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1.
Environ Sci Technol ; 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38966939

RESUMO

The effect of Zn on Cd accumulation in rice varies under flooding and drainage conditions, and the underlying mechanism during uptake and transport from the soil to grains remains unclear. Isotope fractionation and gene expression were investigated using pot experiments under distinct water regimes and with Zn addition to gain a deeper understanding of the molecular effects of Zn on Cd uptake and transport in rice. The higher OsHMA2 expression but constitutively lower expression of zinc-regulated, iron-regulated transporter-like protein (ZIP) family genes in roots under the drainage regime than the flooding regime caused the enrichment of nonheavy Zn isotopes in the shoots relative to roots but minimally affected Cd isotopic fractionation. Drainage regime seem to exert a striking effect on the root-to-shoot translocation of Zn rather than Cd, and increased Zn transport via OsHMA2. The changes in expression patterns in response to Zn addition were similar to those observed upon switching from the flooding to drainage regime, except for OsNRAMP1 and OsNRAMP5. However, soil solution-to-rice plants and root-to-shoot fractionation toward light Zn isotopes with Zn addition (Δ66Znrice plant-soil solution = -0.49 to -0.40‰, Δ66Znshoot-root = -0.36 to -0.27‰) indicated that Zn transport occurred via nonspecific uptake pathways and OsHMA2, respectively. Accordingly, the less pronounced and minimally varied Cd isotope fractionation suggested that OsNRAMP5 and OsHMA2 are crucial for Cd uptake and root-to-shoot transport, respectively, facilitating Cd accumulation in grains. This study demonstrated that a high Zn supply promotes Cd uptake and root-to-shoot transport in rice by sharing distinct pathways, and by utilizing a non-Zn-sensitive pathway with a high affinity for Cd.

2.
RSC Adv ; 14(30): 21623-21634, 2024 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-38979472

RESUMO

Carbon nanofiber membranes (CNMs) are expected to be used in many energy devices to improve the reaction rate. In this paper, CNMs embedded with palladium nanoparticles (Pd-CNMs) were prepared by electrospinning and carbonization using polyimide as the raw material. The effects of carbonization temperature, carbonization atmosphere, and heating rate on the physicochemical properties of the as-obtained Pd-CNMs were studied in detail. On this basis, the electrocatalytic performance of Pd-CNMs prepared under optimal conditions was characterized. The results showed that highly active zero-valent palladium nanoparticles with uniform particle size could be distributed on the surface of carbon nanofibers. Under vacuum conditions, at a carbonization temperature of 800 °C and a heating rate of 2 °C min-1, Pd-CNMs have lower H2O2 yield, lower Tafel slope (73.3 mV dec-1), higher electron transfer number (∼4), and superior durability, suggesting that Pd-CNMs exhibit excellent electrocatalytic activity for ORR in alkaline electrolyte. Therefore, polyimide-derived CNMs embedded with Pd nanoparticles are expected to become an excellent cathode catalyst layer for fuel cells.

3.
Adv Med Sci ; 2024 Jul 08.
Artigo em Inglês | MEDLINE | ID: mdl-38986767

RESUMO

PURPOSE: Idiopathic pulmonary fibrosis (IPF), a chronic and progressively worsening condition characterized by interstitial lung inflammation and fibrosis of unknown etiology, has a grim prognosis. The treatment options for IPF are limited and new therapeutic strategies are urgently needed. Dietary restriction can improve various inflammatory diseases, but its therapeutic effect on bleomycin (BLM)-induced pulmonary fibrosis mouse model remains unclear. This study aims to investigate whether intermittent fasting (IF) can alleviate BLM-induced pulmonary inflammation and fibrosis. METHODS: Pulmonary fibrosis mouse models were induced by BLM. The IF group underwent 24-hour fasting cycles for one week prior and three weeks following BLM administration. Meanwhile, the ad libitum feeding group had unrestricted access to food throughout the experiment. The evaluation focused on lung pathology via histological staining, qPCR analysis of collagen markers, and immune cell profiling through flow cytometry. RESULTS: IF group significantly reduced inflammation and fibrosis in lung tissues of BLM-induced mice compared to ad libitum feeding group. qPCR results showed IF remarkably decreased the mRNA expression of Col 1a and Col 3a in the lungs of BLM-induced mouse models. IF also reduced the numbers of regulatory T cells (Tregs), T helper 17 (Th17) cells, monocytes, and monocyte-derived alveolar macrophages (MoAMs) in the lung tissues. CONCLUSIONS: IF may improve BLM-induced pulmonary fibrosis by decreasing numbers of immune cells including Treg cells, Th17 cells, monocytes, and MoAMs in the lungs. This study offers experimental validation for dietary intervention as a viable treatment modality in IPF management.

4.
Nat Commun ; 15(1): 5737, 2024 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-38982157

RESUMO

Exploring the promiscuity of native enzymes presents a promising strategy for expanding their synthetic applications, particularly for catalyzing challenging reactions in non-native contexts. In this study, we explore the promiscuous potential of old yellow enzymes (OYEs) to facilitate the Morita-Baylis-Hillman reaction (MBH reaction), leveraging substrate similarities between MBH reaction and reduction reaction. Using mass spectrometry and spectroscopic techniques, we confirm promiscuity of GkOYE in both MBH and reduction reactions. By blocking H- and H+ transfer pathways, we engineer GkOYE.8, which loses its reduction ability but enhances its MBH activity. The structural basis of MBH reaction catalyzed by GkOYE.8 is obtained through mutation studies and kinetic simulations. Furthermore, enantiocomplementary mutants GkOYE.11 and GkOYE.13 are obtained by directed evolution, exhibiting the ability to accept various aromatic aldehydes and alkenes as substrates. This study demonstrates the potential of leveraging substrate similarities to unlock enzyme functionalities, enabling the catalysis of new-to-nature reactions.


Assuntos
Biocatálise , Especificidade por Substrato , Cinética , Aldeídos/metabolismo , Aldeídos/química , Catálise , Mutação , Alcenos/metabolismo , Alcenos/química , Proteínas de Bactérias/metabolismo , Proteínas de Bactérias/genética , Proteínas de Bactérias/química , Engenharia de Proteínas
5.
Food Chem ; 457: 140165, 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38936118

RESUMO

Para-hydroxybenzoic acid (PHBA) is extensively used as an additive in the food and cosmetics industries, significantly enhancing product shelf life and stability. While microbial fermentation offers an environment-friendly and sustainable method for producing PHBA, the titer and productivity are limited due to product toxicity and complex metabolic flux distributions. Here, we initially redesigned a L-phenylalanine-producing Escherichia coli by employing rational metabolic engineering strategies, resulting in the production of PHBA reached the highest reported level of 14.17 g/L. Subsequently, a novel accelerated evolution system was devised comprising deaminase, the alpha subunit of RNA polymerase, an uracil-DNA glycosylase inhibitor, and the PHBA-responsive promoter PyhcN. This system enabled us to obtain a mutant strain exhibiting a 47% increase in the half-inhibitory concentration (IC50) for PHBA within 15 days. Finally, the evolved strain achieved a production of 21.35 g/L PHBA in a 5-L fermenter, with a yield of 0.19 g/g glucose and a productivity rate of 0.44 g/L/h. This engineered strain emerges as a promising candidate for industrial production of PHBA through an eco-friendly approach.

6.
Materials (Basel) ; 17(11)2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38893745

RESUMO

Precast ultra-high-performance concrete (UHPC) has emerged as indispensable in the engineering sector due to its cost-effectiveness and superior performance. Currently, precast UHPC grapples with challenges pertaining to slow setting times and insufficient early strength, largely attributed to its high water-reducing agent content. Effective utilization of early strength agents to augment UHPC's early strength is pivotal in addressing this issue. This study investigates the efficacy of two distinct concrete early strength agents, namely calcium formate (Ca(HCO2)2) and aluminum sulfate (Al2(SO4)3). A UHPC system with a water/cement ratio of 0.17 was used; both single and compound doping experiments were conducted using varied dosages of the aforementioned early strength agents. Our results show that both early strength agents significantly reduce setting time and enhance early strength at appropriate dosages. Specifically, the addition of 0.3% Ca(HCO2)2 led to a 33.07% decrease in setting time for UHPC. Moreover, the incorporation of 0.3% Ca(HCO2)2 and 0.5% Al2(SO4)3 resulted in a strength of 81.9 MPa at 1.5 days, representing a remarkable increase of 118.4%. It is noteworthy that excessive use of Ca(HCO2)2 inhibits the hydration process, whereas an abundance of Al2(SO4)3 diminishes the early strength effect. Simultaneously, this article provides recommendations regarding the dosage of two distinct early strength agents, offering a novel solution for expediting the production of prefabricated UHPC with a low water/cement ratio and high water-reducing agent content.

7.
ACS Nano ; 18(25): 16113-16125, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38857428

RESUMO

Urinary extracellular vesicles (uEVs) are regarded as highly promising liquid-biopsy biomarkers for the early diagnosis and prognosis of bladder cancer (BC). However, detection of uEVs remains technically challenging owing to their huge heterogeneity and ultralow abundance in real samples. We herein present a choline phosphate-grafted platinum nanozyme (Pt@CP) that acts as a universal EV probe for the construction of a high-throughput and high-sensitivity immunoassay, which allowed multiplex profiling of uEV protein markers for BC detection. With the Pt@CP-based immunoassays, three uEV protein markers (MUC-1, CCDC25, and GLUT1) were identified for BC, by which the BC cases (n = 48), cystitis patients (n = 27), and healthy donors (n = 24) were discriminated with high clinical sensitivity and specificity (area under curve = 98.3%). For the BC cases (n = 9) after surgery, the Pt@CP-based immunoassay could report the postoperative residual tumor that cannot be observed by cystoscopy, which is clinically significant for assessing BC recurrence. This work provides generally high sensitivity for EV detection, facilitating the discovery and clinical use of EV-based biomarkers.


Assuntos
Biomarcadores Tumorais , Vesículas Extracelulares , Neoplasias da Bexiga Urinária , Neoplasias da Bexiga Urinária/diagnóstico , Neoplasias da Bexiga Urinária/patologia , Humanos , Vesículas Extracelulares/química , Biomarcadores Tumorais/análise , Fosforilcolina/química , Imunoensaio/métodos , Platina/química , Feminino
8.
Chem Commun (Camb) ; 60(53): 6777-6780, 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38868861

RESUMO

D-UiO-66-NIM with high proton conductivity has been synthesized through the dual strategy of defect engineering and ligand modification. Moreover, D-UiO-66-NIM exhibits good temperature cycling stability and durability in proton conductivity. This work has developed a new method to obtain efficient MOF-based proton conductors.

9.
Cell Res ; 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38898113

RESUMO

The shift of carbon utilization from primarily glucose to other nutrients is a fundamental metabolic adaptation to cope with decreased blood glucose levels and the consequent decline in glucose oxidation. AMP-activated protein kinase (AMPK) plays crucial roles in this metabolic adaptation. However, the underlying mechanism is not fully understood. Here, we show that PDZ domain containing 8 (PDZD8), which we identify as a new substrate of AMPK activated in low glucose, is required for the low glucose-promoted glutaminolysis. AMPK phosphorylates PDZD8 at threonine 527 (T527) and promotes the interaction of PDZD8 with and activation of glutaminase 1 (GLS1), a rate-limiting enzyme of glutaminolysis. In vivo, the AMPK-PDZD8-GLS1 axis is required for the enhancement of glutaminolysis as tested in the skeletal muscle tissues, which occurs earlier than the increase in fatty acid utilization during fasting. The enhanced glutaminolysis is also observed in macrophages in low glucose or under acute lipopolysaccharide (LPS) treatment. Consistent with a requirement of heightened glutaminolysis, the PDZD8-T527A mutation dampens the secretion of pro-inflammatory cytokines in macrophages in mice treated with LPS. Together, we have revealed an AMPK-PDZD8-GLS1 axis that promotes glutaminolysis ahead of increased fatty acid utilization under glucose shortage.

10.
Shock ; 2024 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-38899838

RESUMO

ABSTRACT: Sepsis is a highly prevalent and deadly disease. Currently, there is a lack of ideal biomarker prognostis models for sepsis. We attempt to construct a model capable of predicting the prognosis of sepsis patients by integrating transcriptomic and proteomic data. Through analysis of proteomic and transcriptomic data, we identified 25 differentially expressed genes (DEGs). Single-factor Cox-Lasso regression analysis identified 16 DEGs (OS-DEGs) associated with patient prognosis. Through multi-factor Cox-Lasso regression analysis, a prognostic model based on these 16 genes was constructed. Kaplan-Meier (K-M) survival analysis and receiver operating characteristic (ROC) curve analysis were used to further validate the high stability and good predictive ability of this prognostic model with internal and external data. Gene Ontology (GO) and Kyoto Encyclopedia of Genes and Genomes (KEGG) pathway enrichment analysis of OS-DEGs and differentially expressed genes between high and low-risk groups based on the prognostic model revealed significant enrichment in immune-related pathways, particularly those associated with viral regulation.

11.
J Mol Cell Cardiol ; 194: 3-15, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38844061

RESUMO

Diabetic cardiomyopathy (DCM) is a heart failure syndrome, and is one of the major causes of morbidity and mortality in diabetes. DCM is mainly characterized by ventricular dilation, myocardial hypertrophy, myocardial fibrosis and cardiac dysfunction. Clinical studies have found that insulin resistance is an independent risk factor for DCM. However, its specific mechanism of DCM remains unclear. 8-hydroxyguanine DNA glycosylase 1(OGG1)is involved in DNA base repair and the regulation of inflammatory genes. In this study, we show that OGG1 was associated with the occurrence of DCM. for the first time. The expression of OGG1 was increased in the heart tissue of DCM mice, and OGG1 deficiency aggravated the cardiac dysfunction of DCM mice. Metabolomics show that OGG1 deficiency resulted in obstruction of glycolytic pathway. At the molecular level, OGG1 regulated glucose uptake and insulin resistance by interacting with PPAR-γ in vitro. In order to explore the protective effect of exogenous OGG1 on DCM, OGG1 adeno-associated virus was injected into DCM mice through tail vein in the middle stage of the disease. We found that the overexpression of OGG1 could improve cardiac dysfunction of DCM mice, indicating that OGG1 had a certain therapeutic effect on DCM. These results demonstrate that OGG1 is a new molecular target for the treatment of DCM and has certain clinical significance.

12.
ACS Synth Biol ; 13(6): 1879-1892, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38847341

RESUMO

Aromatic d-amino acids (d-AAs) play a pivotal role as important chiral building blocks and key intermediates in fine chemical and drug synthesis. Meso-diaminopimelate dehydrogenase (DAPDH) serves as an excellent biocatalyst in the synthesis of d-AAs and their derivatives. However, its strict substrate specificity and the lack of efficient engineering methods have hindered its widespread application. Therefore, this study aims to elucidate the catalytic mechanism underlying DAPDH from Proteus vulgaris (PvDAPDH) through the examination of its crystallographic structure, computational simulations of potential energies and molecular dynamics simulations, and site-directed mutagenesis. Mechanism-guided computational design showed that the optimal mutant PvDAPDH-M3 increased specific activity and catalytic efficiency (kcat/Km) for aromatic keto acids up to 124-fold and 92.4-fold, respectively, compared to that of the wild type. Additionally, it expanded the substrate scope to 10 aromatic keto acid substrates. Finally, six high-value-added aromatic d-AAs and their derivatives were synthesized using a one-pot three-enzyme cascade reaction, exhibiting a good conversion rate ranging from 32 to 84% and excellent stereoselectivity (enantiomeric excess >99%). These findings provide a potential synthetic pathway for the green industrial production of aromatic d-AAs.


Assuntos
Aminoácido Oxirredutases , Aminoácidos Aromáticos , Simulação de Dinâmica Molecular , Mutagênese Sítio-Dirigida , Aminoácido Oxirredutases/metabolismo , Aminoácido Oxirredutases/genética , Aminoácido Oxirredutases/química , Especificidade por Substrato , Aminoácidos Aromáticos/metabolismo , Aminoácidos Aromáticos/biossíntese , Proteus vulgaris/enzimologia , Proteus vulgaris/genética , Biocatálise , Proteínas de Bactérias/genética , Proteínas de Bactérias/metabolismo , Proteínas de Bactérias/química
13.
Biochim Biophys Acta Mol Cell Res ; 1871(7): 119785, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38885843

RESUMO

We previously reported that integrin alpha 7 (ITGA7) was downregulated in colorectal cancer (CRC) tissues and CRC cell lines and that the lower expression of ITGA7 in CRC tissues was correlated with distant metastasis, suggesting that ITGA7 may function as a suppressor in CRC. The present research was conducted to further investigate the role and mechanisms of ITGA7 in CRC progression. First, bisulfite modification and genomic sequencing (BSP) results showed that the methylation rate of ITGA7 promoter was higher in 10 CRC tissues than in the matched normal tissues. Additionally, 5-Aza-CdR treatment increased ITGA7 expression in CRC cells. Gain-of-function assays revealed the inhibitory role of ITGA7 in CRC cell proliferation and migration. Mechanistically, RNA sequencing, RT-qPCR, and cytoplasm and nuclear separation and rescue assays indicated that knockdown of ITGA7 activated the transcription of MMP9, SETD7, and ADAM15 by enhancing the nuclear translocation of NF-κB. Moreover, CoIP and Western blot suggested a mechanistic model in which ITGA7 binds to CKAP4 to block the interaction of CKAP4 and PI3K p85α and thereby suppress the PI3K/AKT/NF-κB pathway. Accordingly, the current study suggests that ITGA7 functions as a suppressor in CRC progression and that its expression is controlled by promoter methylation.

14.
Adv Mater ; : e2403881, 2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38899836

RESUMO

Xenes, mono-elemental atomic sheets, exhibit Dirac/Dirac-like quantum behavior. When interfaced with other 2D materials such as boron nitride, transition metal dichalcogenides, and metal carbides/nitrides/carbonitrides, it enables them with unique physicochemical properties, including structural stability, desirable bandgap, efficient charge carrier injection, flexibility/breaking stress, thermal conductivity, chemical reactivity, catalytic efficiency, molecular adsorption, and wettability. For example, BN acts as an anti-oxidative shield, MoS2 injects electrons upon laser excitation, and MXene provides mechanical flexibility. Beyond precise compositional modulations, stacking sequences, and inter-layer coupling controlled by parameters, achieving scalability and reproducibility in hybridization is crucial for implementing these quantum materials in consumer applications. However, realizing the full potential of these hybrid materials faces challenges such as air gaps, uneven interfaces, and the formation of defects and functional groups. Advanced synthesis techniques, a deep understanding of quantum behaviors, precise control over interfacial interactions, and awareness of cross-correlations among these factors are essential. Xene-based hybrids show immense promise for groundbreaking applications in quantum computing, flexible electronics, energy storage, and catalysis. In this timely perspective, recent discoveries of novel Xenes and their hybrids are highlighted, emphasizing correlations among synthetic parameters, structure, properties, and applications. It is anticipated that these insights will revolutionize diverse industries and technologies.

15.
Arch Dermatol Res ; 316(5): 176, 2024 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-38758283

RESUMO

Psoriasis is a chronic immune mediated inflammatory skin disease with systemic manifestations. It has been reported that caloric restriction could improve severity of psoriasis patients. However, the mechanism of intermittent fasting effects on psoriasis has not been investigated. Caloric restriction is known to reduce the number of circulating inflammatory monocytes in a CCL2-dependent manner. However, it is still unknown whether caloric restriction can improve psoriasis by regulating monocytes through CCL2. In this study, we used imiquimod (IMQ)-induced psoriasis-like mouse model to explore the effects and the mechanisms of intermittent fasting on psoriasis-like dermatitis. We found that intermittent fasting could significantly improve IMQ-induced psoriasis-like dermatitis, and reduce the number of γδT17 cells and IL-17 production in draining lymph nodes and psoriatic lesion via inhibiting proliferation and increasing death of γδT17 cells. Furthermore, intermittent fasting could significantly decrease monocytes in blood, and this was associated with decreased monocytes, macrophages and DC in psoriasis-like skin inflammation. Reduced monocytes in circulation and increased monocytes in BM of fasting IMQ-induced psoriasis-like mice is through reducing the production of CCL2 from BM to inhibit monocyte egress to the periphery. Our above data shads light on the mechanisms of intermittent fasting on psoriasis.


Assuntos
Quimiocina CCL2 , Modelos Animais de Doenças , Jejum , Imiquimode , Monócitos , Psoríase , Animais , Psoríase/imunologia , Psoríase/induzido quimicamente , Psoríase/patologia , Monócitos/imunologia , Monócitos/metabolismo , Camundongos , Jejum/sangue , Quimiocina CCL2/metabolismo , Células Th17/imunologia , Interleucina-17/metabolismo , Pele/patologia , Pele/imunologia , Humanos , Camundongos Endogâmicos C57BL , Masculino , Proliferação de Células , Restrição Calórica , Jejum Intermitente
16.
Chembiochem ; 25(11): e202400142, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38742957

RESUMO

The widespread attention towards 1,4-butanediol (BDO) as a key chemical raw material stems from its potential in producing biodegradable plastics. However, the efficiency of its biosynthesis via current bioprocesses is limited. In this study, a dual-pathway approach for 1,4-BDO production from succinic acid was developed. Specifically, a double-enzyme catalytic pathway involving carboxylic acid reductase and ethanol dehydrogenase was proposed. Optimization of the expression levels of the pathway enzymes led to a significant 318 % increase in 1,4-BDO titer. Additionally, the rate-limiting enzyme MmCAR was engineered to enhance the kcat/KM values by 50 % and increase 1,4-BDO titer by 46.7 %. To address cofactor supply limitations, an NADPH and ATP cycling system was established, resulting in a 48.9 % increase in 1,4-BDO production. Ultimately, after 48 hours, 1,4-BDO titers reached 201 mg/L and 1555 mg/L in shake flask and 5 L fermenter, respectively. This work represents a significant advancement in 1,4-BDO synthesis from succinic acid, with potential applications in the organic chemical and food industries.


Assuntos
Butileno Glicóis , Escherichia coli , Ácido Succínico , Butileno Glicóis/metabolismo , Butileno Glicóis/química , Ácido Succínico/metabolismo , Ácido Succínico/química , Escherichia coli/metabolismo , Escherichia coli/genética , Biocatálise , Álcool Desidrogenase/metabolismo , Oxirredutases/metabolismo , Oxirredutases/genética , Fermentação
17.
Environ Sci Technol ; 58(25): 11003-11015, 2024 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-38807562

RESUMO

Labile organic matter (OM) immobilized by secondary iron (Fe) minerals from chemodenitrification may be an effective way to immobilize organic carbon (OC). However, the underlying mechanisms of coupled chemodenitrification and OC sequestration are poorly understood. Here, OM immobilization by secondary Fe minerals from chemodenitrification was investigated at different C/Fe ratios. Kinetics of Fe(II) oxidation and nitrite reduction rates decreased with increasing C/Fe ratios. Despite efficient sequestration, the immobilization efficiency of OM by secondary minerals varied with the C/Fe ratios. Higher C/Fe ratios were conducive to the formation of ferrihydrite and lepidocrocite, with defects and nanopores. Three contributions, including inner-core Fe-O and edge- and corner-shared Fe-Fe interactions, constituted the local coordination environment of mineral-organic composites. Microscopic analysis at the molecular scale uncovered that labile OM was more likely to combine with secondary minerals with poor crystallinity to enhance its stability, and OM distributed within nanopores and defects had a higher oxidation state. After chemodenitrification, high molecular weight substances and substances high in unsaturation or O/C ratios including phenols, polycyclic aromatics, and carboxylic compounds exhibited a stronger affinity to Fe minerals in the treatments with lower C/Fe ratios. Collectively, labile OM immobilization can occur during chemodenitrification. The findings on OM sequestration coupled with chemodenitrification have significant implications for understanding the long-term cycling of Fe, C, and N, providing a potential strategy for OM immobilization in anoxic soils and sediments.


Assuntos
Ferro , Minerais , Minerais/química , Ferro/química , Oxirredução , Carbono/química , Cinética
18.
ACS Synth Biol ; 13(6): 1820-1830, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38767944

RESUMO

Cadaverine is a critical C5 monomer for the production of polyamides. Pyridoxal 5'-phosphate (PLP), as a crucial cofactor for the key enzyme lysine decarboxylase in the cadaverine biosynthesis pathway, has seen a persistent shortage, leading to limitations in cadaverine production. To address this issue, a dual-pathway strategy was implemented, synergistically enhancing both endogenous and heterologous PLP synthesis modules and resulting in improved PLP synthesis. Subsequently, a growth-stage-dependent molecular switch was introduced to balance the precursor competition between PLP synthesis and cell growth. Additionally, a PLP sensor-based negative feedback circuit was constructed by integrating a newly identified PLP-responsive promoter PygjH and an arabinose-regulated system, dynamically regulating the expression of the PLP synthetic genes and preventing excessive intracellular PLP accumulation. The optimal strain, L18, cultivated in the minimal medium AM1, demonstrated cadaverine production with a titer, yield, and productivity of 64.03 g/L, 0.23 g/g glucose, and 1.33 g/L/h, respectively. This represents the highest titer reported to date in engineered Escherichia coli by fed-batch fermentation in a minimal medium.


Assuntos
Cadaverina , Meios de Cultura , Escherichia coli , Engenharia Metabólica , Fosfato de Piridoxal , Cadaverina/metabolismo , Cadaverina/biossíntese , Fosfato de Piridoxal/metabolismo , Escherichia coli/genética , Escherichia coli/metabolismo , Engenharia Metabólica/métodos , Meios de Cultura/química , Regiões Promotoras Genéticas , Carboxiliases/genética , Carboxiliases/metabolismo
19.
J Hazard Mater ; 473: 134632, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38781852

RESUMO

Recent increases in organophosphate ester (OPE) application have led to their widespread presence, yet little is known about their temporal trends in food. This study collected milk samples from 13 countries across three continents during 2020-2023, finding detectable OPEs in all samples (range: 2.25-19.7; median: 7.06 ng/g ww). Although no statistical temporal differences were found for the total OPEs during the 4-year sampling campaign, it was interesting to observe significant variations in the decreasing trend for Cl-OPEs and concentration variations for aryl-OPEs and alkyl-OPEs (p < 0.05), indicating changing OPE use patterns. Packaged milk exhibited significant higher OPE levels than those found in directly collected raw unpackaged milk, and milk with longer shelf-life showed higher OPE levels, revealing packaging material as a contamination source. No significant geographical differences were observed in milk across countries (p > 0.05), but Shandong Province, a major OPE production site in China, showed relatively higher OPE concentrations. The Monte Carlo simulation of estimated daily intakes indicated no exposure risk from OPEs through milk consumption. The molecular docking method was used to assess human hormone binding affinity with OPEs, amongst which aryl-OPEs had the highest binding energies. The Toxicological-Priority-Index method which integrated chemical property, detection frequency, risk quotients, hazardous quotients and endocrine-disrupting effects was employed to prioritize OPEs. Aryl-OPEs showed the highest scores, deserving attention in the future.


Assuntos
Contaminação de Alimentos , Leite , Leite/química , Animais , Humanos , Contaminação de Alimentos/análise , Ésteres/análise , Organofosfatos/análise , Simulação de Acoplamento Molecular
20.
Sci Total Environ ; 934: 173340, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38763201

RESUMO

Arsenic release and reduction in anoxic environments can be mitigated or facilitated by biochar amendment. However, the key fractions in biochars and how they control arsenic transformation remain poorly understood. In this study, a biochar produced from pomelo peel was rich in colloids and was used to evaluate the roles of the colloidal and residual fractions of biochar in arsenic transformation in anoxic paddy soil. Bulk biochar showed a markedly higher maximum adsorption capacity for As(III) at 1732 mg/kg than for As(V) at 75.7 mg/kg, mainly because of the colloidal fraction on the surface. When compared with the control and treatments with the colloidal/residual fraction, the addition of bulk biochar facilitated As(V) reduction and release in the soil during days 0-12, but decreased the dissolved As(III) concentration during days 12-20. The colloidal fraction revealed significantly higher electron donating capacity (8.26 µmole-/g) than that of bulk biochar (0.88 µmole-/g) and residual fraction (0.65 µmole-/g), acting as electron shuttle to promote As(V) reduction. Because the colloidal fraction was rich in aliphatic carbon, fulvic acid-like compounds, potassium, and calcium, it favored As(III) adsorption when more As(III) was released, probably via organic-cation-As(III) complexation. These findings provide deeper insight into the role of the colloidal fraction of biochar in controlling anaerobic arsenic transformation, which will be helpful for the practical application of biochar in arsenic-contaminated environments.


Assuntos
Arsênio , Carvão Vegetal , Poluentes do Solo , Solo , Carvão Vegetal/química , Arsênio/análise , Adsorção , Solo/química , Coloides/química , Citrus/química , Recuperação e Remediação Ambiental/métodos
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