Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 35
Filtrar
1.
J Am Chem Soc ; 146(6): 4153-4161, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38300827

RESUMO

Separating ethane (C2H6) from ethylene (C2H4) is an essential and energy-intensive process in the chemical industry. Here, we report two flexible diamondoid coordination networks, X-dia-1-Ni and X-dia-1-Ni0.89Co0.11, that exhibit gate-opening between narrow-pore (NP) and large-pore (LP) phases for C2H6, but not for C2H4. X-dia-1-Ni0.89Co0.11 thereby exhibited a type F-IV isotherm at 273 K with no C2H6 uptake and a high uptake (111 cm3 g-1, 1 atm) for the NP and LP phases, respectively. Conversely, the LP phase exhibited a low uptake of C2H4 (12.2 cm3 g-1). This C2H6/C2H4 uptake ratio of 9.1 for X-dia-1-Ni0.89Co0.11 far surpassed those of previously reported physisorbents, many of which are C2H4-selective. In situ variable-pressure X-ray diffraction and modeling studies provided insight into the abrupt C2H6-induced structural NP to LP transformation. The promise of pure gas isotherms and, more generally, flexible coordination networks for gas separations was validated by dynamic breakthrough studies, which afforded high-purity (99.9%) C2H4 in one step.

2.
J Hazard Mater ; 466: 133624, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38295726

RESUMO

The generation, migration and reaction paths of electrons are the key steps for photodegradation of pollutants. However, efficient operation of the above pathways is still challenging. Herein, by strong coordination and slow pyrolysis, we constructed a narrow band Zn-Mn bimetallic photoactive core-shell material (Mn@Zn-N-C, Eg = 3.38 eV) with abundant oxygen vacancies for enhancing the above electronic paths. The photodegradation experiments of tetracycline hydrochloride (TCH) showed that the formation and transfer of vacancy-induced free electrons in the synthesized Mn@Zn-N-C was the key to improve the photocatalytic activity. The DFT calculation results revealed that the photogenerated electrons can transfer along the Mn-O-Zn bridge in Mn@Zn-N-C, and promote the formation of MnIV, which directly capture the free electrons and reset itself to MnII site. In this case, the introduction of Mn would enhance the separation of h+ and e-. The adjacent vacancies and defects then also trapped the above free electrons and hinder the recombination of photogenerated carriers. Simultaneously, the localized valence electron transfer between the above redox pairs (Mn4+/Mn2+ and Zn2+/Zn0) also promoted the long-term stability of the photocatalytic process. In summary, using vacancy induction strategy to regulate the evolution of valence- and free-electrons is a promising method to improve the production-transfer-utilization efficiency of photogenerated carriers.

3.
Small ; 20(23): e2308005, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38148319

RESUMO

The conversion of CO2 into valuable carbon-based products using clean and renewable solar energy has been a significant challenge in photocatalysis. It is of paramount importance to develop efficient photocatalysts for the catalytic conversion of CO2 using visible light. In this study, the Ni-MOF-74 material is successfully modified to achieve a highly porous structure (Ni-74-Am) through temperature and solvent modulation. Compared to the original Ni-MOF-74, Ni-74-Am contains more unsaturated Ni active sites resulting from defects, thereby enhancing the performance of CO2 photocatalytic conversion. Remarkably, Ni-74-Am exhibits outstanding photocatalytic performance, with a CO generation rate of 1380 µmol g-1 h-1 and 94% CO selectivity under visible light, significantly surpassing the majority of MOF-based photocatalysts reported to date. Furthermore, experimental characterizations reveal that Ni-74-Am has significantly higher efficiency of photogenerated electron-hole separation and faster carrier migration rate for photocatalytic CO2 reduction. This work enriches the design and application of defective MOFs and provides new insights into the design of MOF-based photocatalysts for renewable energy and environmental sustainability. The findings of this study hold significant promise for developing efficient photocatalysts for CO2 reduction under visible-light conditions.

4.
Ecotoxicol Environ Saf ; 268: 115691, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37979359

RESUMO

The slow rate of electron transfer and the large consumption of carbon sources are technical bottlenecks in the biological treatment of wastewater. Here, we first proposed to domesticate aerobic denitrifying bacteria (ADB) from heterotrophic to autotrophic by electricity (0.6 V) under zero organic carbon source conditions, to accelerate electron transfer and shorten hydraulic retention time (HRT) while increasing the biodegradation rate. Then we investigated the extracellular electron transfer (EET) mechanism mediated by this process, and additionally examined the integrated nitrogen removal efficiency of this system with composite pollution. It was demonstrated that compared with the traditional membrane bioreactor (MBR), the BEC displayed higher nitrogen removal efficiency. Especially at C/N = 0, the BEC exhibited a NO3--N removal rate of 95.42 ± 2.71 % for 4 h, which was about 6.5 times higher than that of the MBR. Under the compound pollution condition, the BEC still maintained high NO3--N and tetracycline removal (94.52 ± 2.01 % and 91.50 ± 0.001 %), greatly superior to the MBR (10.64 ± 2.01 % and 12.00 ± 0.019 %). In addition, in-situ electrochemical tests showed that the nitrate in the BEC could be directly converted to N2 by reduction using electrons from the cathode, which was successfully demonstrated as a terminal electron acceptor.


Assuntos
Desnitrificação , Elétrons , Carbono , Processos Heterotróficos , Processos Autotróficos , Nitratos , Nitrogênio/metabolismo , Reatores Biológicos
5.
iScience ; 26(10): 107933, 2023 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-37841594

RESUMO

Catalytic conversion of biomass provides an alternative way for the production of organic acids from renewable feedstocks. The emerging process contains complex reactions and strategies to cut down those complex biogenic materials into target molecules. Here, we review the catalytic conversion of cellulosic biomass toward high-valued organic acids. This work has summarized the key controlling reactions which lead toward formic acid, glycolic acid, or sugar acids in oxidative conditions and the main pathways for lactic acid or levulinic acid in the anaerobic environment from cellulosic biomass and its derivatives. We evaluate and compare different strategies and methods such as one-pot and two-step conversion. Additionally, the optimization of catalytic reactions has been discussed to realize the design of C-C coupling reactions, the development of multifunctional materials, and new efficient system. In all, this article gives an insight guide to precisely convert cellulosic biomass into target organic acids.

6.
Environ Pollut ; 336: 122449, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37633439

RESUMO

Although alkaline sulfite activation of ferrate (Fe(VI)) has advantages of fast response and high activity for degradation of organic contaminants, the specific production pathways of active species and the pH conditions still hinder its widespread application. Based on this, our study constructed a novel advanced oxidation process of calcium sulfite (CaSO3) could activated Fe(VI) continuously by Ca2+ buffering and investigated the mechanism under different pH values and CaSO3 dosages with ciprofloxacin as a target organic pollutant. The results showed that Ca2+ stabilized the process at a neutral/weakly alkaline microenvironment of pH 7-8, which could alleviate the hydrolysis of ≡FeIV=O by protons and iron hydroxyl groups. Besides, the removal of pollutants occurred efficiently when sulfate (SO32-) was excessive and had a 3:1 ratio of SO32- to Fe(VI), achieving more than 99% removal of electron-rich phenolic organic pollutants within 2 min. By adding different radical scavengers and combining electrochemical analysis methods and electron paramagnetic resonance spectroscopy techniques to revealed that the main active species in Fe(VI)/CaSO3 process were ≡FeIV=O/≡FeV=O. Furthermore, the reactivity of various sulfate species (such as SO32-, SO3•-, SO4•-, SO5•-) with Fe(VI) was calculated using density functional theory (DFT), and it was found that Fe(VI)-SO32- reaction has a much lower energy barrier (-36.08 kcal/mol), indicating that SO32- can readily activate Fe(VI) and generate ≡FeIV=O to attack the atoms with high Fukui index (f -) in organic pollutants. The above results confirm the feasibility of Fe(VI)/CaSO3 process. Thus, this study can theoretically and practically prove that the main active species is ≡FeIV=O, rather than SO4•- or •OH in Fe(VI)/CaSO3 process.


Assuntos
Cálcio , Poluentes Químicos da Água , Poluentes Químicos da Água/análise , Ferro/química , Oxirredução , Sulfitos , Óxidos de Enxofre , Sulfatos
7.
RSC Adv ; 13(35): 24628-24638, 2023 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-37601589

RESUMO

Acetylene hydrogenation is a well-accepted solution to reduce by-products in the ethylene production process, while one of the key technical difficulties lies in developing a catalyst that can provide highly dispersed active sites. In this work, a highly crystalline layered covalent organic framework (COF) material (TbBpy) with excellent thermal stability was synthesized and firstly applied as support for ultrasmall Pd nanoparticles to catalyze acetylene hydrogenation. 100% of C2H2 conversion and 88.2% of C2H4 selectivity can be obtained at 120 °C with the space velocity of 70 000 h-1. The reaction mechanism was elucidated by applying a series of characterization techniques and theoretical calculation. The results indicate that the coordination between Pd and N atom in the bipyridine functional groups of COFs successfully increased the dispersibility and stability of Pd particles, and the introduction of COFs not only improved the adsorption of acetylene and H2 onto catalyst surface, but enhanced the electron transfer process, which can be responsible for the high selectivity and activity of catalyst. This work, for the first time, reported the excellent performance of Pd@TbBpy as a catalyst for acetylene hydrogenation and will facilitate the development and application of COFs materials in the area of petrochemicals.

8.
RSC Adv ; 13(36): 24878-24886, 2023 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-37614796

RESUMO

A new simple Pt(ii) terpyridyl salt that shows reversible response towards acetonitrile and irreversible response towards methanol has been reported, accompanied with the colorimetric/luminescent changing from red to yellow. Experimentally and theoretically, the spectroscopic change derives from the hydrogen bonds between crystal water in the Pt(ii) terpyridyl salt and external organic molecules, and the different strength of hydrogen bond leads either reversible or irreversible stimuli-response. Furthermore, this Pt(ii) terpyridyl salt has been on one hand applied as a probe for sensing acetonitrile in water solution, with high selectivity, good reversibility, proper sensitivity and fast response rate, and on the other hand as advanced anticounterfeiting materials. The current study provides a new approach to acquire and design either reversible or irreversible stimuli-responsive luminescent materials.

9.
Environ Sci Technol ; 57(34): 12922-12930, 2023 08 29.
Artigo em Inglês | MEDLINE | ID: mdl-37580903

RESUMO

FeOCl is a highly effective candidate material for advanced oxidation process (AOP) catalysts, but there remain enormous uncertainties about the essence of its outstanding activity. Herein, we clearly elucidate the mechanism involved in the FeOCl-catalyzed perdisulfate (PDS) activation, and the role of surface hydroxyls in bridging the electron transfer between Fe sites and PDS onto the FeOCl/H2O interface is highlighted. ATR-FTIR and Raman analyses reveal that phosphate could suppress the activity of FeOCl via substituting its surface hydroxyls, demonstrating the essential role of hydroxyl in PDS activation. By the use of X-ray absorption fine structure and density functional theory calculations, we found that the polar surface of FeOCl experienced prominent hydrolyzation, which enriched abundant electrons within the microarea around the Fe site, leading to a stronger attraction between FeOCl and PDS. As a result, PDS adsorption onto the FeOCl/H2O interface was obviously enhanced, the bond length of O-O in adsorbed PDS was lengthened, and the electron transfer from Fe atoms to O-O was also promoted. This work proposed a new strategy for PDS-based AOP development and a hint of building efficient heterogeneous AOP catalysts via regulating the hydroxylation of active sites.


Assuntos
Elétrons , Radical Hidroxila , Transporte de Elétrons , Oxirredução
10.
RSC Adv ; 13(22): 15041-15054, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37200691

RESUMO

The GO- and SBA-15-modified UiO-66 adsorbents were developed for removal of trace Cr(vi) from wastewater and investigated to understand the effect of different hybrid ways on the absorption activity and reaction mechanism. The characterization results confirmed that the UiO-66 nanoparticles could be encapsulated by the SBA-15 matrix and anchored onto GO layers. Due to different exposure modes, the adsorption results showed that the GO-modified UiO-66 had better Cr(vi) trapping performance with the maximum removal efficiency of 97% within 3 min, presenting one of the most efficient Cr(vi) removal materials. Kinetic models showed that the adsorption process included fast, exothermic, spontaneous and pseudo-secondary chemical adsorption. By comparison with the Freundlich and Temkin model, the results revealed that the adsorption process of Cr(vi) by UiO-66@SBA-15 involved some multi-layer physical adsorption, while Cr(vi) was adsorbed onto the UiO-66@GO surface. The mechanism study also found that the fixation of Cr was the chemical action of UiO-66 on GO. Additionally, the encapsulated way increases the protection of UiO-55 from surface damage. In all, both hard-core-shell UiO-66@SBA-15 and piece UiO-66@Go increase the absorption activity of Cr(vi), but the different hybrid ways lead to different activities, absorption processes and regeneration abilities.

11.
Sci China Life Sci ; 66(9): 2167-2184, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-37115490

RESUMO

MYC is an oncogenic transcription factor with a novel role in enhancing global transcription when overexpressed. However, how MYC promotes global transcription remains controversial. Here, we used a series of MYC mutants to dissect the molecular basis for MYC-driven global transcription. We found that MYC mutants deficient in DNA binding or known transcriptional activation activities can still promote global transcription and enhance serine 2 phosphorylation (Ser2P) of the RNA polymerase (Pol) II C-terminal domain (CTD), a hallmark of active elongating RNA Pol II. Two distinct regions within MYC can promote global transcription and Ser2P of Pol II CTD. The ability of various MYC mutants to promote global transcription and Ser2P correlates with their ability to suppress CDK9 SUMOylation and enhance positive transcription elongation factor b (P-TEFb) complex formation. We showed that MYC suppresses CDK9 SUMOylation by inhibiting the interaction between CDK9 and SUMO enzymes including UBC9 and PIAS1. Furthermore, MYC's activity in enhancing global transcription positively contributes to its activity in promoting cell proliferation and transformation. Together, our study demonstrates that MYC promotes global transcription, at least in part, by promoting the formation of the active P-TEFb complex via a sequence-specific DNA-binding activity-independent manner.


Assuntos
Fator B de Elongação Transcricional Positiva , Sumoilação , Fator B de Elongação Transcricional Positiva/genética , Fator B de Elongação Transcricional Positiva/metabolismo , Fatores de Transcrição/metabolismo , Fosforilação , RNA Polimerase II/genética , RNA Polimerase II/metabolismo , DNA/genética , DNA/metabolismo , Transcrição Gênica
12.
Int J Biol Macromol ; 237: 124121, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-36966858

RESUMO

A scheme combining alkali­oxygen cooking and ultrasonic etching cleaning was developed for the short range preparation of CNF from bagasse pith, which has a soft tissue structure and is rich in parenchyma cells. This scheme expands the utilization path of sugar waste sucrose pulp. The effect of NaOH, O2, macromolecular carbohydrates, and lignin on subsequent ultrasonic etching was analyzed, and it was found that the degree of alkali­oxygen cooking was positively correlated with the difficulty of subsequent ultrasonic etching. The mechanism of ultrasonic nano-crystallization was found to be the bidirectional etching mode from the edge and surface cracks of the cell fragments by ultrasonic microjet in the microtopography of CNF. The optimum preparation scheme was obtained under the condition of 28 % NaOH content and 0.5 MPa O2, which solves the problem of low-value utilization of bagasse pith and environmental pollution, providing a new possibility for the source of CNF.


Assuntos
Álcalis , Oxigênio , Oxigênio/química , Álcalis/química , Hidróxido de Sódio/química , Ultrassom , Celulose/química , Carboidratos , Culinária
13.
ACS Nano ; 17(3): 1725-1738, 2023 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-36734978

RESUMO

Converting carbon dioxide (CO2) into value-added fuels or chemicals through photothermal catalytic CO2 hydrogenation is a promising approach to alleviate the energy shortage and global warming. Understanding the nanostructured material strategies in the photothermal catalytic CO2 hydrogenation process is vital for designing photothermal devices and catalysts and maximizing the photothermal CO2 hydrogenation performance. In this Perspective, we first describe several essential nanomaterial design concepts to enhance sunlight absorption and utilization in photothermal CO2 hydrogenation. Subsequently, we review the latest progress in photothermal CO2 hydrogenation into C1 (e.g., CO, CH4, and CH3OH) and multicarbon hydrocarbon (C2+) products. Finally, the relevant challenges and opportunities in this exciting research realm are discussed. This perspective provides a comprehensive understanding for the light-heat synergy over nanomaterials and instruction for rational photothermal catalyst design for CO2 utilization.

14.
PLoS Negl Trop Dis ; 16(11): e0010954, 2022 11.
Artigo em Inglês | MEDLINE | ID: mdl-36413567

RESUMO

BACKGROUND: Arginine kinase (AK) is one of the crucial enzymes involved in energy metabolism in invertebrates, and has been proposed as the target for RNA interference (RNAi)-based control of agricultural insect pests. While there is only one AK gene in most insects, two AK genes were identified in Culex pipiens pallens, the primary vector of lymphatic filariasis and epidemic encephalitis. METHODS: The full-length cDNA sequences of CpAK1 and CpAK2 genes were obtained by reverse transcription PCR(RT-PCR) and rapid amplification of cDNA ends (RACE). The expression levels of CpAK1 and CpAK2 in different developmental stages and tissues were detected by reverse transcription quantitative PCR (RT-qPCR). The role of CpAK1 and CpAK2 in the reproduction and blood feeding behavior was analyzed using RNA interference (RNAi). RESULTS: Full-length cDNAs of CpAK1 and CpAK2 were isolated from Cx. pipiens pallens. Analysis of the expression pattern revealed that the mRNA level of CpAK1 was significantly higher than CpAK2 in all development stages and tissues examined, and the expressions of both CpAK1 and CpAK2 were upregulated in response to blood feeding. The co-knockdown of CpAK1 and CpAK2 mediated by RNAi led to high mortality (74.3%) of adult female mosquitoes and decreased hatchability (59.9%). Remarkably, the blood feeding rate and the engorgement rate of the female mosquitoes were negatively affected by co-injection of dsRNAs targeting CpAK1 and CpAK2. CONCLUSION: CpAK1 and CpAK2 were detected in all developmental stages and tissues, but showed divergence in expression level. RNAi-mediated knockdown of AK genes leads to high mortality and negatively affect blood-feeding behavior of Cx. pipiens pallens, suggesting that AK could be used for the target of RNAi-based mosquito control in the future.


Assuntos
Arginina Quinase , Culex , Feminino , Animais , Culex/genética , Interferência de RNA , Mosquitos Vetores , Comportamento Alimentar
15.
J Environ Manage ; 323: 116256, 2022 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-36126592

RESUMO

Defects and vacancies are the essential reasons for the removal of heavy metal ions from wastewater by low-cost biochar materials. This study aimed to use chemically activated hemp stem core alkali extraction residue biochar as an adsorbent to remove nickel (Ni) and copper (Cu) ions from the simulated waste liquid. A large number of defects and vacancies were introduced into the pyrolysis process to study the efficient removal of heavy metal ions Cu and Ni by hemp rod biomass carbon material (HSR-BC) with different carbon base mass ratios and temperatures. The specific surface area of the prepared hemp rod active biochar was highly correlated with the aperture and carbon base ratio and temperature, and reached the maximum value (1429 m2/g) at 600 °C with the ratio of carbon to base (1:3.5). The removal rates of heavy metals Ni(II) and Cu(II) were as high as 94.25% and 99.54%, respectively, and the adsorption capacities were up to 7.85 mg/g and 24.88 mg/g. The adsorption isotherm follows the Langmuir equation and chemo-adsorption was the main adsorption process. Comparing the surface defects and vacancies of biochar materials before and after adsorption showed that the defects of sp-C and oxygen vacancies produced on the edge of the carbon were the main active sites of the biochar material, an amount of carbon defects would become an anchor site for the Lewis acidic groups, the defective acid site strengthened the electron transfer between the functional group and the Ni(II)/Cu(II), promoted the strong cooperation of Ni(II)/Cu(II) ions with -COOH group to enable efficient and rapid adsorption removal. In addition, a large number of carbon-deficient structures could quickly anchor the Ni(II)/Cu(II) due to their local electron deficiency state, which was difficult to desorb. This study provided an in-depth understanding and guidance for the development of low-cost biochar materials with excellent removal performance of heavy metal ions.


Assuntos
Cannabis , Metais Pesados , Poluentes Químicos da Água , Adsorção , Álcalis , Carbono , Carvão Vegetal , Cobre , Íons , Cinética , Metais Pesados/química , Níquel , Oxigênio , Águas Residuárias , Poluentes Químicos da Água/química
16.
Phys Chem Chem Phys ; 24(6): 3686-3694, 2022 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-35080221

RESUMO

A series of LaCoO3 perovskite catalysts substituted by Sr in the A site (La1-xSrxCoO3) were prepared via a facile sol-gel method. The catalytic activity of these perovskite catalysts for the deep oxidation of toluene was evaluated. It was found that Sr substitution significantly enhanced the redox properties, the concentration of oxygen vacancies, and surface Co3+ active species via an electron interaction between Sr and Co from the results of Raman spectroscopy, H2-TPR (temperature programmed reduction), O2-TPD (temperature programmed desorption) and XPS (X-ray photoelectron spectroscopy). Typically, La0.82Sr0.18CoO3 (L0.82S0.18C) exhibited a superior catalytic performance among these samples owing to its best reducibility and highest number of active species. Kinetic analysis further revealed a higher reaction rate (5.1 × 10-7 mol g-1·s-1 at 210 °C) and a lower apparent activation energy (69.1 kJ mol-1) for toluene oxidation on the L0.82S0.18C sample in comparison to those on the others. In situ DRIFTS (diffuse reflectance infrared Fourier transform spectroscopy) confirmed the easy desorption of immediate products from the surface of the L0.82S0.18C sample, which could be responsible for its remarkable performance. These results could provide an efficient strategy for promoting the toluene oxidation through finely tuning the reducibility and surface active phase of the catalysts.

17.
Environ Technol ; 43(4): 489-499, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-32657263

RESUMO

Cold caustic extraction (i.e. CCE) is an essential technique for removing hemicellulose from paper-grade pulp and thus obtaining high-purity dissolving pulp in pulp and paper industry. The generated wastewater from the CCE process contains large amounts of valuable hemicellulose which should be properly treated in a cost-effective way. Therefore, in this research, the hemicellulose has been used as a raw material for preparing hemicellulose-graft-polyacrylamide (hemi-g-pAAm) hydrogel particles for efficiently adsorbing methylene blue (MB) from aqueous solutions. The mass transfer kinetic behaviours of hemicellulose during a multiple CCE process were also studied. The MB adsorption kinetic test results showed that the removal efficiency can be higher than 90% for the simulated wastewater containing 500 mg/L of MB. Of note, the maximum removal capacities for the wastewater samples containing 500 and 1000 mg/L of MB could be reached up to ∼1800 and ∼2300 (mg/g) respectively with the equilibrium time of ∼40 min. Compared to other reported materials, the superior adsorption performance of the prepared hemicellulose-based hydrogel proved its great potential for application in the wastewater treatment of dye industry.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Adsorção , Biomassa , Hidrogéis , Azul de Metileno , Polissacarídeos
18.
Chemosphere ; 291(Pt 3): 132950, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34801575

RESUMO

MIL-100(Fe), a kind of iron-based metal-organic framework materials (MOFs), can be synthesized at room temperature or hydrothermal conditions, which are promising precursor materials for preparing photocatalysts to degrade some recalcitrant chlorophenols in industrial wastewater. However, the relationship between the structural characterization of MIL-100(Fe) derivatives and their photodegradation behavior of chlorophenol pollutants is still unclear. Thus, in this work, a porous Z-scheme α-Fe2O3/MIL-100(Fe) composite was successfully fabricated via partial-pyrolysis of MIL-100(Fe) precursor synthesized through green synthesis route, which was further used for degrading high-concentration of 2,4-dichlorophenol under visible-light illumination (λ > 420 nm). The effects of synthesis route and pyrolysis temperature of MIL-100(Fe) on the degradation efficiencies of as-derived materials for 2,4-dichlorophenol were investigated. The structure-activity relationship was illuminated in detail. Otherwise, the influence of several process factors, i.e., initial concentration and pH of the 2,4-dichlorophenol solution, catalyst dosage on the degradation efficiency of 2,4-dichlorophenol has also been performed. The removal efficiency of 2,4-dichlorophenol with the initial concentration of 100 mg L-1 reached up to 87.65% under optimized conditions. Lastly, the possible mechanism was explored based on trapping experiments and some other characterization results. The study in this paper not only exhibited new insight into the modified α-Fe2O3 material with high photocatalytic activity but also provided a promising method for treating wastewater containing 2,4-dichlorophenol or other similar organic pollutants.


Assuntos
Estruturas Metalorgânicas , Clorofenóis , Fotólise , Relação Estrutura-Atividade
19.
J Biol Chem ; 297(6): 101389, 2021 12.
Artigo em Inglês | MEDLINE | ID: mdl-34762910

RESUMO

SRY-box 2 (Sox2) is a transcription factor with critical roles in maintaining embryonic stem (ES) cell and adult stem cell functions and in tumorigenesis. However, how Sox2 exerts its transcriptional function remains unclear. Here, we used an in vitro protein-protein interaction assay to discover transcriptional regulators for ES cell core transcription factors (Oct4, Sox2, Klf4, and c-Myc) and identified members of the steroid receptor coactivators (SRCs) as Sox2-specific interacting proteins. The SRC family coactivators have broad roles in transcriptional regulation, but it is unknown whether they also serve as Sox2 coactivators. We demonstrated that these proteins facilitate Sox2 transcriptional activity and act synergistically with p300. Furthermore, we uncovered an acetylation-enhanced interaction between Sox2 and SRC-2/3, but not SRC-1, demonstrating it is Sox2 acetylation that promotes the interaction. We identified putative Sox2 acetylation sites required for acetylation-enhanced interaction between Sox2 and SRC-3 and demonstrated that acetylation on these sites contributes to Sox2 transcriptional activity and recruitment of SRC-3. We showed that activation domains 1 and 2 of SRC-3 both display a preferential binding to acetylated Sox2. Finally, functional analyses in mouse ES cells demonstrated that knockdown of SRC-2/3 but not SRC-1 in mouse ES cells significantly downregulates the transcriptional activities of various Sox2 target genes and impairs ES cell stemness. Taken together, we identify specific SRC family proteins as novel Sox2 coactivators and uncover the role of Sox2 acetylation in promoting coactivator recruitment and Sox2 transcriptional function.


Assuntos
Coativador 1 de Receptor Nuclear/metabolismo , Coativador 2 de Receptor Nuclear/metabolismo , Coativador 3 de Receptor Nuclear/metabolismo , Fatores de Transcrição SOXB1/metabolismo , Transcrição Gênica , Acetilação , Animais , Células HEK293 , Células HeLa , Humanos , Camundongos , Coativador 1 de Receptor Nuclear/genética , Coativador 2 de Receptor Nuclear/genética , Coativador 3 de Receptor Nuclear/genética , Fatores de Transcrição SOXB1/genética
20.
J Biol Chem ; 297(4): 101200, 2021 10.
Artigo em Inglês | MEDLINE | ID: mdl-34537242

RESUMO

As a conserved posttranslational modification, SUMOylation has been shown to play important roles in chromatin-related biological processes including transcription. However, how the SUMOylation machinery associates with chromatin is not clear. Here, we present evidence that multiple SUMOylation machinery components, including SUMO E1 proteins SAE1 and SAE2 and the PIAS (protein inhibitor of activated STAT) family SUMO E3 ligases, are primarily associated with the nuclear matrix rather than with chromatin. We show using nuclease digestion that all PIAS family proteins maintain nuclear matrix association in the absence of chromatin. Of importance, we identify multiple histones including H3 and H2A.Z as directly interacting with PIAS1 and demonstrate that this interaction requires the PIAS1 SAP (SAF-A/B, Acinus, and PIAS) domain. We demonstrate that PIAS1 promotes SUMOylation of histones H3 and H2B in both a SAP domain- and an E3 ligase activity-dependent manner. Furthermore, we show that PIAS1 binds to heat shock-induced genes and represses their expression and that this function also requires the SAP domain. Altogether, our study reveals for the first time the nuclear matrix as the compartment most enriched in SUMO E1 and PIAS family E3 ligases. Our finding that PIAS1 interacts directly with histone proteins also suggests a molecular mechanism as to how nuclear matrix-associated PIAS1 is able to regulate transcription and other chromatin-related processes.


Assuntos
Cromatina/metabolismo , Histonas/metabolismo , Proteínas Inibidoras de STAT Ativados/metabolismo , Proteínas Modificadoras Pequenas Relacionadas à Ubiquitina/metabolismo , Sumoilação , Transcrição Gênica , Cromatina/genética , Células HEK293 , Células HeLa , Histonas/genética , Humanos , Domínios Proteicos , Proteínas Inibidoras de STAT Ativados/genética , Proteínas Modificadoras Pequenas Relacionadas à Ubiquitina/genética
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA