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1.
Small ; : e2402496, 2024 Oct 14.
Artículo en Inglés | MEDLINE | ID: mdl-39402776

RESUMEN

In pharmaceuticals, the structural and functional alterations induced by biotransformation are well-documented. Many pharmaceuticals exist in various crystal forms, which govern their transformation and significantly impact their activity. However, in the field of inorganic nanomedicine, there is a paucity of research focusing on the influence of crystal form-dependent "metabolism" (transformation) on their activity and biomechanism. This study delves into the distinct performances of two crystal forms of manganese sulfide (MnS), namely α-MnS and γ-MnS, in bacteria-infected diabetic wound healing. In the initial stage of a wound, where the environment is neutral to slightly alkaline, MnS partially converts to MnxOy (comprising Mn2O3 and Mn3O4) and concurrently produces hydrogen sulfide (H2S); the conversion efficiency of γ-MnS significantly surpasses that of α-MnS. Additionally, γ-MnS is more soluble than α-MnS, which allows it to generate more Mn2+. These components collectively contribute to the superior bacteriostatic properties of MnS. In wound related cells, MnS stimulates the production of collagen I and vascular endothelial growth factor (VEGF), promote the M1 macrophages polarizing to the M2 phenotype, for extracellular matrix (ECM) remodeling. Notably, different transformation products have distinct functions. Consequently, the activity of MnS is dependent on its original crystal form related solubility and transformation efficiency.

2.
Cell Commun Signal ; 22(1): 519, 2024 Oct 25.
Artículo en Inglés | MEDLINE | ID: mdl-39456056

RESUMEN

BACKGROUND: Podocyte injury causes proteinuria and accelerates glomerular sclerosis during diabetic kidney disease (DKD). Disruptor of telomeric silencing 1-like (DOT1L), an evolutionarily conserved histone methyltransferase, has been reported in preventing kidney fibrosis in chronic kidney disease models. However, whether DOT1L exerts beneficial effects in diabetes induced podocyte injury and the underlying molecular mechanisms need further exploration. METHODS: The expression of DOT1L was confirmed by Western blotting in MPC-5 cells and cortex of kidney from db/db mice, as well as immunofluorescence staining in human renal biopsy samples. The effect of DOT1L on podocyte injury was obtained using MPC-5 cells and db/db mice. The potential target genes regulated by DOT1L was measured by RNA-sequencing. Then, a series of molecular biological experiments was performed to investigate the regulation of PLCL1 by DOT1L in MCP-5 cells and db/db mice. Lipid accumulation was assessed by UPLC-MS/MS analysis and Oil Red O staining. RESULTS: DOT1L expression was significantly declined in high glucose (HG)-treated MPC-5 cells, podocyte regions of kidney tissues from db/db mice and human renal biopsy samples. Subsequent investigations revealed that upregulation of DOT1L ameliorated HG-induced cell apoptosis in MPC-5 cells as well as primary podocytes. Furthermore, podocyte-specific DOT1L overexpression inhibited diabetic podocyte injury in db/db mice. Mechanistically, we revealed that DOT1L upregulated phospholipase C-like 1 (PLCL1) expression by mediating H3K79me2 at its promoter and PLCL1 silencing suppressed the protective role of DOT1L on podocyte injury. Moreover, DOT1L improved diabetes induced abnormal fatty acid metabolism in podocytes and PLCL1 knockdown reversed its protective effects. CONCLUSIONS: Taken together, our results indicate that DOT1L protects podocyte injury via PLCL1-mediated fatty acid metabolism and provides new insights into the therapeutic target of DKD.


Asunto(s)
Nefropatías Diabéticas , N-Metiltransferasa de Histona-Lisina , Podocitos , Podocitos/patología , Podocitos/metabolismo , Nefropatías Diabéticas/patología , Nefropatías Diabéticas/metabolismo , Nefropatías Diabéticas/genética , Animales , N-Metiltransferasa de Histona-Lisina/metabolismo , N-Metiltransferasa de Histona-Lisina/genética , Humanos , Ratones , Masculino , Apoptosis/genética , Ratones Endogámicos C57BL , Línea Celular
3.
Artículo en Inglés | MEDLINE | ID: mdl-39437330

RESUMEN

Passivation technology is crucial for reducing interface defects and impacting the performance of crystalline silicon (c-Si) solar cells. Concurrently, maintaining a thin passivation layer is essential for ensuring efficient carrier transport. With an ultrathin passivated contact structure, both Silicon Heterojunction (SHJ) cells and Tunnel Oxide Passivated Contact (TOPCon) solar cells achieve an efficiency surpassing 26%. To reduce production costs and simplify solar cell manufacturing processes, the rapid development of organic material passivation technology has emerged. However, its widespread industrial production is hindered by environmental safety concerns, such as strong acid corrosion and biological and ecological safety issues. Here, we discovered a low-cost self-assembled monolayer (SAM) hole-selective transport material known as 2PACz ([2-(9H-carbazol-9-yl) ethyl] phosphonic acid) with phosphate groups to form c-Si solar cells for the first time. The ultrathin film of 2PACz with phosphate groups can establish strong and stable P-O-Si bonds on the silicon surface. Meanwhile, like 2PACz, a uniform ultrathin film with a carbazole function group can offer electron-localizing and thus hole-selective properties, which provides ideas for studying dopant-free silicon solar cells. As a result of such interfacial passivation engineering, it plays an important role in repairing porous structures, such as pyramid-textured silicon surfaces, and cutting losses during the commercialization of c-Si solar cells. Crucially, this advancement offers insights for the development of new high-efficiency ultrathin film passivation methods in the postsilicon era.

4.
Eur J Pharm Sci ; 203: 106899, 2024 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-39265705

RESUMEN

BACKGROUND: Species differences in CYP2D6 drug metabolism complicate the extrapolation of in vivo pharmacokinetic data to humans and impact the prediction of drug responses. This study aimed to develop an in vivo model to predict human responses to CYP2D6 metabolized compounds and to evaluate medication risks and disease development. METHODS: We used embryonic stem cell (ES) targeting and CRISPR-Cas9 technology to create a humanized CYP2D6 mouse model by inserting the human wild-type CYP2D6 gene and knocking out the mouse Cyp2d locus. Metoprolol was used as the substrate probe to examine the pharmacokinetic properties of exogenous substances, tissue distribution, and in situ metabolism of CYP2D6. Untargeted and quantitative metabolomics analyses compared endogenous substance metabolism between different species of CYP2D6 enzymes. RESULTS: No significant differences in CYP2D6 homologous protein distribution and expression of primary metabolic organs were found between humanized CYP2D6 mice and wild-type (WT) mice. The activity and metabolic capacity of CYP2D6 in humanized mice were substantially lower than homologous Cyp2d22 of WT mice in metabolizing metoprolol. The levels of several glycerolipids and glycerophospholipid-related metabolites were down-regulated in humanized CYP2D6 mice. Triglyceride TG (14:0_22:6_22:6) was significantly downregulated in male and female humanized mice, suggesting a strong association with reduced CYP2D6 activity. CONCLUSIONS: This study established a robust animal model to investigate human CYP2D6-mediated metabolic profiles of exogenous and endogenous compounds, predict medication risks, and explore the potential roles of CYP2D6 in organ-specific toxicity and disease development.


Asunto(s)
Citocromo P-450 CYP2D6 , Metoprolol , Citocromo P-450 CYP2D6/metabolismo , Citocromo P-450 CYP2D6/genética , Animales , Humanos , Masculino , Metoprolol/metabolismo , Metoprolol/farmacocinética , Femenino , Ratones , Metaboloma , Ratones Noqueados , Distribución Tisular
5.
Small ; : e2405358, 2024 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-39291888

RESUMEN

The replacement of oxygen evolution reactions with organic molecule oxidation reactions to enable energy-efficient hydrogen production has been a subject of interest. However, further reducing reaction energy consumption and releasing hydrogen from organic molecules continue to pose significant challenges. Herein, a strategy is proposed to produce hydrogen and formic acid from formaldehyde using Ag/Co3O4 interface catalysts at the anode. The key to improving the performance of Ag-based catalysts for formaldehyde oxidation lies in the strong SMSI achieved through the well-designed "spontaneous redox reaction" between Ag and Co3O4 precursors. Nano-sized Ag particles are uniformly dispersed on Co3O4 nanosheets, and electron-deficient Agδ+ are formed by the SMSI between Ag and Co3O4. Ag/Co3O4 demonstrates exceptional formaldehyde oxidation activity at low potentials of 0.32 V versus RHE and 0.65 V versus RHE, achieving current densities of 10 and 100 mA cm-2, respectively. The electrolyzer "Ag/Co3O4||20% Pt/C" achieves over 195% hydrogen efficiency and over 98% formic acid selectivity, maintaining stable operation for 60 hours. This work not only presents a novel approach to precisely modulate Ag particle size and interface electronic structure via SMSI, but also provides a promising approach to efficient and energy-saving hydrogen production and the transformation of harmful formaldehyde.

6.
Environ Sci Technol ; 58(28): 12379-12389, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-38961056

RESUMEN

Accumulating evidence linked extreme temperature events (ETEs) and fine particulate matter (PM2.5) to cardiometabolic multimorbidity (CMM); however, it remained unknown if and how ETEs and PM2.5 interact to trigger CMM occurrence. Merging four Chinese national cohorts with 64,140 free-CMM adults, we provided strong evidence among ETEs, PM2.5 exposure, and CMM occurrence. Performing Cox hazards regression models along with additive interaction analyses, we found that the hazards ratio (HRs) of CMM occurrence associated with heatwave and cold spell were 1.006-1.019 and 1.063-1.091, respectively. Each 10 µg/m3 increment of PM2.5 concentration was associated with 17.9% (95% confidence interval: 13.9-22.0%) increased risk of CMM. Similar adverse effects were also found among PM2.5 constituents of nitrate, organic matter, sulfate, ammonium, and black carbon. We observed a synergetic interaction of heatwave and PM2.5 pollution on CMM occurrence with relative excess risk due to the interaction of 0.999 (0.663-1.334). Our study provides novel evidence that both ETEs and PM2.5 exposure were positively associated with CMM occurrence, and the heatwave interacts synergistically with PM2.5 to trigger CMM.


Asunto(s)
Material Particulado , Humanos , Estudios de Cohortes , Multimorbilidad , Contaminantes Atmosféricos , Masculino , Femenino , China/epidemiología , Persona de Mediana Edad , Exposición a Riesgos Ambientales
7.
Adv Sci (Weinh) ; 11(31): e2400174, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38889298

RESUMEN

Perovskite oxides and organic-inorganic halide perovskite materials, with numerous fascinating features, have been subjected to extensive studies. Most of the properties of perovskite materials are dependence on their ferroelectricity that denoted by remanent polarization (Pr). Thus, the increase of Pr in perovskite films is mainly an effort in material physics. At present, commonplace improvement schemes, i.e., controlling material crystallinity, and post-annealing by using a high-temperature process, are normally used. However, a simpler and temporal strategy for Pr improvement is always unavailable to perovskite material researchers. In this study, an organic coating layer, low-temperature, and vacuum-free strategy is proposed to improve the Pr, directly increasing the Pr from 36 to 56 µC cm-2. Further study finds that the increased Pr originates from the suppression of the oxygen defects and Ti defects. This organic coating layer strategy for passivating the defects may open a new way for the preparation of higher-performance and cost-effective perovskite products, further improving its prospective for application in the electron devices field.

8.
Adv Sci (Weinh) ; 11(21): e2401070, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38526150

RESUMEN

Herein, a robust microporous aluminum tetracarboxylate framework, MIL-120(Al)-AP, (MIL, AP: Institute Lavoisier and Ambient Pressure synthesis, respectively) is reported, which exhibits high CO2 uptake (1.9 mmol g-1 at 0.1 bar, 298 K). In situ Synchrotron X-ray diffraction measurements together with Monte Carlo simulations reveal that this structure offers a favorable CO2 capture configuration with the pores being decorated with a high density of µ2-OH groups and accessible aromatic rings. Meanwhile, based on calculations and experimental evidence, moderate host-guest interactions Qst (CO2) value of MIL-120(Al)-AP (-40 kJ mol-1) is deduced, suggesting a relatively low energy penalty for full regeneration. Moreover, an environmentally friendly ambient pressure green route, relying on inexpensive raw materials, is developed to prepare MIL-120(Al)-AP at the kilogram scale with a high yield while the Metal- Organic Framework (MOF) is further shaped with inorganic binders as millimeter-sized mechanically stable beads. First evidences of its efficient CO2/N2 separation ability are validated by breakthrough experiments while operando IR experiments indicate a kinetically favorable CO2 adsorption over water. Finally, a techno-economic analysis gives an estimated production cost of ≈ 13 $ kg-1, significantly lower than for other benchmark MOFs. These advancements make MIL-120(Al)-AP an excellent candidate as an adsorbent for industrial-scale CO2 capture processes.

9.
Adv Sci (Weinh) ; 11(12): e2306993, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38233212

RESUMEN

Passivating contactsin heterojunction (HJ) solar cells have shown great potential in reducing recombination losses, and thereby achieving high power conversion efficiencies in photovoltaic devices. In this direction, carbon nanomaterials have emerged as a promising option for carbon/silicon (C/Si) HJsolar cells due to their tunable band structure, wide spectral absorption, high carrier mobility, and properties such as multiple exciton generation. However, the current limitations in efficiency and active area have hindered the industrialization of these devices. In this review, they examine the progress made in overcoming these constraints and discuss the prospect of achieving high power conversion efficiency (PCE) C/Si HJ devices. A C/Si HJ solar cell is also designed by introducing an innovative interface passivation strategy to further boost the PCE and accelerate the large area preparationof C/Si devices. The physical principle, device design scheme, and performanceoptimization approaches of this passivated C/Si HJ cells are discussed. Additionally, they outline potential future pathways and directions for C/Si HJ devices, including a reduction in their cost to manufacture and their incorporation intotandem solar cells. As such, this review aims to facilitate a deeperunderstanding of C/Si HJ solar cells and provide guidance for their further development.

10.
Immunopharmacol Immunotoxicol ; 46(2): 172-182, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38174705

RESUMEN

OBJECTIVE: The activation of the NLRP3 inflammasome has been implicated in male infertility. Our study aimed to investigate the therapeutic role of Thiolutin (THL), an inhibitor of the NLRP3 inflammasome, on oligoasthenospermia (OA) and to elucidate its mechanisms. MATERIALS AND METHODS: Semen from 50 OA and 20 healthy males were analyzed to assess the sperm quality and levels of inflammatory markers. Their correlation was determined using Pearson's correlation coefficient. The BALB/c mice were intraperitoneal injected by cyclophosphamide at 60 mg/kg/day for five days to induce OA, followed by a two-week treatment with THL or L-carnitine. Reproductive organ size and H&E staining were determined to observe the organ and seminiferous tubule morphology. ELISA and western blotting were utilized to measure sex hormone levels, inflammatory markers, and NLRP3 inflammasome levels. Furthermore, male and female mice were co-housed to observe pregnancy success rates. RESULTS: OA patients exhibited a decrease in sperm density and motility compared to healthy individuals, along with elevated levels of IL-1ß, IL-18 and NLRP3 inflammasome. In vivo, THL ameliorated OA-induced atrophy of reproductive organs, hormonal imbalance, and improved sperm density, motility, spermatogenesis and pregnancy success rates with negligible adverse effects on weight or liver-kidney function. THL also demonstrated to be able to inhibit the activation of NLRP3 inflammasome and associated proteins in OA mice. DISCUSSION: THL can improve sperm quality and hormonal balance in OA mice through the inhibition of NLRP3 inflammasome activation. Thus, THL holds promising potential as a therapeutic agent for OA.


Asunto(s)
Inflamasomas , Proteína con Dominio Pirina 3 de la Familia NLR , Masculino , Humanos , Femenino , Ratones , Animales , Inflamasomas/metabolismo , Proteína con Dominio Pirina 3 de la Familia NLR/metabolismo , Semen/metabolismo , Ciclofosfamida/efectos adversos , Fertilidad , Espermatozoides/metabolismo , Pirrolidinonas
11.
Adv Mater ; 36(2): e2305957, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37838943

RESUMEN

Transition-metal sulfides have been regarded as perspective anode candidates for high-energy Na-ion batteries. Their application, however, is precluded severely by either low charge storage or huge volumetric change along with sluggish reaction kinetics. Herein, an effective synergetic Sn incorporation-Zn substitution strategy is proposed based on copper-based sulfides. First, Na-ion storage capability of copper sulfide is significantly improved via incorporating an alloy-based Sn element. However, this process is accompanied by sacrifice of structural stability due to the high Na-ion uptake. Subsequently, to maintain the high Na-ion storage capacity, and concurrently improve cycling and rate capabilities, a Zn substitution strategy (taking partial Sn sites) is carried out, which could significantly promote Na-ion diffusion/reaction kinetics and relieve mechanical strain-stress within the crystal framework. The synergetic Sn incorporation and Zn substitution endow copper-based sulfides with high specific capacity (≈560 mAh g-1 at 0.5 A g-1 ), ultrastable cyclability (80 k cycles with ≈100% capacity retention), superior rate capability up to 200 A g-1 , and ultrafast charging feature (≈4 s per charging with ≈190 mAh g-1 input). This work provides in-depth insights for developing superior anode materials via synergetic multi-cation incorporation/substitution, aiming at solving their intrinsic issues of either low specific capacity or poor cyclability.

12.
Ecotoxicol Environ Saf ; 269: 115803, 2024 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-38091674

RESUMEN

Particulate matter pollution could increase the risk of kidney disease, while evidence for ozone exposure is less well-established. Here, we aimed to evaluate the effect of ozone pollution on renal function and explore mechanisms. We first conducted a cross-sectional study based on Wuhan Chronic Disease Cohort Study baseline information. We recruited 2699 eligible participants, estimated their residential ozone concentrations, collected fasting peripheral blood samples for biochemical analysis and calculated the estimated glomerular filtration rate (eGFR). The linear regression model was applied to evaluate the long-term association between ozone pollution and eGFR. Then, we recruited another 70 volunteers as a panel with 8 rounds follow-up visits. We calculated the eGFR and measured fasting blood glucose and lipid levels. The linear mixed-effect model along with mediation analysis were performed to confirm the short-term association and explore potential mechanisms, respectively. For the long-term association, a 10.95 µg/m3 increment of 3-year ozone exposure was associated with 2.96 mL/min/1.73 m2 decrease in eGFR (95%CI: -4.85, -1.06). Furthermore, the drinkers exhibited a pronounced declination of eGFR (-7.46 mL/min/1.73 m2, 95%CI: -11.84, -3.08) compared to non-drinkers in relation to ozone exposure. Additionally, a 19.02 µg/m3 increase in 3-day ozone concentrations was related to 2.51 mL/min/1.73 m2 decrease in eGFR (95%CI: -3.78, -1.26). Hyperglycemia and insulin resistance mediated 12.2% and 16.5% of the aforementioned association, respectively. Our findings indicated that higher ozone pollution could affect renal function, and the hyperglycemia and insulin resistance linked to ozone might be the underlying mechanisms.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Hiperglucemia , Resistencia a la Insulina , Ozono , Humanos , Ozono/toxicidad , Ozono/análisis , Contaminantes Atmosféricos/toxicidad , Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Estudios de Cohortes , Estudios Transversales , Exposición a Riesgos Ambientales/efectos adversos , Exposición a Riesgos Ambientales/análisis , Material Particulado/análisis , Hiperglucemia/inducido químicamente , Homeostasis , Glucosa , Riñón/química
13.
Sci Total Environ ; 912: 168910, 2024 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-38013101

RESUMEN

To investigate the impacts of spatial expansion by Phragmites australis on spatiotemporal variations of sulfur (S) fractions in marsh soils of the Min River estuary (Southeast China), the contents of total sulfur (TS) and inorganic sulfur (IS) fractions (Water-Soluble-S, W-S-S; Adsorbed-S, A-S; HCl-Soluble-S, H-S-S; and HCl-Volatile-S, H-V-S) were determined in soils of Cyperus malaccensis marsh (before expansion, BE stage), P. australis-C. malaccensis marsh (during expansion, DE stage) and P. australis marsh (after expansion, AE stage) by space-for-time substitution method. Results showed that the expansion of P. australis greatly altered the spatiotemporal variations of TS and IS fractions in marsh soils. The TS contents in soils at AE stage were significantly lower than those at DE and BE stages throughout a year (p < 0.01). Higher levels of W-S-S, A-S, H-S-S and total inorganic sulfur (TIS) generally occurred in soils at DE and AE stages, whereas higher values of H-V-S were observed in soils at BE stage. Although P. australis expansion did not alter the temporal variations of TS stock in soils greatly, the values during autumn and winter were generally higher than those in spring and summer (p < 0.05). The highest TIS stocks in soils of different expansion stages were observed in spring, while the lowest values occurred in summer. The expansion of P. australis significantly increased the IS supply capacity of soils and, compared with the BE stage, stocks of W-S-S, A-S, H-S-S and TIS in soils of all sampling seasons at DE and AE stages increased by 51.40 %, 50.76 %, 63.35 %, 50.52 % and 20.00 %, 31.46 %, 42.93 %, 27.56 %, respectively. It was worth noting that stocks of H-V-S in soils at DE and AE stages showed a decreasing trend compared to the BE stage, implying that the expansion of P. australis might reduce the production of sulfides. This paper found that, compared with C. malaccensis, the increased available IS stocks in soils might be an effective strategy for P. australis to maintain its expansion advantage and the decreased volatile-S in soils might be more favorable for boosting its competitiveness. Our study provided valuable information for understanding the interspecific competition mechanism between P. australis and C. malaccensis. Next step, in order to protect the diversity of marsh vegetations in the Min River estuary, effective measures should be taken to suppress the rapid expansion of P. australis.

14.
J Chem Phys ; 159(24)2023 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-38153154

RESUMEN

Natural gas hydrates, mainly existing in permafrost and on the seabed, are expected to be a new energy source with great potential. The exploitation technology of natural gas hydrates is one of the main focuses of hydrate-related studies. In this study, a large-size liquid aqueous solution wrapping a methane hydrate system was established and molecular dynamics simulations were used to investigate the phase equilibrium conditions of methane hydrate at different methane concentrations and interfacial geometries. It is found that the methane concentration of a solution significantly affects the phase equilibrium of methane hydrates. Different methane concentrations at the same temperature and pressure can lead to hydrate formation or decomposition. At the same temperature and pressure, in a system reaching equilibrium, the size of spherical hydrate clusters is coupled to the solution concentration, which is proportional to the Laplace pressure at the solid-liquid interface. Lower solution concentrations reduce the phase equilibrium temperature of methane hydrates at the same pressure; as the concentration increases, the phase equilibrium temperature gradually approaches the actual phase equilibrium temperature. In addition, the interfacial geometry of hydrates affects the thermodynamic stability of hydrates. The spherical hydrate particles have the highest stability for the same volume. Through this study, we provide a stronger foundation to understand the principles driving hydrate formation/dissociation relevant to the exploitation of methane hydrates.

15.
J Am Chem Soc ; 145(46): 25103-25108, 2023 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-37938934

RESUMEN

Although interlocked three-dimensional molecules display unique properties associated with their spatial structures, their synthesis and study of their host-guest properties remain challenging. We report the formation of a novel [2]catenane, [Et4N]@[(Tp*WS3Cu3Cl)2(cis-bpype)3]2(OTf)5 ([Et4N][1](OTf)5), by self-assembly of the cluster node [Tp*WS3Cu3Cl]+ and the organic linker (Z)-1,2-diphenyl-1,2-bis(4-(pyridin-4-yl)phenyl)ethene (cis-bpype). Single-crystal X-ray and NMR analyses established that [1]4+ is formed by the interpenetration of two cluster-organic cages. Unique cation-in-cation host-guest complexes were observed with this catenane. The crystalline, empty catenane was formed by taking advantage of the electrostatic repulsion-induced weak binding of the host. Encapsulation experiments also reveal that the empty catenane can adaptively encapsulate cations such as [Et4N]+ and [Pr4N]+ in the cross cavity but is unable to encapsulate [Bu4N]+ and [Me4N]+, although the size of the latter is compatible with that of the cavity. Theoretical calculations and volume analysis allow to unravel the ingenious role of catenane structures and the interplay between electrostatic repulsion and attractive noncovalent interactions for size-specific recognition behavior in host-guest systems involving species with similar electric charges.

16.
J Phys Chem B ; 127(48): 10447-10457, 2023 Dec 07.
Artículo en Inglés | MEDLINE | ID: mdl-37991934

RESUMEN

Electric fields have been proven to be capable of significantly affecting the equilibrium state of hydrates. In this study, the thermodynamic properties and structural changes of methane hydrate (MH) in various anion solutions in an electric field at 0.7 V/nm were investigated by molecular dynamics simulations. The presence of anions significantly enhances the instability of methane hydrates under electric fields, leading to a staged dissociation process. First, the anions coexist with MH to form a temporary metastable structure under the action of an electric field. Then, the migration of anions causes the dissociation of nearby hydrates and the formation of flow channels in the hydrate layer, which leads to the complete dissociation of MH after a period. The promotive effects of F-, Br-, I-, and Cl- ions were close, while SO42- was relatively weak. The anions are still in hydration shells in the MH phase, but the structure of the hydration shells differs slightly from that in solution (the coordination numbers of I- and SO42- ions increased). The migration resistances of multiple anions to cross the surface of the hydrate layer are similar. However, inside the hydrate phase, the anions with a larger radius have a higher migration resistance. It is difficult for SO42- ions to migrate inside the hydrate phase, and they tend to form a metastable structure on the hydrate surface. Combining our previous studies, SrCl2 solution has the best hydrate promotion under an electric field environment.

17.
Microsyst Nanoeng ; 9: 116, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37744264

RESUMEN

In this paper, we review the integration of microfluidic chips and computer vision, which has great potential to advance research in the life sciences and biology, particularly in the analysis of cell imaging data. Microfluidic chips enable the generation of large amounts of visual data at the single-cell level, while computer vision techniques can rapidly process and analyze these data to extract valuable information about cellular health and function. One of the key advantages of this integrative approach is that it allows for noninvasive and low-damage cellular characterization, which is important for studying delicate or fragile microbial cells. The use of microfluidic chips provides a highly controlled environment for cell growth and manipulation, minimizes experimental variability and improves the accuracy of data analysis. Computer vision can be used to recognize and analyze target species within heterogeneous microbial populations, which is important for understanding the physiological status of cells in complex biological systems. As hardware and artificial intelligence algorithms continue to improve, computer vision is expected to become an increasingly powerful tool for in situ cell analysis. The use of microelectromechanical devices in combination with microfluidic chips and computer vision could enable the development of label-free, automatic, low-cost, and fast cellular information recognition and the high-throughput analysis of cellular responses to different compounds, for broad applications in fields such as drug discovery, diagnostics, and personalized medicine.

18.
Adv Sci (Weinh) ; 10(26): e2302778, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37442769

RESUMEN

Various catalysts are developed to improve the performance of metal oxide semiconductor gas sensors, but achieving high selectivity and response intensity in chemiresistive gas sensors (CGSs) remains a significant challenge. In this study, an in situ-annealing approach to synthesize Cu catalytic sites on ultrathin WO2.72 nanowires for detecting toluene at ultralow concentrations (Ra /Rg = 1.9 at 10 ppb) with high selectivity is developed. Experimental and molecular dynamic studies reveal that the Cu single atoms (SAs) act as active sites, promoting the oxidation of toluene and increasing the affinity of Cu single-atom catalysts (SACs)-containing sensing materials for toluene while weakening the association with carbon dioxide or water vapor. Density functional theory studies show that the selective binding of toluene to Cu SAs is due to the favorable binding sites provided by Cu SAs for toluene molecules over other gaseous species, which aids the adsorption of toluene on WO2.72 nanowires. This study demonstrates the successful atomic-level interface regulation engineering of WO2.72 nanowire-supported Cu SAs, providing a potential strategy for the development of highly active and durable CGSs.

19.
J Colloid Interface Sci ; 646: 159-166, 2023 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-37187049

RESUMEN

Developing piezocatalysts with excellent piezocatalytic hydrogen evolution reaction (HER) performance is highly desired but also challenging. Here, facet engineering and cocatalyst engineering are employed to synergistically improve the piezocatalytic HER efficiency of BiVO4 (BVO). Monoclinic BVO catalysts with distinct exposed facets are synthesized by adjusting pH of hydrothermal reaction. The BVO with highly exposed {110} facet exhibits a superior piezocatalytic HER performance (617.9 µmol g-1h-1) compared with that with {010} facet, owing to the strong piezoelectric property, high charge transfer efficiency, and excellent hydrogen adsorption/desorption capacity. The HER efficiency is enhanced by 44.7% by selectively depositing cocatalyst of Ag nanoparticles specifically on the reductive {010} facet of BVO, where the Ag-BVO interface provides the directional electron transport for high-efficiency charge separation. Under the collaboration between cocatalyst of CoOx on {110} facet and the hole sacrificial agent of methanol, the piezocatalytic HER efficiency is evidently enhanced by 2 times because CoOx and methanol can impede the water oxidation and improve the charge separation. This easy and simple strategy provides an alternative perspective on designing high-performance piezocatalysts.

20.
Adv Mater ; 35(32): e2211806, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37226815

RESUMEN

Polycrystalline perovskite films fabricated on flexible and textured substrates often are highly defective, leading to poor performance of perovskite devices. Finding substrate-tolerant perovskite fabrication strategies is therefore paramount. Herein, this study shows that adding a small amount of Cadmium Acetate (CdAc2 ) in the PbI2 precursor solution results in nano-hole array films and improves the diffusion of organic salts in PbI2 and promotes favorable crystal orientation and suppresses non-radiative recombination. Polycrystalline perovskite films on the flexible substrate with ultra-long carrier lifetimes exceeding 6 µs are achieved. Eventually, a power conversion efficiency (PCE) of 22.78% is obtained for single-junction flexible perovskite solar cells (FPSCs). Furthermore, it is found that the strategy is also applicable for textured tandem solar cells. A champion PCE of 29.25% (0.5003 cm2 ) is demonstrated for perovskite/silicon tandem solar cells (TSCs) with CdAc2 . Moreover, the un-encapsulated TSCs maintains 109.78% of its initial efficiency after 300 h operational at 45 °C in a  nitrogen atmosphere. This study provides a facile strategy for achieving high-efficiency perovskite-based solar cells.

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