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1.
ACS Nano ; 18(33): 22533-22547, 2024 Aug 20.
Article in English | MEDLINE | ID: mdl-39115190

ABSTRACT

Organic-inorganic hybrid metal halide perovskite solar cells have been considered as one of the most promising next-generation photovoltaic technologies. Nevertheless, perovskite defects and Li+ ionic migration will seriously affect the power conversion efficiency and stability of the formal device. Herein, we designed two crown ether derivatives (PC12 and PC15) with different cavity diameters, which selectively bind to different metal cations. It is found that PC15 in perovskite precursor solution can actively regulate the nucleation and crystallization processes and passivate the uncoordinated Pb2+ ions, while PC12 at the interface between the perovskite layer and hole-transporting layer can effectively inhibit the migration of Li+ ions and reduce nonradiative recombination losses. Therefore, PC12 and PC15 can act as "lubricant" and defect passivators, as well as inhibitors of ion migration, when they are synergistically applied at the surface and bulk of perovskite layer. Consequently, the optimized device achieved a champion efficiency of 24.8% with significantly improved humidity, thermal, and light stability.

2.
Adv Mater ; : e2406219, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39135405

ABSTRACT

In pulse power systems, multilayer ceramic capacitors (MLCCs) encounter significant challenges due to the heightened loading electric field (E), which can lead to fatigue damage and ultrasonic concussion caused by electrostrictive strain. To address these issues, an innovative strategy focused on achieving an ultra-weak polarization-strain coupling effect is proposed, which effectively reduces strain in MLCCs. Remarkably, an ultra-low electrostrictive coefficient (Q33) of 0.012 m4 C-2 is achieved in the composition 0.55(Bi0.5Na0.5)TiO3-0.45Pb(Mg1/3Nb2/3)O3, resulting in a significantly reduced strain of 0.118% at 330 kV cm-1. At the atomic scale, the local structural heterogeneity leads to an expanded and loose lattice structure, providing ample space for large ionic displacement polarization instead of lattice stretching when subjected to the applied E. This unique behavior not only promotes energy storage performance (ESP) but also accounts for the observed ultra-low Q33 and strain. Consequently, the MLCC device exhibits an impressive energy storage density of 14.6 J cm-3 and an ultrahigh efficiency of 93% at 720 kV cm-1. Furthermore, the superior ESP of the MLCC demonstrates excellent fatigue resistance and temperature stability, making it a promising solution for practical applications. Overall, this pivotal strategy offers a cost-effective solution for state-of-the-art MLCCs with ultra-low strain-vibration in pulse power systems.

3.
Food Chem ; 459: 140383, 2024 Nov 30.
Article in English | MEDLINE | ID: mdl-39003857

ABSTRACT

The traditional starch-based intelligent freshness labels struggle to maintain long-term structural stability when exposed to moisture. To solve this problem, we prepared composite crosslinked labels using phytic acid for double crosslinking of corn starch and soybean isolate proteins, with anthocyanin serving as the chromogenic dye. The mechanical properties, hydrophobic characteristics, and pH responsivity of these crosslinked labels were assessed in this study. The prepared double-crosslinked labels showed reduced moisture content (15.96%), diminished swelling (147.21%), decreased solubility (28.55%), and minimized water permeability, which suggested that they have enhanced hydrophobicity and densification. The crosslinked labels demonstrated the ability to maintain morphological stability when immersed in water for 12 h. Additionally, the mechanical properties of the crosslinked labels were enhanced without compromising their pH-sensing capabilities, demonstrated a color response visible to the naked eye for milk and coconut water freshness monitoring, suggesting great potential for application in beverages freshness monitoring.


Subject(s)
Beverages , Starch , Water , Starch/chemistry , Water/chemistry , Water/analysis , Beverages/analysis , Solubility , Hydrogen-Ion Concentration , Hydrophobic and Hydrophilic Interactions , Food Labeling , Anthocyanins/chemistry , Anthocyanins/analysis , Zea mays/chemistry
4.
J Cheminform ; 16(1): 67, 2024 Jun 07.
Article in English | MEDLINE | ID: mdl-38849874

ABSTRACT

Identification of interactions between chemical compounds and proteins is crucial for various applications, including drug discovery, target identification, network pharmacology, and elucidation of protein functions. Deep neural network-based approaches are becoming increasingly popular in efficiently identifying compound-protein interactions with high-throughput capabilities, narrowing down the scope of candidates for traditional labor-intensive, time-consuming and expensive experimental techniques. In this study, we proposed an end-to-end approach termed SPVec-SGCN-CPI, which utilized simplified graph convolutional network (SGCN) model with low-dimensional and continuous features generated from our previously developed model SPVec and graph topology information to predict compound-protein interactions. The SGCN technique, dividing the local neighborhood aggregation and nonlinearity layer-wise propagation steps, effectively aggregates K-order neighbor information while avoiding neighbor explosion and expediting training. The performance of the SPVec-SGCN-CPI method was assessed across three datasets and compared against four machine learning- and deep learning-based methods, as well as six state-of-the-art methods. Experimental results revealed that SPVec-SGCN-CPI outperformed all these competing methods, particularly excelling in unbalanced data scenarios. By propagating node features and topological information to the feature space, SPVec-SGCN-CPI effectively incorporates interactions between compounds and proteins, enabling the fusion of heterogeneity. Furthermore, our method scored all unlabeled data in ChEMBL, confirming the top five ranked compound-protein interactions through molecular docking and existing evidence. These findings suggest that our model can reliably uncover compound-protein interactions within unlabeled compound-protein pairs, carrying substantial implications for drug re-profiling and discovery. In summary, SPVec-SGCN demonstrates its efficacy in accurately predicting compound-protein interactions, showcasing potential to enhance target identification and streamline drug discovery processes.Scientific contributionsThe methodology presented in this work not only enables the comparatively accurate prediction of compound-protein interactions but also, for the first time, take sample imbalance which is very common in real world and computation efficiency into consideration simultaneously, accelerating the target identification and drug discovery process.

5.
Sci Total Environ ; 946: 174059, 2024 Oct 10.
Article in English | MEDLINE | ID: mdl-38906286

ABSTRACT

Submerged macrophytes have important impacts on the denitrification and anaerobic ammonia-oxidizing (anammox) processes. Leaf damage in these plants probably changes the rhizosphere environment, affecting organic acid release and denitrifying bacteria. However, there is a lack of comprehensive understanding of the specific changes. This study investigated these changes in the rhizosphere of Potamogeton crispus with four degrees of leaf excision. When 0 %, 30 %, 50 % and 70 % of leaves were excised, the concentrations of total organic acid were 31.45, 32.67, 38.26, and 35.16 mg/L, respectively. The abundances of nirS-type denitrifying bacteria were 2.10 × 1010, 1.59 × 1010, 2.54 × 1010, and 4.67 × 1010 copies/g dry sediment, respectively. The abundances of anammox bacteria were 7.58 × 109, 4.59 × 109, 3.81 × 109, and 3.90 × 109 copies/g dry sediment, respectively. The concentration of total organic acids and the abundance of two denitrification microorganisms in the rhizosphere zone were higher than those in the root zone and non-rhizosphere zone. With increasing leaf damage, the number of OTUs in the Pseudomonas genus of nirS-type denitrifying bacteria first increased and then decreased, while that of the Thauera genus was relatively stable. The overall increase in the OTU number of anammox bacteria indicated that leaf damage promotes root exudates release, thereby leading to an increase in their diversity. The co-occurrence network revealed that the two denitrification microorganisms had about 60.52 % positive connections in rhizosphere while 64.73 % negative connections in non-rhizosphere. The abundance and community composition of both denitrification microorganisms were positively correlated with the concentrations of various substances such as oxalic acid, succinic acid, total organic acids and NO2--N. These findings demonstrate that submerged plant damage has significantly impacts on the structure of denitrification microbial community in the rhizosphere, which may alter the nitrogen cycling process in the deposit sediment. SYNOPSIS: This study reveals leaf damage of macrophyte changed the rhizosphere denitrification microbial community, which is helpful to further understand the process of nitrogen cycle in water.


Subject(s)
Denitrification , Microbiota , Plant Leaves , Rhizosphere , Plant Leaves/metabolism , Plant Leaves/microbiology , Bacteria/metabolism , Bacteria/classification , Soil Microbiology
6.
ChemSusChem ; 17(14): e202400466, 2024 Jul 22.
Article in English | MEDLINE | ID: mdl-38727153

ABSTRACT

As a result of full-scale ongoing global efforts, the power conversion efficiency (PCE) of the organic-inorganic metal halide perovskite has skyrocketed. Unfortunately, the long-term operational stability for commercialization standards is still lagging owing to intrinsic defects such as ion migration-induced degradation, undercoordinated Pb2+, and shallow defects initiated by disordered crystal growth. Herein, we employed multifunctional, non-volatile tetra-methyl guanidine hydrochloride [TMGHCL] ionic liquid (IL) as an additive to elucidate defects' passivation effects on organic-inorganic metal halide perovskite. More specifically, the formation of hydrogen bonds between H+ in GA+ and I- and coordinate bonding between Cl- and undercoordinated Pb2+ could significantly passivate these defects. The hypothesis was confirmed by both experimental and DFT simulations displaying that the optimized ratio of IL integration restrains ion migration, improving grains' size, and significantly elongating the carrier lifetime. Remarkably, the modified cell achieved a peak efficiency of 22.00 % with negligible hysteresis, compared to the control device's PCE of 20.12 %. In addition, the TMGHCL-based device retains its 93.29 % efficiency after 16 days of continuous exposure to air with a relative humidity of 35±5% and temperature of 25±5 °C. This efficient approach of adding IL to perovskites absorber can produce high PCE and has strong commercialization potential.

7.
Article in English | MEDLINE | ID: mdl-38652094

ABSTRACT

The high photoelectric conversion efficiency and low cost of perovskite solar cells (PSCs) have further inspired people's determination to push this technology toward industrialization. The high-quality perovskite films and high-efficiency and stable PSCs are the crucial factors. Ionic liquids have been proven to be an effective strategy for regulating high-quality perovskite films and high-performance PSCs. However, the regulation mechanism between ionic liquids and perovskites still needs further clarification. In this study, a novel sulfonic acid-functionalized ionic liquid, 1-butyl-3-methylimidazolium trifluoromethanesulfonate (BSO3HMImOTf), was used as an effective additive to regulate high-quality perovskite films and high-performance devices. Microscopic mechanism studies revealed strong interactions between BSO3HMImOTf and Pb2+ ions as well as halogens in the perovskite. The perovskite film is effectively passivated with the controlled crystal growth, suppressed ion migration, facilitating to the greatly improved photovoltaic performance, and superior long-term stability. This article reveals the regulatory mechanism of sulfonic acid type ionic liquids through testing characterization and mechanism analysis, providing a new approach for the preparation of high-quality perovskite devices.

8.
J Hazard Mater ; 470: 134183, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38574663

ABSTRACT

Nanomaterials present a vast potential as functional materials in environmental engineering. However, there are challenges with nanocomplex for recyclability, reliable/stable, and scale-up industrial integration. Here, a versatile, low-cost, stable and recycled easily metal-polyphenolic-based material carried by wood powder (bioCar-MPNs) adsorption platform was nano-engineered by a simple, fast self-assembly strategy, in which wood powder is an excellent substrate serving as a scaffold and stabilizer to prevent the nanocomplex from aggregating and is easier to recycle. Life cycle analysis highlights a green preparation process and environmental sustainability for bioCar-MPNs. The metal-polyphenolic nanocomplex coated on the wood surface in bioCar-MPNs presents a remarkable surface adsorption property (1829.4 mg/g) at a low cost (2.4 US dollars per 1000 g bioCar-MPNs) for organic dye. Quartz crystal microbalance analysis (QCM) demonstrates an existing strong affinity between polyphenols and organic dyes. Furthermore, Independent Gradient Model (IGM) and Hirshfeld surface analysis reveal the presence of the electrostatic interactions, π-π interactions, and hydrogen bonding. Meanwhile, adsorption efficiency of bioCar-MPNs maintains over 95% in the presence of co-existing ions (Na+, 0.5 M). Importantly, the reasonable utilization of biomass for water treatment can contribute to achieving the high-value and resource utilization of biomass materials.

9.
J Ethnopharmacol ; 329: 118149, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38580188

ABSTRACT

ETHNOPHARMACOLOGICAL RELEVANCE: Calcium oxalate crystals play a key role in the development and recurrence of kidney stones (also known as urolithiasis); thus, inhibiting the formation of these crystals is a central focus of urolithiasis prevention and treatment. Previously, we reported the noteworthy in vitro inhibitory effects of Aspidopterys obcordata fructo oligosaccharide (AOFOS), an active polysaccharide of the traditional Dai medicine Aspidopterys obcordata Hemsl. (commonly known as Hei Gai Guan), on the growth of calcium oxalate crystals. AIM OF THE STUDY: To investigated the effectiveness and mechanism of AOFOS in treating kidney stones. MATERIALS AND METHODS: A kidney stones rats model was developed, followed by examining AOFOS transport dynamics and effectiveness in live rats. Additionally, a correlation between the polysaccharide and calcium oxalate crystals was studied by combining crystallization experiments with density functional theory calculations. RESULTS: The results showed that the polysaccharide was transported to the urinary system. Furthermore, their accumulation was inhibited by controlling their crystallization and modulating calcium ion and oxalate properties in the urine. Consequently, this approach helped effectively prevent kidney stone formation in the rats. CONCLUSIONS: The present study emphasized the role of the polysaccharide AOFOS in modulating crystal properties and controlling crystal growth, providing valuable insights into their potential therapeutic use in managing kidney stone formation.


Subject(s)
Calcium Oxalate , Crystallization , Kidney Calculi , Animals , Calcium Oxalate/chemistry , Calcium Oxalate/metabolism , Male , Rats , Kidney Calculi/prevention & control , Kidney Calculi/drug therapy , Rats, Sprague-Dawley , Oligosaccharides/pharmacology , Oligosaccharides/chemistry , Urolithiasis/drug therapy , Urolithiasis/prevention & control , Disease Models, Animal , Inulin/chemistry , Inulin/pharmacology
10.
ACS Appl Mater Interfaces ; 16(7): 9078-9087, 2024 Feb 21.
Article in English | MEDLINE | ID: mdl-38326938

ABSTRACT

Piezoelectric ceramics, as essential components of actuators and transducers, have captured significant attention in both industrial and scientific research. The "entropy engineering" approach has been demonstrated to achieve excellent performance in lead-based materials. In this study, the "entropy engineering" approach was employed to introduce the morphotropic phase boundary (MPB) into the bismuth ferrite (BF)-based lead-free system. By employing this strategy, a serial of novel "medium to high entropy" lead-free piezoelectric ceramics were successfully synthesized, namely (1-x)BiFeO3-x(Ba0.2Sr0.2Ca0.2Bi0.2Na0.2)TiO3 (BF-xBSCBNT, x = 0.15-0.5). Our investigation systematically examined the phase structure, domain configuration, and ferroelectric/piezoelectric properties as a function of conformational entropy. Remarkable performances with a largest strain of 0.50% at 100 kV/cm, remanent polarization ∼40.07 µC/cm2, coercive field ∼74.72 kV/cm, piezoelectric coefficient ∼80 pC/N, and d33* ∼500 pm/V were achieved in BF-0.4BSCBNT ceramics. This exceptional performance can be attributed to the presence of MPB, coexisting rhombohedral and cubic phases, along with localized nanodomains. The concept of high-entropy lead-free piezoelectric ceramics in this study provides a promising strategy for the exploration and development of the next generation of lead-free piezoelectric materials.

11.
Environ Pollut ; 346: 123623, 2024 Apr 01.
Article in English | MEDLINE | ID: mdl-38387545

ABSTRACT

Microplastics (MPs), pollutants detected at high frequency in the environment, can be served as carriers of many kinds of pollutants and have typical characteristics of environmental persistence and bioaccumulation. The potential risks of MPs ecological environment and health have been widely concerned by scholars and engineering practitioners. Previous reviews mostly focused on the pollution characteristics and ecological toxicity of MPs, but there were few reviews on MPs analysis methods, aging mechanisms and removal strategies. To address this issue, this review first summarizes the contamination characteristics of MPs in different environmental media, and then focuses on analyzing the detection methods and analyzing the aging mechanisms of MPs, which include physical aging and chemical aging. Further, the ecotoxicity of MPs to different organisms and the associated enhanced removal strategies are outlined. Finally, some unresolved research questions related to MPs are prospected. This review focuses on the ageing and ecotoxic behaviour of MPs and provides some theoretical references for the potential environmental risks of MPs and their deep control.


Subject(s)
Environmental Pollutants , Water Pollutants, Chemical , Microplastics/toxicity , Microplastics/analysis , Plastics/toxicity , Environmental Monitoring/methods , Water Pollutants, Chemical/toxicity , Water Pollutants, Chemical/analysis , Environmental Pollutants/toxicity , Environmental Pollutants/analysis
12.
Int J Biol Macromol ; 261(Pt 2): 129822, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38307437

ABSTRACT

The impact of citric acid, carboxymethyl cellulose, carboxymethyl starch, sodium trimetaphosphate, or soybean protein on the crosslinking of starch-based films was examined. These crosslinking starch films were then used to create pH-sensitive food labels using a casting method. Blueberry anthocyanins were incorporated into these smart labels as a pH-sensitive colorimetric sensor. The mechanical properties, moisture resistance, and pH responsiveness of these smart labels were then examined. Crosslinking improved the mechanical properties and pH sensitivity of the labels. These different crosslinking agents also affected the hydrophobicity of the labels to varying degrees. Soybean protein was the only additive that led to labels that could sustain their structural integrity after immersion in water for 12 h. Because it increased the hydrophobicity of the labels, which decreased their water vapor permeability, moisture content, swelling index, and water solubility by 47 %, 29 %, 52 % and 10 %, respectively. The potential of using these labels to monitor the freshness of chicken breast was then examined. Only the films containing soybean protein exhibited good pH sensitivity, high structural stability, and low pigment leakage. This combination of beneficial attributes suggests that the composite films containing starch and soybean protein may be most suitable for monitoring meat freshness.


Subject(s)
Anthocyanins , Soybean Proteins , Anthocyanins/chemistry , Meat , Permeability , Starch/chemistry , Food Packaging , Hydrogen-Ion Concentration
13.
Int. microbiol ; 27(1): 67-79, Feb. 2024. ilus, graf
Article in English | IBECS | ID: ibc-230244

ABSTRACT

Complete ammonia oxidation (comammox) bacteria can complete the whole nitrification process independently, which not only challenges the classical two-step nitrification theory but also updates long-held perspective of microbial ecological relationship in nitrification process. Although comammox bacteria have been found in many ecosystems in recent years, there is still a lack of research on the comammox process in rhizosphere of emergent macrophytes in lakeshore zone. Sediment samples were collected in this study from rhizosphere, far-rhizosphere, and non-rhizosphere of emergent macrophytes along the shore of Lake Liangzi, a shallow lake. The diversity of comammox bacteria and amoA gene abundance of comammox bacteria, ammonia-oxidizing archaea (AOA), and ammonia-oxidizing bacteria (AOB) in these samples were measured. The results showed that comammox bacteria widely existed in the rhizosphere of emergent macrophytes and fell into clade A.1, clade A.2, and clade B, and clade A was the predominant community in all sampling sites. The abundance of comammox amoA gene (6.52 × 106–2.45 × 108 copies g−1 dry sediment) was higher than that of AOB amoA gene (6.58 × 104–3.58 × 106 copies g−1 dry sediment), and four orders of magnitude higher than that of AOA amoA gene (7.24 × 102–6.89 × 103 copies g−1 dry sediment), suggesting that the rhizosphere of emergent macrophytes is more favorable for the growth of comammox bacteria than that of AOB and AOA. Our study indicated that the comammox bacteria may play important roles in ammonia-oxidizing processes in all different rhizosphere regions.(AU)


Subject(s)
Humans , Rhizosphere , Soil Microbiology , Ammonia , Lakes/microbiology , Archaea , Oxidation-Reduction , Microbiology , Microbiological Techniques , Ecosystem
14.
Angew Chem Int Ed Engl ; 63(16): e202401394, 2024 04 15.
Article in English | MEDLINE | ID: mdl-38396356

ABSTRACT

Carbohydrates play pivotal roles in an array of essential biological processes and are consequently involved in many diseases. To meet the needs of glycobiology research, chemical enzymatic and non-enzymatic methods have been developed to generate glycoconjugates with well-defined structures. Herein, harnessing the unique properties of C6-oxidized glycans, we report a straightforward and robust strategy for site- and stereoselective glycomodification of biomolecules with N-terminal tryptophan residues by a carbohydrate-promoted Pictet-Spengler reaction, which is not adapted to typical aldehyde substrates under biocompatible conditions. This method reliably delivers highly homogeneous glycoconjugates with stable linkages and thus has great potential for functional modulation of peptides and proteins in glycobiology research. Moreover, this reaction can be performed at the glycosites of glycopeptides, glycoproteins and living-cell surfaces in a site-specific manner. Control experiments indicated that the protected α-O atom of aldehyde donors and free N-H bond of the tryptamine motif are crucial for this reaction. Mechanistic investigations demonstrated that the reaction exhibited a first-order dependence on both tryptophan and glycan, and deprotonation/rearomatization of the pentahydro-ß-carbolinium ion intermediate might be the rate-determining step.


Subject(s)
Carbohydrates , Tryptophan , Tryptophan/chemistry , Proteins/chemistry , Aldehydes/chemistry , Polysaccharides , Glycoconjugates
15.
ISA Trans ; 147: 328-336, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38290863

ABSTRACT

The mechanical properties serve as crucial quality indicators for cold-rolled strips. For a long time, the mechanical properties mechanism and data-driven models can't comprehensively consider sufficient factors to achieve high-accuracy prediction due to the "data-isolated island" between production lines. In this research, we introduce a multi-process collaborative platform based on the industrial internet system. This platform is designed to enable real-time collection of diverse and heterogeneous data from both upstream and downstream processes of cold rolling. On this basis, a novel mechanical properties interval prediction model is proposed using the sparrow search algorithm to optimize fast learning network under the LUBE framework. We trained the model by using a dataset collected from a large steel plant. Based on the rolling theory and Pearson correlation coefficient, 25 features are selected as the inputs of the prediction model. The experimental results and comparison show that the proposed model is feasible and outperforms other machine learning models, such as the artificial bee colony algorithm optimized extreme learning machine and back propagation neural network model.

16.
Life Sci Space Res (Amst) ; 40: 115-125, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38245336

ABSTRACT

The circadian clock extensively regulates physiology and behavior. In space, astronauts encounter many environmental factors that are dramatically different from those on Earth; however, the effects of these factors on circadian rhythms and the mechanisms remain largely unknown. The present study aimed to investigate the changes in the mouse diurnal rhythm and gut microbiome under simulated space capsule conditions, including microgravity, noise and low atmospheric pressure (LAP). Noise and LAP were loaded in the capsule while the conditions in the animal room remained constant. The mice in the capsule showed disturbed locomotor rhythms and faster adaptation to a 6-h phase advance. RNA sequencing of hypothalamus samples containing the suprachiasmatic nucleus (SCN) revealed that microgravity simulated by hind limb unloading (HU) and exposure to noise and LAP led to decreases in the quantities of differentially expressed genes (DEGs), including circadian clock genes. Changes in the rhythmicity of genes implicated in pathways of cardiovascular deconditioning and more concentrated phases were found under HU or noise and LAP. Furthermore, 16S rRNA sequencing revealed dysbiosis in the gut microbiome, and noise and LAP may repress the temporal discrepancy in the microbiome community structure induced by microgravity. Changes in diurnal oscillations were observed in a number of gut bacteria with critical physiological consequences on metabolism and immunodefense. We also found that the superimposition of noise and LAP may repress normal changes in global gene expression and adaptation in the gut microbiome. Our data demonstrate that in addition to microgravity, exposure to noise and LAP affect the robustness of circadian rhythms and the community structure of the gut microbiome, and these factors may interfere with each other in their adaptation to respective conditions. These findings are important for furthering our understanding of the alterations in circadian rhythms in the complex environment of space.


Subject(s)
Gastrointestinal Microbiome , Weightlessness , Mice , Animals , Weightlessness/adverse effects , RNA, Ribosomal, 16S/genetics , Circadian Rhythm/genetics , Atmospheric Pressure
17.
Int J Biol Macromol ; 256(Pt 2): 128487, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38042324

ABSTRACT

CotA laccases are multicopper oxidases known for promiscuously oxidizing a broad range of substrates. However, studying substrate promiscuity is limited by the complexity of electron transfer (ET) between substrates and laccases. Here, a systematic analysis of factors affecting ET including electron donor acceptor coupling (ΗDA), driving force (ΔG) and reorganization energy (λ) was done. Catalysis rates of syringic acid (SA), syringaldehyde (SAD) and acetosyringone (AS) (kcat(SAD) > kcat(SA) > kcat(AS)) are not entirely dependent on the ability to form phenol radicals indicated by ΔG and λ calculated by Density Functional Theory (SA < SAD ≈ AS). In determined CotA/SA and CotA/SAD structures, SA and SAD bound at 3.9 and 3.7 Å away from T1 Cu coordinating His419 ensuring a similar ΗDA. Abilities of substrate to form phenol radicals could mainly account for difference between kcat(SAD) and kcat(SA). Furthermore, substrate pocket is solvent exposed at the para site of substrate's phenol hydroxyl, which would destabilize binding of AS in the same orientation and position resulting in low kcat. Our results indicated shallow partially covered binding site with propensity of amino acids distribution might help CotA discriminate lignin-phenol derivatives. These findings give new insights for developing specific catalysts for industrial application.


Subject(s)
Laccase , Lignin , Laccase/chemistry , Lignin/metabolism , Phenol , Electron Transport , Phenols
18.
Sci Total Environ ; 912: 168822, 2024 Feb 20.
Article in English | MEDLINE | ID: mdl-38043821

ABSTRACT

The preparation of biochar from digestate is one of the effective ways to achieve the safe disposal and resource utilization of digestate. Nevertheless, up to now, a comprehensive review encompassing the factors influencing anaerobic digestate-derived biochar production and its applications is scarce in the literature. Therefore, to fill this gap, the present work first outlined the research hotspots of digestate in the last decade using bibliometric statistical analysis with the help of VOSviewer. Then, the characteristics of the different sources of digestate were summarized. Furthermore, the influencing factors of biochar preparation from digestate and the modification methods of digestate-derived biochar and associated mechanisms were analyzed. Notably, a comprehensive synthesis of anaerobic digestate-derived biochar applications is provided, encompassing enhanced anaerobic digestion, heavy metal remediation, aerobic composting, antibiotic/antibiotic resistance gene removal, and phosphorus recovery from digestate liquor. The economic and environmental impacts of digestate-derived biochar were also analyzed. Finally, the development prospect and challenges of using biochar from digestate to combat environmental pollution are foreseen. The aim is to not only address digestate management challenges at the source but also offer a novel path for the resourceful utilization of digestate.


Subject(s)
Charcoal , Environmental Restoration and Remediation , Environment , Environmental Pollution , Anaerobiosis
19.
Int Microbiol ; 27(1): 67-79, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38062210

ABSTRACT

Complete ammonia oxidation (comammox) bacteria can complete the whole nitrification process independently, which not only challenges the classical two-step nitrification theory but also updates long-held perspective of microbial ecological relationship in nitrification process. Although comammox bacteria have been found in many ecosystems in recent years, there is still a lack of research on the comammox process in rhizosphere of emergent macrophytes in lakeshore zone. Sediment samples were collected in this study from rhizosphere, far-rhizosphere, and non-rhizosphere of emergent macrophytes along the shore of Lake Liangzi, a shallow lake. The diversity of comammox bacteria and amoA gene abundance of comammox bacteria, ammonia-oxidizing archaea (AOA), and ammonia-oxidizing bacteria (AOB) in these samples were measured. The results showed that comammox bacteria widely existed in the rhizosphere of emergent macrophytes and fell into clade A.1, clade A.2, and clade B, and clade A was the predominant community in all sampling sites. The abundance of comammox amoA gene (6.52 × 106-2.45 × 108 copies g-1 dry sediment) was higher than that of AOB amoA gene (6.58 × 104-3.58 × 106 copies g-1 dry sediment), and four orders of magnitude higher than that of AOA amoA gene (7.24 × 102-6.89 × 103 copies g-1 dry sediment), suggesting that the rhizosphere of emergent macrophytes is more favorable for the growth of comammox bacteria than that of AOB and AOA. Our study indicated that the comammox bacteria may play important roles in ammonia-oxidizing processes in all different rhizosphere regions.


Subject(s)
Ammonia , Archaea , Archaea/genetics , Rhizosphere , Ecosystem , Lakes/microbiology , Oxidation-Reduction , Phylogeny , Bacteria , Soil Microbiology
20.
Nanoscale ; 16(3): 1247-1253, 2024 Jan 18.
Article in English | MEDLINE | ID: mdl-38116609

ABSTRACT

Graphene's unique gapless band structure and remarkably large third-order optical susceptibility have drawn significant attention to its nonlinear optical response, particularly in the context of coherent anti-Stokes Raman scattering (CARS). Under the combined influence of phononic and electronic resonances, the CARS response of graphene has been observed to exhibit a distinctive feature of time-resolved dip-to-peak evolution. Here, we report a greatly enhanced double resonance Raman mode beyond the G mode of multi-layer graphene with broadband CARS measurements. The significant difference in the intensity ratio between CARS and SR for this mode may be attributed to the preferential activation of low-frequency phonons in the impulsive stimulated Raman scattering process (ISRS) and a lower dephasing rate. Our results build on a foundation towards a deeper exploration of the coherent Raman response of two-dimensional materials.

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