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1.
Opt Lett ; 49(7): 1824-1827, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38560874

RESUMO

Lanthanide-doped upconversion (UC) materials have been extensively investigated for their unique capability to convert low-energy excitation into high-energy emission. Contrary to previous reports suggesting that efficient UC luminescence (UCL) is exclusively observed in materials with a wide bandgap, we have discovered in this study that Y2Mo4O15:Yb3+/Tm3+ microcrystals, a narrowband material, exhibit highly efficient UC emission. Remarkably, these microcrystals do not display any four- or five-photon UC emission bands. This particular optical phenomenon is independent of the variation in doping ion concentration, temperature, phonon energy, and excitation power density. Combining theoretical calculations and experimental results, we attribute the vanishing emission bands to the strong interaction between the bandgap of the Y2Mo4O15 host matrix (3.37 eV) and the high-energy levels (1I6 and 1D2) of Tm3+ ions. This interaction can effectively catalyze the UC emission process of Tm3+ ions, which leads to Y2Mo4O15:Yb3+/Tm3+ microcrystals possessing very strong UCL intensity. The brightness of these microcrystals outshines commercial UC NaYF4:Yb3+,Er3+ green phosphors by a factor of 10 and is 1.4 times greater than that of UC NaYF4:Yb3+,Tm3+ blue phosphors. Ultimately, Y2Mo4O15:Yb3+/Tm3+ microcrystals, with their distinctive optical characteristics, are being tailored for sophisticated anti-counterfeiting and information encryption applications.

2.
Opt Lett ; 49(11): 2978-2981, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38824307

RESUMO

Upconversion (UC) materials are renowned for their ability to convert low-energy photons into high-energy ones. The manipulation of parameters allows for the observation of multicolored UC luminescence (UCL) within a single material system. While modulation of multicolored UCL commonly relies on excitation at approximately 980 nm, investigation into multicolored UC materials activated by a 1532 nm excitation source remains comparatively scarce. In this work, we introduce NaLnF4:Er3+ as a novel class of smart luminescent materials. When the power density of a 1532 nm laser increases from 0.5 to 20.0 W/cm2, the emission peak positions remain unchanged, but the red-to-green (R/G) ratio decreases significantly from 18.82 to 1.48, inducing a color shift from red to yellow and ultimately to green. In contrast, no color variation is observed when NaLnF4:Er3+ is excited with a 980 nm laser at different power densities. This power-dependent multicolored UCL of NaLnF4:Er3+ excited at 1532 nm can be attributed to the competitive processes of upward pumping and downward relaxation of electrons on the 4I9/2 level of Er3+. By utilizing the unique UC characteristics of NaLnF4:Er3+, its potential utility in anti-counterfeiting applications is demonstrated. Our research highlights the distinctive optical properties of NaLnF4:Er3+ and provides novel insights into the use of luminescent materials in optical anti-counterfeiting technologies.

3.
Langmuir ; 40(39): 20616-20628, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39282865

RESUMO

The production of sludge biochar (SBC) from residual sludge offers a solution to the challenges associated with sludge disposal and facilitates the reutilization of resources. In the present research, a bimetallic-modified sludge biochar, designated as FeCu-SBC, was synthesized by varying the doping ratios of FeSO4 and CuSO4. This material was intended for the effective degradation of tetracycline (TC) in aqueous environments via the activation of peroxydisulfate. The FeCu2-SBC (90% degradation rate) composite, synthesized through the incorporation of Fe and Cu in a 1:2 ratio with SBC, exhibited a degradation rate of TC, which was 2.7 times higher than that of SBC (32.85% degradation rate) and 1.8 times higher than that of FeCu (50% degradation rate). Research examining the mechanisms involved revealed that FeCu underwent degradation solely through the radical (•OH) pathway, whereas FeCu2-SBC was subject to degradation through both radical (SO4•-) and nonradical (1O2) pathways. This phenomenon was attributed to the distinct π-π, C═O, and defect structures in FeCu2-SBC compared to FeCu, which facilitated the activation process leading to the production of reactive species. This investigation presented a cost-effective approach for producing bimetallic-modified sludge biochar, offering perspectives on determining the crucial elements influencing the streamlined TC degradation pathway.


Assuntos
Carvão Vegetal , Ferro , Esgotos , Tetraciclina , Carvão Vegetal/química , Tetraciclina/química , Esgotos/química , Ferro/química , Cobre/química , Peróxido de Hidrogênio/química , Poluentes Químicos da Água/química , Poluentes Químicos da Água/isolamento & purificação
4.
Langmuir ; 40(12): 6198-6211, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38468362

RESUMO

Titanium silicon molecular sieve (TS-1) is an oxidation catalyst that possesses a long lifetime of charge transfer excited state, high Ti utilization efficiency, large specific surface area, and good adsorption property; therefore, TS-1 acts as a Ti-based photocatalyst candidate. In this work, TS-1 coupled Bi2MoO6 (TS-1/BMO) photocatalysts were fabricated via a facile hydrothermal route. Interestingly, the optimized TS-1/BMO-1.0 catalyst exhibited a decent photodegradation property toward tetracycline hydrochloride (85.49% in 120 min) under the irradiation of full spectrum light, which were 4.38 and 1.76 times compared to TS-1 and BMO, respectively. The enhanced photodegradation property of the TS-1/BMO-1.0 catalyst could be attributed to the reinforced light-harvesting capacity of the photocatalyst, high charge mobility, and suitable band structure for tetracycline hydrochloride degradation. In addition, the mechanism of photocatalytic degradation of tetracycline hydrochloride by the TS-1/BMO-1.0 catalyst was reasonably proposed based on the band structure, trapping, and ESR tests. This research provided feasible ideas for the design and construction of high-efficiency photocatalysts for contaminant degradation.

5.
Langmuir ; 40(11): 5590-5605, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38457783

RESUMO

Metal-organic frameworks (MOFs) have garnered attention across various fields due to their noteworthy features like high specific surface area, substantial porosity, and adjustable performance. In the realm of water treatment, MOFs exhibit great potential for eliminating pollutants such as organics, heavy metals, and oils. Nonetheless, the inherent powder characteristics of MOFs pose challenges in terms of recycling, pipeline blockage, and even secondary pollution in practical applications. Addressing these issues, the incorporation of MOFs into sponges proves to be an effective solution. Strategies like one-pot synthesis, in situ growth, and impregnation are commonly employed for loading MOFs onto sponges. This review comprehensively explores the synthesis strategies of MOFs and sponges, along with their applications in water treatment, aiming to contribute to the ongoing advancement of MOF materials.

6.
Ecotoxicol Environ Saf ; 283: 116846, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-39116693

RESUMO

Myriophyllum aquaticum (M. aquaticum), as a Cd-highly enriched and tolerant species, has greater application in phytoremediation of Cd-polluted waters. Mechanisms of Cd uptake and transport of M. aquaticum were comprehensively investigated in this work. Transport direction of Cd was observed both from the roots to the aboveground and vice versa. The aboveground can be harvested during vigorous growth and flowering periods, further improving the efficient phytoremediation of Cd-polluted wastewater. Moreover, analysis of transpiration inhibition, low-temperature treatment and metabolic inhibition indicated that the uptake and transport of Cd by M. aquaticum can be achieved via the coexistence of the free diffusion-dominated apoplast pathway dominated by transpiration and the "cellular pathway" dominated by active absorption, with the active energy-demanding cellular pathway playing a dominant role. The obtained results have important implications in the in-depth exploration of uptake, transport and distribution mechanisms of heavy metals during phytoremediation of aquatic plants.


Assuntos
Biodegradação Ambiental , Cádmio , Raízes de Plantas , Poluentes Químicos da Água , Áreas Alagadas , Cádmio/metabolismo , Poluentes Químicos da Água/metabolismo , Raízes de Plantas/metabolismo , Transporte Biológico , Águas Residuárias , Magnoliopsida/metabolismo
7.
J Environ Sci (China) ; 142: 43-56, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38527895

RESUMO

Alkali metal potassium was beneficial to the electronic regulation and structural stability of transition metal oxides. Herein, K ions were introduced into manganese oxides by different methods to improve the degradation efficiency of toluene. The results of activity experiments indicated that KMnO4-HT (HT: Hydrothermal method) exhibited outstanding low-temperature catalytic activity, and 90% conversion of toluene can be achieved at 243°C, which was 41°C and 43°C lower than that of KNO3-HT and Mn-HT, respectively. The largest specific surface area was observed on KMnO4-HT, facilitating the adsorption of toluene. The formation of cryptomelane structure over KMnO4-HT could contribute to higher content of Mn3+ and lattice oxygen (Olatt), excellent low-temperature reducibility, and high oxygen mobility, which could increase the catalytic performance. Furthermore, two distinct degradation pathways were inferred. Pathway Ⅰ (KMnO4-HT): toluene → benzyl → benzoic acid → carbonate → CO2 and H2O; Pathway ⅠⅠ (Mn-HT): toluene → benzyl alcohol → benzoic acid → phenol → maleic anhydride → CO2 and H2O. Fewer intermediates were detected on KMnO4-HT, indicating its stronger oxidation capacity of toluene, which was originated from the doping of K+ and the interaction between KOMn. More intermediates were observed on Mn-HT, which can be attributed to the weaker oxidation ability of pure Mn. The results indicated that the doping of K+ can improve the catalytic oxidation capacity of toluene, resulting in promoted degradation of intermediates during the oxidation of toluene.


Assuntos
Compostos de Manganês , Manganês , Tolueno , Manganês/química , Oxigênio/química , Dióxido de Carbono , Óxidos/química , Oxirredução , Catálise , Ácido Benzoico
8.
J Clin Nurs ; 32(9-10): 2073-2085, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-35304785

RESUMO

BACKGROUND: Obstetric critical illness is an important factor that leads to an increase in maternal mortality. Early warning assessment can effectively reduce maternal and neonatal mortality and morbidity. However, there are multiple early warning systems, and the effect and applicability of each system in China still need to be explored. OBJECTIVES: To elaborate on the application, effectiveness and challenges of the existing early warning systems for high-risk obstetric women in China and to provide a reference for clinical practice. DESIGN: A scoping review guided by the Arksey and O'Malley framework and reported using the Preferred Reporting Items for Systematic Reviews and Meta-Analysis for scoping review (PRISMA-ScR) guidelines. ELIGIBILITY CRITERIA: We included original studies related to early warning and excluded those that were guidelines, consensus and reviews. The included studies were published in Chinese or English by Chinese scholars as of June 2021. DATA SOURCES: CNKI, Wanfang, VIP, Cochrane, CINAHL, Embase, PubMed and Web of Science databases were searched systematically, and the reference sections of the included papers were snowballed. RESULTS: In total, 598 articles were identified. These articles were further refined using keyword searches and exclusion criteria, and 17 articles met the inclusion criteria. We extracted data related to each study's population, methods and results. Early warning tools, outcome indices, effects and challenges are discussed. CONCLUSIONS: Although all studies have shown that early warning systems have good application effects, the use of early warning systems in China is still limited, with poor regional management and poor sensitivity for specific obstetric women. Future research needs to develop more targeted early warning tools for high-risk obstetric women and address the current challenges in clinical applications.


Assuntos
Estado Terminal , Gravidez , Recém-Nascido , Humanos , Feminino , China , Bases de Dados Factuais
9.
Gut ; 70(1): 180-193, 2021 01.
Artigo em Inglês | MEDLINE | ID: mdl-32253259

RESUMO

OBJECTIVE: Non-alcoholic fatty liver disease (NAFLD) is a common prelude to cirrhosis and hepatocellular carcinoma. The genetic rs641738 C>T variant in the lysophosphatidylinositol acyltransferase 1 (LPIAT1)/membrane bound O-acyltransferase domain-containing 7, which incorporates arachidonic acid into phosphatidylinositol (PI), is associated with the entire spectrum of NAFLD. In this study, we investigated the mechanism underlying this association in mice and cultured human hepatocytes. DESIGN: We generated the hepatocyte-specific Lpiat1 knockout mice to investigate the function of Lpiat1 in vivo. We also depleted LPIAT1 in cultured human hepatic cells using CRISPR-Cas9 systems or siRNA. The effect of LPIAT1-depletion on liver fibrosis was examined in mice fed high fat diet and in liver spheroids. Lipid species were measured using liquid chromatography-electrospray ionisation mass spectrometry. Lipid metabolism was analysed using radiolabeled glycerol or fatty acids. RESULTS: The hepatocyte-specific Lpiat1 knockout mice developed hepatic steatosis spontaneously, and hepatic fibrosis on high fat diet feeding. Depletion of LPIAT1 in cultured hepatic cells and in spheroids caused triglyceride accumulation and collagen deposition. The increase in hepatocyte fat content was due to a higher triglyceride synthesis fueled by a non-canonical pathway. Indeed, reduction in the PI acyl chain remodelling caused a high PI turnover, by stimulating at the same time PI synthesis and breakdown. The degradation of PI was mediated by a phospholipase C, which produces diacylglycerol, a precursor of triglyceride. CONCLUSION: We found a novel pathway fueling triglyceride synthesis in hepatocytes, by a direct metabolic flow of PI into triglycerides. Our findings provide an insight into the pathogenesis and therapeutics of NAFLD.


Assuntos
Aciltransferases/genética , Proteínas de Membrana/genética , Hepatopatia Gordurosa não Alcoólica/etiologia , Fosfatidilinositóis/metabolismo , Triglicerídeos/metabolismo , Animais , Técnicas de Cultura de Células , Modelos Animais de Doenças , Hepatócitos/metabolismo , Hepatócitos/patologia , Humanos , Metabolismo dos Lipídeos , Camundongos , Camundongos Knockout , Hepatopatia Gordurosa não Alcoólica/metabolismo , Hepatopatia Gordurosa não Alcoólica/patologia
10.
Bull Environ Contam Toxicol ; 106(6): 1044-1049, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33825910

RESUMO

Due to the strict control on bisphenol A (BPA) in many countries, bisphenol analogues (BPs) are being widely used as alternative materials to manufacture epoxy resins and polycarbonate plastics, resulting in their occurrence in sewage treatment plants (STPs). In this study, the occurrence and distribution of 7 BPs in a large-scale STP in Beijing China was investigated. Wastewater samples were collected from the influents and effluents of each processing unit, and extracted by solid-phase extraction. Target compounds were quantified by ultra-performance liquid chromatography tandem mass spectrometry (HPLC-MS/MS). The total concentrations of seven BPs (ΣBPs) were 400.42 ± 48.12 ng/L in the raw sewage, 438.60 ± 46.50 ng/L in the primary effluent, 17.21 ± 13.12 ng/L in the secondary effluent, and 11.33 ± 4.84 ng/L in the tertiary effluent, respectively. Bisphenol S (BPS) and BPA were the predominant congener in raw sewage with an overall contribution of 29.32% and 70.22% to the ΣBPs, indicating that there was a large amount of BPS and BPA consumption in the study area. During a one-week sampling period, ΣBPs changed slightly at the same sampling site. It was found that high removal efficiencies were achieved for BPs in anoxic and oxic secondary clarifier treatment units, suggesting that biodegradation and sorption played major roles in BPs elimination in the STP. After tertiary treatment, all BPs except BPA were completely removed, suggesting the necessity to investigate the fate and toxicity of BPA in the aquatic environment.


Assuntos
Esgotos , Poluentes Químicos da Água , Pequim , Compostos Benzidrílicos/análise , China , Fenóis , Esgotos/análise , Espectrometria de Massas em Tandem , Poluentes Químicos da Água/análise
11.
Water Sci Technol ; 81(4): 813-823, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-32460284

RESUMO

A nitrogen-doped reduced graphene oxide/Fe3O4 composite (NGO-Fe3O4) was prepared through the simplified hydrothermal and deposition-precipitation method and characterized by X-ray diffraction, scanning electron microscopy and Fourier transform infrared spectroscopy. The degradation efficiency of oxytetracycline (OTC) by NGO-Fe3O4 activated peroxodisulfate (PDS) under visible light irradiation was studied. The degradation efficiency reached 100% within 32.5 min (the initial OTC concentration 50 mg L-1 and PDS 1 mM; [NGO-Fe3O4]:[ PDS] = 4:1; pH = 3.0). No apparent decrease in degradation efficiency was observed after five cycles. SO4 -· and ·OH were the main active oxides for OTC degradation in this system. Moreover, four degradation pathways were proposed, namely hydroxylation, dehydration, decarbonylation and demethylation according to the analysis results of high-performance liquid chromatography mass spectrometry.


Assuntos
Oxitetraciclina , Luz , Microscopia Eletrônica de Varredura , Óxidos , Difração de Raios X
12.
Phys Chem Chem Phys ; 17(35): 22711-20, 2015 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-26256454

RESUMO

The aggregation and fibril formation of amyloid ß(Aß) peptides onto a ganglioside-GM1-containing lipid membrane is a cause of neurodegenerative diseases. The mechanism of the initial binding and the conformational changes of Aß on the membrane should be clarified. Fluorescence microscopy and Raman spectroscopy have been performed to investigate the supporting planar lipid bilayers (SPBs) composed of ganglioside-GM1, sphingomyelin and cholesterol. It is demonstrated that the SPBs are in a liquid-crystalline state when placed on mica, and increasing the amount of ganglioside-GM1 can decrease the lateral interaction between the acyl chains of the SPBs. It has been found that Aß(1-40) initially interacts with the galactose ring of the ganglioside-GM1 head group, leading to its binding and gradual aggregation on the membrane surface. The obvious change observed in Raman spectroscopy in the ν(C-H) region confirms that the hydrophobic C-terminal of Aß(1-40) inserts itself into the hydrophobic part of the SPBs. The Raman data indicate that α-helix and ß-sheet structures of Aß(1-40) increase and coexist over longer time frames. Based on these results, a model was proposed to describe the mechanism of the conformational changes and the aggregation of Aß(1-40) that are mediated by ganglioside-GM1-containing SPBs.


Assuntos
Peptídeos beta-Amiloides/química , Colesterol/química , Gangliosídeo G(M1)/química , Bicamadas Lipídicas/química , Fragmentos de Peptídeos/química , Esfingomielinas/química , Silicatos de Alumínio/química , Interações Hidrofóbicas e Hidrofílicas , Análise Espectral Raman , Propriedades de Superfície
13.
Angew Chem Int Ed Engl ; 54(50): 15276-9, 2015 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-26482125

RESUMO

Contrary to the classical silylene dimerization leading to a disilene structure, phosphine stabilized hydro- and chloro-silylenes (2 a,b) undergo an unique dimerization via silylene insertion into SiX σ-bonds (X=H, Cl), which is reversible at room temperature. DFT calculations indicate that the insertion reaction proceeds in one step in a concerted manner.

14.
ChemSusChem ; 17(9): e202400241, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38494446

RESUMO

The design of high activity catalyst for the efficiently conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) gains great interest. The rationally tailoring of electronic structure directly affects the interaction between catalysts and organic substrates, especially molecular oxygen as the oxidant. This work, the bimetallic catalysts AuPd/CeO2 were prepared by the combining method of chemical reduction and photo-deposition, effectively concerting charge between Au and Pd and forming the electron-rich state of Au. The increasing of oxygen vacancy concentration of CeO2 by acidic treatment can facilitate the adsorption of HMF for catalysts and enhance the yield of FDCA (99.0 %). Moreover, a series of experiment results combining with density functional theory calculation illustrated that the oxidation performance of catalyst in HMF conversion was strongly related to the electronic state of interfacial Au-Pd-CeO2. Furthermore, the electron-rich state sites strengthen the adsorption and activation of molecular oxygen, greatly promoting the elimination of ß-hydride for the selective oxidation of 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) to FDCA, accompanied with an outgoing FDCA formation rate of 13.21 mmol ⋅ g-1 ⋅ min-1 at 80 °C. The perception exhibited in this research could be benefit to understanding the effects of electronic state for interfacial sites and designing excellent catalysts for the oxidation of HMF.

15.
ACS Appl Mater Interfaces ; 16(38): 51055-51064, 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39276066

RESUMO

Broadband photodetectors covering ultraviolet (UV) to near-infrared (NIR) wavelengths play an essential role in communications, imaging, and biosensing. Developing a single photodetector with a broadband optical response operating at room temperature can significantly reduce the complexity and cost of receiver systems for multispectral applications. In this work, utilizing the porous structure characteristics of Cs2AgBiBr6:Sn thin films, a self-powered detector with broad spectral response (UV-vis-NIR) was achieved by constructing an effective Cs2AgBiBr6:Sn/PDPP3T heterojunction. This photodetector possesses a broad response spectrum from 350 to 950 nm with an average detection rate exceeding 1011 Jones and maintains excellent photoelectric performance over two months. Sn2+ doping effectively reduces the bandgap of Cs2AgBiBr6, enhancing its near-infrared absorption and optimizing energy level alignment with conjugated polymer (diketopyrrolopyrrole-terthiophene, PDPP3T). More importantly, the porous structure derived from Sn doping significantly improves carrier extraction and transport under a near-infrared light response at the heterojunction interface. Utilizing its broad spectral response characteristics in the UV-vis-NIR range, a novel information transfer and encryption system employing full optical modulation has been realized within a single perovskite photodetector. This work provides a new approach to fabricating lead-free double perovskite broadband photodetectors with potential applications in photonic devices.

16.
Environ Sci Pollut Res Int ; 31(25): 36702-36715, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38753232

RESUMO

The composite material SBC-Fe-x with sludge and Fe3+ was developed by different calcination temperatures (600, 700, and 800 °C) for the removal of tetracycline (TC). The adsorption rates of SBC-Fe-600, SBC-Fe-700, and SBC-Fe-800 were 77.5%, 89%, and 91%, respectively. Furthermore, the Langmuir model indicated that the maximum adsorption capacity of SBC-Fe-700 (157.93 mg/g) was three times greater than that of SBC-Fe-600. The conclusions were confirmed by a series of characterizations that SBC-Fe-700 showed a larger specific surface area, well-developed pore structure, rich oxygen-containing functional groups and a high degree of graphitization. The results of pH experiments indicated the broad applicability of SBC-Fe-700 for TC adsorption. In addition, SBC-Fe-700 suggested outstanding performance in different water environments. This work produced a feasible adsorbent for the removal of TC, and a new direction for sludge resource utilization was proposed.


Assuntos
Carvão Vegetal , Esgotos , Tetraciclina , Poluentes Químicos da Água , Tetraciclina/química , Adsorção , Esgotos/química , Carvão Vegetal/química , Poluentes Químicos da Água/química , Pirólise , Ferro/química , Temperatura , Purificação da Água/métodos
17.
ACS Nano ; 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38951518

RESUMO

Global warming is a crisis that humanity must face together. With greenhouse gases (GHGs) as the main factor causing global warming, the adoption of relevant processes to eliminate them is essential. With the advantages of high specific surface area, large pore volume, and tunable synthesis, metal-organic frameworks (MOFs) have attracted much attention in GHG storage, adsorption, separation, and catalysis. However, as the pool of MOFs expands rapidly with new syntheses and discoveries, finding a suitable MOF for a particular application is highly challenging. In this regard, high-throughput computational screening is considered the most effective research method for screening a large number of materials to discover high-performance target MOFs. Typically, high-throughput computational screening generates voluminous and multidimensional data, which is well suited for machine learning (ML) training to improve the screening efficiency and explore the relationships between the multidimensional data in depth. This Review summarizes the general process and common methods for using ML to screen MOFs in the field of GHG removal. It also addresses the challenges faced by ML in exploring the MOF space and potential directions for the future development of ML for MOF screening. This aims to enhance the understanding of the integration of ML and MOFs in various fields and broaden the application and development ideas of MOFs.

18.
Guang Pu Xue Yu Guang Pu Fen Xi ; 33(5): 1215-9, 2013 May.
Artigo em Zh | MEDLINE | ID: mdl-23905322

RESUMO

Dithiobis-succinimidyl propionate (DTSP), an important homobifunctional crosslinker, has been widely used for the covalent immobilization of proteins onto solid supports by amine coupling. In the present study, adsorption of DTSP on vacuum-deposited gold island films was analyzed by means of surface-enhanced infrared absorption spectroscopy (SEIRAS). For the sake of a reliable assignment of the vibrational spectra, IR intensity of the adsorption model of TSP on one gold surface was calculated using density functional theory (DFT) at the Beck' s three-parameter Lee-Yang-Parr (B3LYP) level with the LANL2DZ basis set. SEIRAS and multiple-angle-of-incidence polarization infrared reflection-absorption spectroscopy indicated that TSP is arranged orderly in a tilted fashion with a dihedral angle of 65 degrees between the plane of succinimidyl ring and the gold surface. The binding kinetics revealed that that the time constant of self-assembly of the TSP layer is 220 sec. Furthermore, the coupling process of amino-nitrilotriacetic acid (ANTA) with surface-bound TSP monolayer was monitored in situ by SEIRAS. Three negative bands observed at 1 807, 1 776, and 1 728 cm(-1) respectively provided direct evidence for the reaction of the succinimidyl ester. The appearance of one intense band at 1 566 cm(-1) gave a clear support for the presence of the cross-link between ANTA and TSP. We hope that the results in current investigation will contribute to the better understanding of properties of DTSP and related reactions at the molecular level.


Assuntos
Reagentes de Ligações Cruzadas/química , Ouro/química , Espectrofotometria Infravermelho/métodos , Succinimidas/química , Absorção , Eletroquímica , Eletrodos , Propriedades de Superfície
19.
Sci Rep ; 13(1): 3665, 2023 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-36871104

RESUMO

Soil organic carbon (C) and aggregates are the important components of soil fertility and the foundation of sustainable agriculture. The storage and protection of SOC in aggregates is widely regarded as the material basis of soil organic C accumulation. However, current understanding of soil aggregate and its associated organic C is insufficient to elucidate the regulation mechanism of soil organic C. A nine-year field experiment including chemical fertilizer (FR) and organic manure (OM) treatments was set up in the eastern plain of Funiu Mountain, central China. Using chemical analysis, physical sieving as well as nuclear magnetic resonance (NMR) methods, we mainly probed into the response of soil organic C concentration and composition, and C functional groups, water-stable aggregates to different treatments. Furthermore, scanning electronic microscopy (SEM) and partial least square structural equation modelling (PLS-SEM) was conducted to characterise the different size aggregates and to analyse the mechanism of soil organic C accumulation and stabilisation at aggregate scales. After nine years of farming, OM treatment substantially increased soil organic C content (by 3.77 g kg-1) and significantly enhanced the formation of macro-aggregates (> 250 µm), while FR had no significant influence on soil organic C. At the aggregate scale, the amounts of soil organic C, C physical fractions (particulate and mineral-associated organic C), total nitrogen and microbial biomass carbon associated in macro-aggregates (> 250 µm) were obviously higher than that in micro-aggregates and silt + clay fraction, and OM treatment greatly increased the accumulation of soil organic C and its components in macro-aggregates. Moreover, microbial biomass carbon (MBC) amounts in aggregates were remarkably increased (27-116%) by the application of OM. And MBC had a positively effect on the physical fractions of SOC but not on the C chemical structure within aggregates. The present study indicated that soil organic C accumulation mainly rely on macro-aggregates (> 250 µm). Intra-particulate organic carbon (POC) and mineral-associated organic carbon (MOC) within macro-aggregates played an important role in soil organic C accumulation. Meanwhile, soil microbes were a driving force for the accumulation of soil organic C physical fractions (POC and MOC). We concluded that OM treatment accelerated the synergistic process between organic C sequestration and soil aggregation, and showed great potential to increase soil organic C accumulation.

20.
J Colloid Interface Sci ; 646: 922-931, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37235937

RESUMO

Recently, quasi two-dimensional (Q-2D) perovskites with alternating cations in the interlayer space (ACI) have attracted more attentions owing to their elevated stability compared with three-dimensional (3D) analogs. While the efficiency of the devices derived from Q-2D perovskites is much smaller than that based on 3D perovskites. Here, we utilized urea and methoxyamine hydrochloride (MOAH) dual additives to acquire high quality Q-2D ACI perovskite GA(MA)5Pb5I16 (GA = guanidinium, MA = methylammonium) films. The efficiency of the perovskite solar cells (PSCs) derived from the Q-2D perovskite films induced by the synergistic effect of urea and MOAH dual additives increases to 20.32% from 17.21% for the devices without additive. This efficiency enhancement could be attributed to the enlarged grain size, improved crystallinity, optimized quantum well thickness distribution, and reduced trap states of the perovskite films. Moreover, the solar cells with dual additives present improved stability. The efficiency of devices with dual additives holds 95% of the original value after storage for 1600 h in ambient air. These results prove that the synergistic effect of urea and MOAH is an effective method to achieve highly efficient and stable Q-2D PSCs.

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