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1.
Proc Natl Acad Sci U S A ; 120(26): e2220178120, 2023 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-37339202

RESUMO

The compositional and thermal state of Earth's mantle provides critical constraints on the origin, evolution, and dynamics of Earth. However, the chemical composition and thermal structure of the lower mantle are still poorly understood. Particularly, the nature and origin of the two large low-shear-velocity provinces (LLSVPs) in the lowermost mantle observed from seismological studies are still debated. In this study, we inverted for the 3D chemical composition and thermal state of the lower mantle based on seismic tomography and mineral elasticity data by employing a Markov chain Monte Carlo framework. The results show a silica-enriched lower mantle with a Mg/Si ratio less than ~1.16, lower than that of the pyrolitic upper mantle (Mg/Si = 1.3). The lateral temperature distributions can be described by a Gaussian distribution with a standard deviation (SD) of 120 to 140 K at 800 to 1,600 km and the SD increases to 250 K at 2,200 km depth. However, the lateral distribution in the lowermost mantle does not follow the Gaussian distribution. We found that the velocity heterogeneities in the upper lower mantle mainly result from thermal anomalies, while those in the lowermost mantle mainly result from compositional or phase variations. The LLSVPs have higher density at the base and lower density above the depth of ~2,700 km than the ambient mantle, respectively. The LLSVPs are found to have ~500 K higher temperature, higher Bridgmanite and iron content than the ambient mantle, supporting the hypothesis that the LLSVPs may originate from an ancient basal magma ocean formed in Earth's early history.

2.
Chemistry ; 29(57): e202301457, 2023 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-37449985

RESUMO

As one of the most commonly bulky chemicals, chlorine is conventionally manufactured by electrolysis of NaCl solution in the chlor-alkali process, which requires a huge supply of electrical energy. The photocatalytic route to produce chlorine by using solar energy and NaCl solution offers a promising strategy to reduce energy consumption and bring economic benefits. Herein, it was found that the introduction of CO2 would enhance the productivity of Cl2 from 8.24 µmol⋅h-1 to 39.6 µmol⋅h-1 in NaCl solution over BiOCl. Experimental studies reveal that the CO2 species (CO3 2- ) entered into the crystal texture of BiOCl and the interlayer space between [Bi2 O2 ]2+ slabs were increased and distorted, accelerating the cycle of Cl species. Besides, the cycle of carbonate species also existed and accelerated the reaction efficiency of Cl- oxidation to Cl2 . This work provides a new feasible method of using abundant CO2 resources to accelerate the process of chlorine production via photocatalysis.

3.
Langmuir ; 39(51): 18757-18767, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38096544

RESUMO

Realizing macroscopic superlubricity in the presence of external electric fields (EEFs) at the steel interfaces is still challenging. In this work, macroscopic superlubricity with a coefficient of friction value of approximately 0.008 was realized under EEFs with the lubrication of LiPF6-based ionic liquids at steel interfaces. The roles of cations and anions in the superlubricity realization under EEFs were studied. Based on the experimental results, the macroscopic superlubricity behavior of Li(PEG)PF6 under EEFs at steel interfaces is attributed to the strong hydration effect of Li+ cations and the complete reactions of anions that contributed to the formation of a boundary film on the appropriate surface. Moreover, the reduction in the number of iron oxides in the boundary film on the disc was beneficial for friction reduction. We also provide a calculation model to describe the relationship between the hydration effect and the optimal voltage position, at which the lowest friction might occur. Ultimately, this work proves that macroscopic superlubricity can be realized under EEFs at steel interfaces and provides a foundation for engineering applications of superlubricity in an electrical environment.

4.
Soft Matter ; 19(5): 841-850, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36453836

RESUMO

Structural stabilization for a membrane structure under high-frequency vibration is still a recognized problem. In nature, honeybee wings with non-uniform material properties demonstrate excellent anti-interference ability. However, the correlation between the structural stabilization and mechanical properties of insect wings has not been completely verified. Here we demonstrate that the sclerotization diversity partially distinguishes the stiffness inhomogeneity of the wing structure. Furthermore, a wing cross-section model with diversity in elastic modulus is constructed to analyze the effect of stiffness distribution on stress optimization during flight. Our results demonstrate that the heterogeneous stiffness promotes the stress distribution and structural stabilization of the wing during flight, which may inspire more optimal designs for anisotropic high-strength membrane structures.


Assuntos
Voo Animal , Insetos , Abelhas , Animais , Módulo de Elasticidade , Asas de Animais , Anisotropia , Fenômenos Biomecânicos , Modelos Biológicos
5.
Phys Chem Chem Phys ; 25(42): 28861-28870, 2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37853781

RESUMO

Two-dimensional (2D) materials have garnered significant interest in the fields of optoelectronics and electronics due to their unique and diverse properties. In this work, the electron transport, ferroelectric, piezoelectric, and optical properties of 2D In2Te3 were systematically investigated using first-principles based on density functional theory. The analysis of the phonon spectrum and elastic modulus of the Born effective criterion indicates that the structure of the novel 2D In2Te3 is dynamically stable. The calculation results show that 2D In2Te3 exhibits a carrier mobility as high as 3680.99 cm2 V-1 s-1 (y direction), a high in-plane polarization of 2.428 × 10-10 C m-1, and an excellent ferroelectric phase transition barrier (52.847 meV) and piezoelectric properties (e11 = 1.52 × 10-10 C m-1). The higher carrier mobility is attributed to the band degeneracy and small carrier effective mass. In addition, biaxial strain is an effective way to modulate the band gap and optical properties of 2D In2Te3. These properties indicate that 2D In2Te3 is a promising candidate material for flexible electronic devices and ferroelectric photovoltaic devices.

6.
Nature ; 551(7681): 494-497, 2017 11 22.
Artigo em Inglês | MEDLINE | ID: mdl-29168804

RESUMO

Ultralow-velocity zones (ULVZs) at Earth's core-mantle boundary region have important implications for the chemical composition and thermal structure of our planet, but their origin has long been debated. Hydrogen-bearing iron peroxide (FeO2Hx) in the pyrite-type crystal structure was recently found to be stable under the conditions of the lowermost mantle. Using high-pressure experiments and theoretical calculations, we find that iron peroxide with a varying amount of hydrogen has a high density and high Poisson ratio as well as extremely low sound velocities consistent with ULVZs. Here we also report a reaction between iron and water at 86 gigapascals and 2,200 kelvin that produces FeO2Hx. This would provide a mechanism for generating the observed volume occupied by ULVZs through the reaction of about one-tenth the mass of Earth's ocean water in subducted hydrous minerals with the effectively unlimited reservoir of iron in Earth's core. Unlike other candidates for the composition of ULVZs, FeO2Hx synthesized from the superoxidation of iron by water would not require an extra transportation mechanism to migrate to the core-mantle boundary. These dense FeO2Hx-rich domains would be expected to form directly in the core-mantle boundary region and their properties would provide an explanation for the many enigmatic seismic features that are observed in ULVZs.

7.
Lung ; 201(5): 489-497, 2023 10.
Artigo em Inglês | MEDLINE | ID: mdl-37823901

RESUMO

BACKGROUND: Chimeric antigen receptor T cell (CAR-T) therapy stands as a precise and targeted approach in the treatment of malignancies. In this study, we investigated the feasibility of targeting Cadherin 17 (CDH17) with CDH17 CAR-T cells as a therapeutic modality for small cell lung cancer (SCLC). METHODS: CDH17 expression levels were assessed in human SCLC tumor tissues and cell lines using qPCR and Western blot. Subsequently, we established CDH17 CAR-T cells and assessed their cytotoxicity by co-culturing them with various SCLC cell lines at different effector-to-target (E:T) ratios, complemented by ELISA assays. To ascertain the specificity of CDH17 CAR-T cells, we conducted experiments on SCLC cells with and without CDH17 expression (shRNAs). Furthermore, we employed an SCLC xenograft model to evaluate the in vivo efficacy of CDH17 CAR-T cells. RESULTS: Our results revealed a significant upregulation of CDH17 in both SCLC tissues and cell lines. CDH17 CAR-T cells exhibited robust cytotoxic activity against SCLC cells in vitro, while demonstrating no cytotoxicity towards CDH17-deficient SCLC cells and HEK293 cells that lack CDH17 expression. Importantly, the production of IFN-γ and TNF-α by CDH17 CAR-T cells correlated with their cytotoxic potency. Additionally, treatment with CDH17 CAR-T cells significantly decelerated the growth rate of SCLC-derived xenograft tumors in vivo. Remarkably, no significant difference in body weight was observed between the control group and the group treated with CDH17 CAR-T cells. CONCLUSIONS: The preclinical data open further venues for the clinical use of CDH17 CAR-T cells as an immunotherapeutic strategy for SCLC treatment.


Assuntos
Neoplasias Pulmonares , Receptores de Antígenos Quiméricos , Carcinoma de Pequenas Células do Pulmão , Humanos , Caderinas/metabolismo , Linhagem Celular Tumoral , Células HEK293 , Neoplasias Pulmonares/terapia , Neoplasias Pulmonares/metabolismo , Receptores de Antígenos Quiméricos/genética , Receptores de Antígenos Quiméricos/metabolismo , Carcinoma de Pequenas Células do Pulmão/terapia , Carcinoma de Pequenas Células do Pulmão/metabolismo , Linfócitos T , Imunoterapia Adotiva
8.
Langmuir ; 38(37): 11440-11450, 2022 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-36075054

RESUMO

Oil-impregnated porous polyimide (PI) materials can provide continuous lubricant supply, which is widely used to manufacture space rolling bearing retainers. The lubrication performance of porous polyimide materials mainly depends on their ability to release and recycle lubricants, which is closely related to pore size. In this paper, to investigate the effect of pore size, porous polyimide materials with different pore sizes were prepared by preheating the retainer tube billet during the limit pressing process. The lubricant content rates at each stage were measured by the lubricant immersion and centrifugal release experiment to show the variation of the lubricant content rate in the porous PI sample during a working cycle. At first, the lubricant can be absorbed into the pore. It is found that the absorption rate is faster for lubricants with a smaller viscosity. Moreover, lubricant thinning caused by temperature rise also improves the absorption rate. After lubricant absorption to saturation, the lubricant is released under the centrifugal effect to provide the lubricant. Increasing pore size and using low-viscosity lubricants are the main ways to improve lubrication. Finally, the lubricant on the surface can be recycled into the pore by capillary effect. The smaller the pore size, the faster the lubricant recycles to saturation. These insights gained in this study can provide guidance for the choice of an oil-impregnated porous retainer in different working conditions.

9.
Langmuir ; 38(23): 7346-7356, 2022 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-35637204

RESUMO

Efficient removal of organic dyes from contaminated water has become a great challenge and urgent work due to increasingly serious environmental problems. Here, we have for the first time prepared nanolayer-constructed TiO(OH)2 microstructures which can present negative charge by deprotonation of the hydroxyl group to efficiently and selectively remove cationic dyes from aqueous solution through electrostatic interaction and an attraction mechanism. The nanolayer-constructed TiO(OH)2 microstructures achieve a high adsorption capacity of 257 mg g-1 for methylene blue (MB). The adsorption kinetics, thermodynamics, and isotherms of MB over the TiO(OH)2 microstructures have been studied systemically. The experimental measurements and corresponding analyses demonstrate that the adsorption process of MB on TiO(OH)2 microstructures follows a kinetic model of pseudo-second-order adsorption, agrees well with the Langmuir isotherm mode, and is a spontaneous and exothermic physisorption. Fourier transform infrared (FT-IR) spectra confirm that the prepared TiO(OH)2 microstructures possess hydroxyl group which can deprotonate to present negative charge in solution. Further experimental studies evidently demonstrate that the TiO(OH)2 microstructures also can remove other cationic dyes with positive charge such as basic yellow 1, basic green 4, and crystal violet but cannot adsorb anionic dye of methyl orange (MO) with negative charge in aqueous solution. The measurements for FT-IR spectra and the adsorption of cationic and anionic dyes evidently reveal that the adsorption of cationic dyes over the TiO(OH)2 microstructures is achieved by the electrostatic interaction and attraction between TiO(OH)2 and the dye. This work opens a strategy for the design of new absorbents to efficiently remove organic dyes from aqueous solution through an electrostatic attraction-driven adsorption process.

10.
Plant Dis ; 2022 Mar 12.
Artigo em Inglês | MEDLINE | ID: mdl-35285262

RESUMO

Black scurf and stem canker on potato (Solanum tuberosum L.), caused by Rhizoctonia solani, is one of the most important soil-borne diseases throughout the world. Isolates of R. solani anastomosis group (AG) 3-PT have been reported as the predominant cause of the disease on potato (Carling 1996) and the same results were also obtained in Heilongjiang Province, China (Yang et al. 2017). In October 2020, 14 diseased potato tubers (cv. Youjin-885) with symptoms typically associated with black scurf were found in Hegang City of Heilongjiang in Northeast China, where potatoes are grown for propagation in the breeding nursery. Pieces of sclerotia were removed from the surface of the potato and were surface sterilized with 70% ethanol for 30 s and 0.5% NaClO for 1 min, then rinsed three times with sterile distilled water and placed on potato dextrose agar (PDA) at 25°C in the dark. After incubation for 48 to 72 h, mycelia resembling Rhizoctonia were microscopically examined for morphological characteristics, and hyphal tips transferred to fresh plates of PDA. The characteristics of the observed isolate were typical of R. solani Kühn, which include hyphal branching at right angles, a septum near the branching point and a slight constriction at the branch base (Yang et al. 2015). Hyphal cells were also determined to be multinucleate by staining with 1% safranin O and 3% KOH solution (Bandoni 1979). PCR amplification and DNA sequencing of the internal transcribed spacer (ITS) region of the ribosomal DNA (rDNA) was performed by using the universal primers ITS4/ITS5 (White et al. 1990). The resulting sequence of 700 bp (GenBank accession no. OL770460) showed more than 99% identity to AG 2-2IV isolates present in GenBank (e.g. AB911322; KR259910). On the basis of morphological characteristics and molecular analysis, the isolate was identified as R. solani AG 2-2IV. Pathogenicity of the isolate was tested in greenhouse conditions. Pathogen-free minitubers (cv. Favorita) of approximately the same size (10 to 20 g) were allowed to sprout at room temperature for 10 days. The minitubers were then planted in autoclaved soil in a plastic pot (4 L capacity), placed in a greenhouse at 18 - 27°C (night-day) with 50% relative humidity and watered as required. The pots were inoculated with 7-mm-diameter mycelial plugs (from one PDA petri plate) near the minituber, which was then covered with potting mix. The control pots were inoculated with sterile plugs of PDA. Each treatment consisted of 10 plants, and the experiment was repeated three times. Two months after stems emerged, plants and progeny tubers were harvested and assessed for disease. Stem cankers typical of R. solani infection and black scurf were observed on plants grown in pots inoculated the mycelial plugs, but the control plants remained disease free. Fungi reisolated from symptomatic stems and tubers were identified as R. solani AG 2-2IV using morphological characters and ITS sequences.Sclerotia were observed on PDA by incubating at 25oC in the dark. Although eight AGs have been previously shown to cause black scurf and stem canker in Heilongjiang (Li et al. 2014; Yang et al. 2015; Yang et al. 2017; Yang et al. 2019; Yang et al. 2020), to our knowledge, this is the first report of AG 2-2IV causing disease on potatoes in Heilongjiang Province, the main potato seed production area of China. Early detection of R. solani AG 2-2IV during potato seed production is necessary to prevent its dispersal via infected tubers to other fields across China. The information of which AG is present will assist in developing management strategies for this disease.

11.
Plant Dis ; 106(1): 266-274, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34615364

RESUMO

Common scab (CS) caused by Streptomyces spp. is a significant soilborne potato disease that results in tremendous economic losses globally. Identification of CS-associated species of the genus Streptomyces can enhance understanding of the genetic variation of these bacterial species and is necessary for the control of this epidemic disease. The present study isolated Streptomyces strain 6-2-1(1) from scabby potatoes in Keshan County, Heilongjiang Province, China. PCR analysis confirmed that the strain harbored the characteristic Streptomyces pathogenicity island (PAI) genes (txtA, txtAB, nec1, and tomA). Pathogenicity assays proved that the strain caused typical scab lesions on potato tuber surfaces and necrosis on radish seedlings and potato slices. Subsequently, the strain was systemically characterized at morphological, physiological, biochemical, and phylogenetic levels. Phylogenetic analysis based on 16S rRNA gene sequences revealed that strain 6-2-1(1) shared 99.86% sequence similarity with Streptomyces rhizophilus JR-41T, isolated initially from bamboo in rhizospheric soil in Korea. PCR amplification followed by Sanger sequencing of the 16S rRNA gene of 164 scabby potato samples collected in Heilongjiang Province from 2019 to 2020 demonstrated that approximately 2% of the tested samples were infected with S. rhizophilus. Taken together, these results demonstrate that S. rhizophilus is capable of causing potato CS disease and may pose a potential challenge to potato production in Heilongjiang Province of China.


Assuntos
Solanum tuberosum , Streptomyces , Filogenia , Doenças das Plantas , RNA Ribossômico 16S/genética , Streptomyces/genética
12.
Langmuir ; 37(30): 9162-9169, 2021 Aug 03.
Artigo em Inglês | MEDLINE | ID: mdl-34297577

RESUMO

The retainer of a space rolling bearing widely made of porous polyimide (PI) materials is oil-impregnated and can continuously release lubricants for lubrication. Understanding the lubricant supply mechanism in porous polyimide retainers is important to improve the lubrication performance of space bearings and therefore extends the bearing life. In this work, molecular dynamics simulations are adopted to model the lubricant outflow process from the pore of the PI material. Coarse-grained models are constructed to investigate the lubricant migration behaviors with different pore sizes and radii of rotation. At rest, a lubricant within the pore fails to outflow due to the capillary effect, which decreases with the increase of the pore size. However, for the rotating pores, if the inertial forces generated by the rotational motion exceed the capillary forces, the lubricants will begin to accumulate and some of the lubricants will flow out. Furthermore, the lubricant in the larger pore is easier to outflow due to the smaller capillary forces. This study quantifies the inertial effect and reveals that the centrifugal force is the main mechanism of lubricant outflow from the pores.

13.
Langmuir ; 37(7): 2426-2435, 2021 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-33560132

RESUMO

Porous polyimide (PI) materials are one of important bearing retainer materials in space applications due to the storage and continuous supply of a lubricant through the porous structure. Understanding the lubricant recycling process in porous polyimide retainers is of vital importance to improve lubricant supply performance of bearing. In this work, through molecular dynamic simulations, coarse-grained models are built to study lubricant recycling processes on porous and solid surfaces. A spontaneous imbibition behavior is observed when the lubricant is present on the porous surface. The dynamic change in the contact angle in this process and the deviation of the effective radius from the volumetric radius because of the molecular structure of polyimide causes the classical Lucas-Washburn (L-W) equation fail to describe the process. By fitting dynamic contact angle and effective radius, a modified L-W equation is developed, which well predicts the process of imbibition. Furthermore, it is found that the lubricants between the porous polyimide surface and the solid surface are recycled by extrusion, and spontaneous imbibition does not occur. In this case, the accumulation of lubricant pressure and weak interfacial interaction between the lubricant and the solid surface are also the main factors that promote lubricant recycling.

14.
Bioprocess Biosyst Eng ; 43(1): 21-31, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31542820

RESUMO

tert-Butyl (3R,5S)-6-chloro-3,5-dihydroxyhexanoate [(3R,5S)-CDHH] is the key chiral intermediate to synthesize the side chain of the lipid-lowering drug rosuvastatin. Carbonyl reductases showed excellent activity for the biosynthesis of (3R,5S)-CDHH. The requirement of cofactor NADH/NADPH leads to high cost for the industrial application of carbonyl reductases. In this study, a self-sufficient biocatalyst based on carbonyl reductase and NADP+ co-immobilization strategy was developed on an amino resin carrier LX-1000HAA (SCR-NADP+@LX-1000HAA). The self-sufficient biocatalyst achieved in situ cofactor regeneration and showed the activity recovery of 77.93% and the specific activity of 70.45 U/g. Asymmetric synthesis of (3R,5S)-CDHH using SCR-NADP+@LX-1000HAA showed high enantioselectivity (> 99% e.e.) and yield (98.54%). Batch reactions were performed for ten cycles without extra addition of NADP+, and the total yield of (3R,5S)-CDHH achieved at 10.56 g/g biocatalyst. The present work demonstrated the potential of the self-sufficient biocatalyst for the asymmetric biosynthesis of rosuvastatin intermediate.


Assuntos
Oxirredutases do Álcool/química , Biocatálise , Candida/enzimologia , Caproatos/síntese química , Enzimas Imobilizadas/química , Proteínas Fúngicas/química , NADP/química , Oxirredutases do Álcool/genética , Candida/genética , Caproatos/química , Enzimas Imobilizadas/genética , Proteínas Fúngicas/genética , Proteínas Recombinantes/química , Proteínas Recombinantes/genética , Rosuvastatina Cálcica/síntese química , Rosuvastatina Cálcica/química
15.
Drug Dev Res ; 80(4): 461-470, 2019 06.
Artigo em Inglês | MEDLINE | ID: mdl-30698296

RESUMO

Isoliquiritigenin (ISL), a natural flavonoid isolated from plant licorice, has various pharmacological properties, including anticancer, anti-inflammatory, and antiviral effects. However, the underlying mechanisms and signaling pathways of ISL in human hepatocellular carcinoma (HCC) cells remain unknown. In this study, we evaluated the effects of ISL on the apoptosis of human HCC cells with a focus on reactive oxygen species (ROS) production. Our results showed that ISL exhibited cytotoxic effects on two human liver cancer cells in a dose-dependent manner. ISL significantly induced mitochondrial-related apoptosis and cell cycle arrest at the G2/M phase, which was accompanied by ROS accumulation in HepG2 cells. However, pretreatment with an ROS scavenger, N-acetyl-l-cysteine (NAC), inhibited ISL-induced apoptosis. In addition, ISL increased the phosphorylation levels of c-Jun N-terminal kinase (JNK), p38 kinase and inhibitor of NF-κB (IκB), and decreased the phosphorylation levels of extracellular signal-regulated kinase (ERK), signal transducer and activator of transcription 3 (STAT3), nuclear factor-kappa B (NF-κB), these effects were blocked by NAC and mitogen-activated protein kinase (MAPK) inhibitors. Taken together, the findings of this study indicate that ISL induced HepG2 cell apoptosis via ROS-mediated MAPK, STAT3, and NF-κB signaling pathways. Therefore, ISL may be a potential treatment for human HCC, as well as other cancer types.


Assuntos
Antineoplásicos Fitogênicos/farmacologia , Apoptose/efeitos dos fármacos , Pontos de Checagem do Ciclo Celular/efeitos dos fármacos , Chalconas/farmacologia , Sistema de Sinalização das MAP Quinases/efeitos dos fármacos , Espécies Reativas de Oxigênio/metabolismo , Técnicas de Cultura de Células , Sobrevivência Celular/efeitos dos fármacos , Células Hep G2 , Humanos , NF-kappa B/metabolismo , Fator de Transcrição STAT3/metabolismo
16.
Phys Chem Chem Phys ; 19(43): 29053-29056, 2017 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-29083014

RESUMO

The hydrogen evolution reaction (HER) using recyclable mediator is being actively pursued as a route for solar energy conversion. Herein, we introduce a catalyst mediator (MoS2) that enables proton-coupled electron transfer (PCET) process on the recyclable TiO2 (H+-TiO2/e-) to a separate, catalytic hydrogen production step without requiring post-light energy input. This approach supplies a new insight to hydrogen evolution with the recyclable proton-electron pairs, stored at the semiconductor after the light irradiation. It was found that 80% of the electrons stored on TiO2 could be devoted to the reduction of H+ into H2 on MoS2 nanosheets in the dark. The electron transfer to MoS2 occurs at a rate of 455 µmol h-1 g-1 and 947 µmol h-1 g-1 in the dark and excited state, respectively.

17.
J Environ Sci (China) ; 60: 78-83, 2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-29031449

RESUMO

Surface junctions between BiOBr and BiVO4 were synthesized. The BiOBr/BiVO4 with 1wt.% of BiOBr exhibited the highest photocatalytic activity in the degradation of RhB under visible-light irradiation. It was found that the highly efficient adsorption of RhB molecules via the electrostatic attraction between Br- and cationic N(Et)2 group played a key role for the high photocatalytic activities of BiOBr/BiVO4. This efficient adsorption promoted the N-deethylation of RhB and thus accelerated the photocatalytic degradation of RhB. Moreover, the metal-to-metal charge transfer (MMCT) mechanism was proposed, which revealed the concrete path paved with Bi-O-Bi chains for the carrier migration in BiOBr/BiVO4. The interaction between photoexcited RhB* and the Bi3+ in BiVO4 provided the driving force for the migration of photo-generated carriers along the Bi-O-Bi chains. This work has not only demonstrated the important role of efficient adsorption in the photocatalytic degradation of organic contaminants, but also developed a facile strategy to improve the efficiency of photocatalysts.


Assuntos
Bismuto/química , Técnicas de Química Sintética/métodos , Modelos Químicos , Processos Fotoquímicos , Vanadatos/química , Adsorção , Luz , Poluentes Químicos da Água
18.
Opt Express ; 24(24): 27870-27881, 2016 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-27906355

RESUMO

Plasmon-based fluorescence modulation has led to important advances in various fields and has paved the way toward promising scientific research aimed at enabling new applications. However, the modulation of fluorescence properties based on both localized surface plasmon (LSP) and cavity modes of propagating surface plasmon polaritons (SPPs) are rarely reported. Here, we raster scanned a hybrid nanowire (HNW) with quantum dots (QDs) adsorbed onto a Ag nanowire (NW) and obtained two-photon fluorescence (TPF) maps of the intensity and decay rate. The spatial distributions of the intensity and decay rate strongly depend on the Fabry-Pérot (FP) cavity modes of the SPPs, the LSP mode launched by the incident laser and the excitation energy of the QDs. A double exponential decay process was observed, which is attributed to different decay channels through the LSP and cavity modes. The experimental results are explained using numerical simulations. This work shows that many physical parameters, such as the polarization of the incident beam and the geometry of the Ag NW, can modulate the fluorescence properties of the QDs, which has potential applications in many important fields.

19.
Chemistry ; 22(39): 13819-13822, 2016 Sep 19.
Artigo em Inglês | MEDLINE | ID: mdl-27442044

RESUMO

Ammonia synthesis under mild conditions is of supreme interest. Photocatalytic nitrogen fixation with water at room temperature and atmospheric pressure is an intriguing strategy. However, the efficiency of this method has been far from satisfied for industrialization, mainly due to the sluggish cleavage of the N≡N bond. Herein, we report a carbon-tungstic-acid (WO3 ⋅H2 O) hybrid for the co-optimization of N2 activation as well as subsequent photoinduced protonation. Efficient ammonia evolution reached 205 µmol g-1 h-1 over this hybrid under simulated sunlight. Nitrogen temperature-programmed desorption revealed the decisive role of carbon in N2 adsorption. Photoactive WO3 ⋅H2 O guaranteed the supply of electrons and protons for subsequent protonation. The universality of carbon modification for enhancing the N2 reduction was further verified over various photocatalysts, shedding light on future materials design for ideal solar energy utilization.

20.
Phys Chem Chem Phys ; 18(27): 18180-6, 2016 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-27333408

RESUMO

Different tunnel structured manganese oxides (1*1, 2*2, and 3*3) have been synthesized via a facile hydrothermal strategy. The three catalysts exhibit high photothermal performance, resulting in a considerable increase of temperature above the light-off temperature for VOC oxidation. On this point, aerobic oxidation reactions of propane and propylene under simulated sunlight and infrared light irradiation were selected as probe reactions to explore their light driven thermocatalytic activity. Furthermore, the light-off curves of the manganese oxides for propane and propylene were carefully investigated, which clearly explained the possibility of combining both the efficient photothermal effect and excellent thermocatalytic activity of the manganese oxides. Results show that the catalytic effects follow the order of 1*1 < 3*3 < 2*2. 2*2 exhibited the best catalytic properties due to better low-temperature reducibility, suitable tunnel structure and the presence of more Mn(4+). This work suggests new applications for traditional catalysts with intense photoabsorption and provides insights into the overall utilization of solar energy.

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