tissue/drug effects , Middle Aged , Superoxide Dismutase/metabolism , Heme Oxygenase-1/metabolism , Heme Oxygenase-1/genetics , Aged , Adiponectin/metabolism , Adiponectin/genetics , Adipocytes/metabolism , Adipocytes/drug effects , Subcutaneous Fat/metabolism , Subcutaneous Fat/drug effects , NF-E2-Related Factor 2
11.
Microbiome ; 12(1): 170, 2024 Sep 10.
Article in English | MEDLINE | ID: mdl-39252128

ABSTRACT

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.


Subject(s)
Hydrogen , Lignin , Hydrogen/metabolism , Lignin/metabolism , Anaerobiosis , Hot Temperature , Cellulose/metabolism , Polysaccharides/metabolism , Metagenomics/methods , Temperature , Bacteria/metabolism , Bacteria/classification , Bacteria/genetics
12.
CNS Neurosci Ther ; 30(9): e70021, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39258790

ABSTRACT

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.


Subject(s)
Hydrogen , Mitochondrial Dynamics , Sepsis-Associated Encephalopathy , Animals , Sepsis-Associated Encephalopathy/drug therapy , Mice , Hydrogen/pharmacology , Hydrogen/administration & dosage , Hydrogen/therapeutic use , Mitochondrial Dynamics/drug effects , Male , Administration, Inhalation , Hippocampus/drug effects , Hippocampus/metabolism , Mitochondria/drug effects , Mitochondria/metabolism , Sepsis/complications , Sepsis/drug therapy , Sepsis/metabolism , Mice, Inbred C57BL , Membrane Potential, Mitochondrial/drug effects , Maze Learning/drug effects
13.
Bioresour Technol ; 412: 131414, 2024 Nov.
Article in English | MEDLINE | ID: mdl-39226941

ABSTRACT

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.


Subject(s)
Electrodes , Hydrogen , Methane , Microbiota , Anaerobiosis , Hydrogen/metabolism , Methane/metabolism , Microbiota/physiology , Gases , Sewage/microbiology , Biofuels , Electrochemical Techniques/methods , Biofilms
14.
Bioresour Technol ; 412: 131432, 2024 Nov.
Article in English | MEDLINE | ID: mdl-39236909

ABSTRACT

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.


Subject(s)
Autotrophic Processes , Benzopyrans , Denitrification , Hydrogen , Hydrogen/metabolism , Nitrates/metabolism , Nitrogen , Bacteria/metabolism , Electrochemical Techniques/methods
15.
Int J Mol Sci ; 25(18)2024 Sep 16.
Article in English | MEDLINE | ID: mdl-39337477

ABSTRACT

Proteins form the fastest-growing therapeutic class. Due to their intrinsic instability, loss of native structure is common. Structure alteration must be carefully evaluated as structural changes may jeopardize the efficiency and safety of the protein-based drugs. Hydrogen deuterium exchange (HDX) has long been used to evaluate protein structure and dynamics. The rate of exchange constitutes a sensitive marker of the conformational state of the protein and of its stability. It is often monitored by mass spectrometry. Fourier transform infrared (FTIR) spectroscopy is another method with very promising capabilities. Combining protein microarrays with FTIR imaging resulted in high throughput HDX FTIR measurements. BaF2 slides bearing the protein microarrays were covered by another slide separated by a spacer, allowing us to flush the cell continuously with a flow of N2 gas saturated with 2H2O. Exchange occurred simultaneously for all proteins and single images covering ca. 96 spots of proteins that could be recorded on-line at selected time points. Each protein spot contained ca. 5 ng protein, and the entire array covered 2.5 × 2.5 mm2. Furthermore, HDX could be monitored in real time, and the experiment was therefore not subject to back-exchange problems. Analysis of HDX curves by inverse Laplace transform and by fitting exponential curves indicated that quantitative comparison of the samples is feasible. The paper also demonstrates how the whole process of analysis can be automatized to yield fast analyses.


Subject(s)
Deuterium Exchange Measurement , Protein Array Analysis , Spectroscopy, Fourier Transform Infrared/methods , Deuterium Exchange Measurement/methods , Protein Array Analysis/methods , Proteins/chemistry , Hydrogen/chemistry
16.
Environ Sci Pollut Res Int ; 31(42): 54920-54937, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39215922

ABSTRACT

The preparation of highly active, rare earth, non-platinum-based catalysts for hydrogen evolution reactions (HER) in alkaline solutions would be useful in realizing green hydrogen production technology. Perovskite oxides are generally regarded as low-active HER catalysts, owing to their unsuitable hydrogen adsorption and water dissociation. In this article, we report on the synthesis of Li2ZrO3 perovskites substituted with samarium and terbium cations at A-sites for the HER. LSmZrO3 (LSmZO) and LTbZrO3 (LTbZO) perovskite oxides are more affordable materials, starting materials in abundance, environmentally friendly due to reduced usage of precious metal and moreover have potential for several sustainable synthesis methods compared to commercial Pt/C. The surface and elemental composition of the prepared materials have been confirmed by X-ray photoelectron spectroscopy (XPS). The morphology and composition analyses of the LSmZO and LTbZO catalysts showed spherical and regular particles, respectively. The electrochemical measurements were used to study the catalytic performance of the prepared catalyst for hydrogen evolution reactions in an alkaline solution. LTbZO generated 2.52 mmol/g/h hydrogen, whereas LSmZO produced 3.34 mmol/g/h hydrogen using chronoamperometry. This was supported by the fact that the HER electrocatalysts exhibited a Tafel slope of less than 120 mV/dec in a 1.0 M alkaline solution. A current density of 10 mA/cm2 is achieved at a potential of less than 505 mV. The hydrogen production rate of LTbZO was only 58.55%, whereas LSmZO had a higher Faradaic efficiency of 97.65%. The EIS results demonstrated that HER was highly beneficial to both electrocatalysts due to the relatively small charge transfer resistance and higher capacitance values.


Subject(s)
Calcium Compounds , Hydrogen , Oxides , Samarium , Terbium , Titanium , Hydrogen/chemistry , Catalysis , Titanium/chemistry , Oxides/chemistry , Calcium Compounds/chemistry , Terbium/chemistry , Samarium/chemistry
17.
ISME J ; 18(1)2024 Jan 08.
Article in English | MEDLINE | ID: mdl-39163484

ABSTRACT

Hydrothermal vent systems release reduced chemical compounds that act as an important energy source in the deep sea. Chemolithoautotrophic microbes inhabiting hydrothermal plumes oxidize these compounds, in particular, hydrogen and reduced sulfur, to obtain the energy required for CO2 fixation. Here, we analysed the planktonic communities of four hydrothermal systems located along the Mid-Atlantic Ridge: Irinovskoe, Semenov-2, Logatchev-1, and Ashadze-2, by combining long-read 16S rRNA gene analysis, fluorescence in situ hybridization, meta-omics, and thermodynamic calculations. Sulfurimonas and SUP05 dominated the microbial communities in these hydrothermal plumes. Investigation of Sulfurimonas and SUP05 MAGs, and their gene transcription in plumes indicated a niche partitioning driven by hydrogen and sulfur. In addition to sulfur and hydrogen oxidation, a novel SAR202 clade inhabiting the plume, here referred to as genus Carboxydicoccus, harbours the capability for CO oxidation and CO2 fixation via reverse TCA cycle. Both pathways were also highly transcribed in other hydrogen-rich plumes, including the Von Damm vent field. Carboxydicoccus profundi reached up to 4% relative abundance (1.0 x 103 cell ml- 1) in Irinovskoe non-buoyant plume and was also abundant in non-hydrothermally influenced deep-sea metagenomes (up to 5 RPKM). Therefore, CO, which is probably not sourced from the hydrothermal fluids (1.9-5.8 µM), but rather from biological activities within the rising fluid, may serve as a significant energy source in hydrothermal plumes. Taken together, this study sheds light on the chemolithoautotrophic potential of the bacterial community in Mid-Atlantic Ridge plumes.


Subject(s)
Bacteria , Chemoautotrophic Growth , Hydrothermal Vents , RNA, Ribosomal, 16S , Seawater , Hydrothermal Vents/microbiology , Atlantic Ocean , RNA, Ribosomal, 16S/genetics , Bacteria/genetics , Bacteria/classification , Bacteria/isolation & purification , Seawater/microbiology , Microbiota , Hydrogen/metabolism , Phylogeny , Sulfur/metabolism , Oxidation-Reduction , In Situ Hybridization, Fluorescence , Carbon Dioxide/metabolism
18.
mSystems ; 9(9): e0014824, 2024 Sep 17.
Article in English | MEDLINE | ID: mdl-39166872

ABSTRACT

Enhancing the availability of representative isolates from hydrothermal vents (HTVs) is imperative for comprehending the microbial processes that propel the vent ecosystem. In recent years, Campylobacteria have emerged as the predominant and ubiquitous taxon across both shallow and deep-sea vent systems. Nevertheless, only a few isolates have been cultured, primarily originating from deep-sea HTVs. Presently, no cultivable isolates of Campylobacteria are accessible in shallow water vent systems (<200 m), which exhibit markedly distinct environmental conditions from their deep-sea counterparts. In this study, we enriched a novel isolate (genus Sulfurospirillum, Campylobacteria) from shallow-water HTVs of Kueishan Island. Genomic and physiological analysis revealed that this novel Campylobacteria species grows on a variety of substrate and carbon/energy sources. The pan-genome and phenotypic comparisons with 12 previously isolated Sulfurospirillum species from different environments supported the identification of functional features in Sulfurospirillum genomes crucial for adaptation to vent environments, such as sulfur oxidation, carbon fixation, biofilm formation, and benzoate/toluene degradation, as well as diverse genes related with signal transportation. To conclude, the metabolic characteristics of this novel Campylobacteria augment our understanding of Campylobacteria spanning from deep-sea to shallow-water vent systems.IMPORTANCECampylobacteria emerge as the dominant and ubiquitous taxa within vent systems, playing important roles in the vent ecosystems. However, isolated representatives of Campylobacteria have been mainly from the deep-sea hydrothermal fields, leaving a significant knowledge gap regarding the functions, activities, and adaptation strategies of the vent microorganisms in shallow-water hydrothermal vents (HTVs). This study bridges this gap by providing insights into the phenomics and genomic diversity of genus Sulfurospirillum (order Campylobacterales, class Campylobacteria) based on data derived from a novel isolate obtained from shallow-water HTVs. Our mesophilic isolate of Sulfurospirillum not only augments the genus diversity of Campylobacteria pure cultures derived from vent systems but also serves as the inaugural reference isolate for Campylobacteria in shallow-water environments.


Subject(s)
Epsilonproteobacteria , Hydrogen , Hydrothermal Vents , Oxidation-Reduction , Hydrothermal Vents/microbiology , Hydrogen/metabolism , Epsilonproteobacteria/genetics , Epsilonproteobacteria/isolation & purification , Epsilonproteobacteria/metabolism , Epsilonproteobacteria/classification , Genome, Bacterial/genetics , Phylogeny , Adaptation, Physiological , Chemoautotrophic Growth
19.
mSystems ; 9(9): e0099924, 2024 Sep 17.
Article in English | MEDLINE | ID: mdl-39189956

ABSTRACT

Hydrogenedentota, a globally distributed bacterial phylum-level lineage, is poorly understood. Here, we established a comprehensive genomic catalog of Hydrogenedentota, including a total of seven clades (or families) with 179 genomes, and explored the metabolic potential and evolutionary history of these organisms. We show that a single genome, especially those belonging to Clade 6, often encodes multiple hydrogenases with genomes in Clade 2, which rarely encode hydrogenases being the exception. Notably, most members of Hydrogenedentota contain a group A3 [FeFe]-hydrogenase (BfuABC) with a non-canonical electron bifurcation mechanism, in addition to substrate-level phosphorylation and electron transport-linked phosphorylation pathways, in energy conservation. Furthermore, we show that BfuABC from Hydrogenedentota fall into five sub-types. Phylogenetic analysis reveals five independent routes for the evolution of BfuABC homologs in Hydrogenedentota. We speculate that the five sub-types of BfuABC might be acquired from Bacillota (synonym Firmicutes) through separate horizontal gene transfer events. These data shed light on the diversity and evolution of bifurcating [FeFe]-hydrogenases and provide insight into the strategy of Hydrogenedentota to adapt to survival in various habitats. IMPORTANCE: The phylum Hydrogenedentota is widely distributed in various environments. However, their physiology, ecology, and evolutionary history remain unknown, primarily due to the limited availability of the genomes and the lack of cultured representatives of the phylum. Our results have increased the knowledge of the genetic and metabolic diversity of these organisms and shed light on their diverse energy conservation strategies, especially those involving electron bifurcation with a non-canonical mechanism, which are likely responsible for their wide distribution. Besides, the organization and phylogenetic relationships of gene clusters coding for BfuABC in Hydrogenedentota provide valuable clues to the evolutionary history of group A3 electron bifurcating [FeFe]-hydrogenases.


Subject(s)
Evolution, Molecular , Hydrogenase , Iron-Sulfur Proteins , Phylogeny , Hydrogenase/genetics , Hydrogenase/metabolism , Hydrogenase/chemistry , Iron-Sulfur Proteins/genetics , Iron-Sulfur Proteins/metabolism , Bacterial Proteins/genetics , Bacterial Proteins/metabolism , Bacterial Proteins/chemistry , Bacteria/genetics , Bacteria/enzymology , Genome, Bacterial , Hydrogen/metabolism , Gene Transfer, Horizontal
20.
Sci Total Environ ; 951: 175673, 2024 Nov 15.
Article in English | MEDLINE | ID: mdl-39168318

ABSTRACT

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.


Subject(s)
Biodegradation, Environmental , Fermentation , Hydrogen , Tetracycline , Waste Disposal, Fluid , Water Pollutants, Chemical , Hydrogen/metabolism , Anaerobiosis , Waste Disposal, Fluid/methods , Water Pollutants, Chemical/metabolism , Water Pollutants, Chemical/analysis , Wastewater , Anti-Bacterial Agents/metabolism , Microbiota , Bacteria/metabolism
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