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1.
Adv Mater ; 36(18): e2311535, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38278520

RESUMO

Hydrogen peroxide (H2O2) is a crucial oxidant in advanced oxidation processes. In situ, photosynthesis of it in natural water holds the promise of practical application for water remediation. However, current photosynthesis of H2O2 systems primarily relies on oxygen reduction, leading to limited performance in natural water with low dissolved oxygen or anaerobic conditions found in polluted water. Herein, a novel photocatalyst based on conjugated polymers with alternating electron donor-acceptor structures and electron-withdrawing side chains on electron donors is introduced. Specifically, carbazole functions as the electron donor, triazine serves as the electron acceptor, and cyano acts as the electron-withdrawing side chain. Notably, the photocatalyst exhibits a remarkable solar-to-chemical conversion of 0.64%, the highest reported in natural water. Furthermore, even in anaerobic conditions, it achieves an impressive H2O2 photosynthetic efficiency of 1365 µmol g-1 h-1, surpassing all the reported photosynthetic systems of H2O2. This remarkable improvement is attributed to the effective relocation of the water oxidation active site from a high-energy carbazole to a low-energy acetylene site mediated by the side chains, resulting in enhanced O2 or H2O2 generation from water. This breakthrough offers a new avenue for efficient water remediation using advanced oxidation technologies in oxygen-limited environments, holding significant implications for environmental restoration.

2.
Talanta ; 271: 125655, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38237278

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) are high-profile organic pollutants to be poisonous, carcinogenic, and mutagenic, and widely distributed at trace levels in the environment. In order to effectively enrich PAHs, two stable covalent organic frameworks (COFs, TAPT-OMe-PDA and TPB-DMTP) were prepared by combining 2,4,6-tri(4-aminophenyl)-1,3,5-triazine (TAPT) and 1,3,5-tri(4-aminophenyl) benzene (TAPB) with 2,5-dimethoxy-phenyl-1,4-diformaldehyde (OMe-PDA), respectively. Even though the surface area of TAPT-OMe-PDA was much lower than that of TPB-DMTP, it still demonstrated much better extraction efficiencies towards PAHs as the solid phase microextraction (SPME) coating. Therefore, the TAPT-OMe-PDA coated fiber was coupled with gas chromatography-mass spectrometry (GC-MS) to establish a practical and sensitive method, after the extraction parameters (extraction time, extraction temperature, desorption temperature, desorption time, salt concentration and pH) were optimized. This developed analytical method showed wide linear ranges, low limits of detection, good repeatability and reproducibility. Finally, five PAHs in three water samples were detected and quantified precisely (2.72-38.7 ng·L-1) with satisfactory recoveries (88.3%-118%).

3.
Anal Chim Acta ; 1277: 341652, 2023 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-37604609

RESUMO

Enrichment and detection of trace pollutants in the real matrix are essential for evaluating water quality. In this study, benefiting from the good affinities of 1,3,6,8-tetra(4-carboxylphenyl)pyrene) (H4TBAPy) with itself and melamine (MA) respectively, the composite hydrogen-bonded organic frameworks (HOFs, MA/PFC-1), PFC-1 self-assembled by 1,3,6,8-tetra(4-carboxylphenyl)pyrene), were successfully constructed by the mild strategy of solvent evaporation at room temperature. Through a series of characterizations, such as Fourier transform infrared spectra, X-ray diffraction, thermal gravimetric analyses, and N2 adsorption-desorption, etc., the MA/PFC-1 was confirmed to be a stable and excellent material. In addition, it possessed high surface area, hierarchical micropores, strong hydrogen bonds, and rich function groups containing N and O heteroatoms, since the newly introduced MA could be another hydrogen bonding motif, as well as increased the polarity of reaction solvent. These advantages make MA/PFC-1 be an ideal coating material for solid phase microextraction (SPME). Satisfactory enrichment factors for nitroaromatic compounds (NACs) were got by the MA/PFC-1 fiber under the optimized conditions obtained by the control variables (extraction time of 60 min, extraction temperature of 80 °C, desorption time of 6 min, desorption temperature of 260 °C, pH value of 7, and stirring speed of 250 rpm). MA/PFC-1 was further used to develop an analytical method for NACs based on head-space SPME coupled with gas chromatography‒mass spectrometry (GC‒MS). The developed method with low limits of detection (4.30-20.83 ng L-1) and good reproducibility (relative standard deviations <8.6%). The excellent performance allowed the successful application of the developed method in the determinations of trace NACs in real water samples with recoveries of 80.1%-119%. This study proposed a mild approach to synthesize composite HOFs via doping MA and developed an environmentally friendly method for the precise determinations of NACs in the environment.

4.
Chem Commun (Camb) ; 59(39): 5910-5913, 2023 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-37170996

RESUMO

A light-fueled dissipative aggregation-induced emission (LDAIE) system is successfully fabricated based on reversible electrostatic interactions between cationic AIE luminogens (AIEgens) and anionic spiropyran (ASP) transformed from sulfonato-merocyanine photoacid (SMEH) upon 420 nm light irradiation. The novel LDAIE system can exhibit reversible and spontaneous AIE fluorescence on/off, showing potential in time-dependent information encryption with self-erasing ability. This work opens new opportunities to fabricate a unique fluorescent anti-counterfeiting platform with high-level security.

5.
Mater Horiz ; 10(7): 2496-2505, 2023 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-37060150

RESUMO

The traditional stored information is statically shown on single 2D planes, which leads to low information storage capacity and secondary information leakage without the proper handling of decrypted information. Developing a 3D multistage information encryption platform with self-erasure function is highly desirable. Here, a novel bilayer hydrogel with synergistic deformation and fluorescence color (SDFC) change is designed for 3D multistage information encryption. The bilayer hydrogel consisting of a shape-deformable hydrogel layer and a fluorescence hydrogel layer with aggregation-induced emission (AIE) properties can exhibit pH-responsive SDFC change. Fluorescence information can be ionoprinted on the fluorescent hydrogel layer based on electrostatic interactions and dynamic covalent bonds. The 2D bilayer hydrogel encoded with information can synergistically produce predesigned 3D shape configuration and enhanced background fluorescence to wrap information, which is only readable after sequential shape recovery with the disappearance of background fluorescence. Furthermore, multistage information can be further obtained by stepwise decryption due to information with differential fluorescence fading rates. The displayed information is automatically self-erased in the end, avoiding the information secondary leakage. This study paves an avenue for broadening conventional 2D single-level information encryption platforms to 3D multistage counterparts with self-erasure and multi-decryption capabilities based on SDFC change of the bilayer hydrogel.

6.
Food Chem ; 415: 135790, 2023 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-36868067

RESUMO

Persistent organic pollutants (POPs) are widely distributed in the environment and are toxic, even at low concentrations. In this study, we first used hydrogen-bonded organic framework (HOF) to enrich POPs, based on solid phase microextraction (SPME). The HOF called PFC-1 (self-assembled by 1,3,6,8-tetra(4-carboxylphenyl)pyrene) has an ultra-high specific surface area, excellent thermochemical stability, and abundant functional groups, making it potential to be an excellent coating in SPME. And the as-prepared PFC-1 fiber have demonstrated outstanding enrichment abilities for nitroaromatic compounds (NACs) and POPs. Furthermore, the PFC-1 fiber was coupled with gas chromatography-mass spectrometry (GC-MS) to develop an ultrasensitive and practical analytical method with wide linearity (0.2-200 ng·L-1), low detection limits for organochlorine pesticides (OCPs) (0.070-0.082 ng·L-1) and polychlorinated biphenyls (PCBs) (0.030-0.084 ng·L-1), good repeatability (6.7-9.9%), and satisfactory reproducibility (4.1-8.2%). Trace concentrations of OCPs and PCBs in drinking water, tea beverage, and tea were also determined precisely with the proposed analytical method.


Assuntos
Poluentes Ambientais , Hidrocarbonetos Clorados , Praguicidas , Bifenilos Policlorados , Poluentes Químicos da Água , Microextração em Fase Sólida/métodos , Bifenilos Policlorados/análise , Poluentes Orgânicos Persistentes , Reprodutibilidade dos Testes , Hidrocarbonetos Clorados/análise , Praguicidas/análise , Poluentes Ambientais/análise , Bebidas/análise , Chá , Poluentes Químicos da Água/análise
7.
J Cardiovasc Med (Hagerstown) ; 24(4): 244-252, 2023 04 01.
Artigo em Inglês | MEDLINE | ID: mdl-36938808

RESUMO

BACKGROUND AND AIMS: High epicardial adipose tissue (EAT) attenuation is a key characteristic of adipose tissue dysfunction and associated with coronary artery disease (CAD). As little is known about the modulation of EAT attenuation by metabolic disorders, we investigated the association between EAT attenuation and CAD risk factors, CAD presence and CAD severity in type 2 diabetes mellitus (T2DM) patients. METHODS: We included 276 inpatients with T2DM and 305 control patients with normal glucose metabolism (NGM), who underwent cardiac computed tomography angiography (CCTA) and coronary artery calcium (CAC) scoring. EAT attenuation and volume were evaluated by contrast-enhanced CCTA image analysis. Furthermore, segment stenosis scores (SSSs) of the left main coronary artery (LMCA), left anterior descending artery (LAD), left circumflex artery (LCX), right coronary artery (RCA), diagonal/intermediate branch (D/I) and obtuse marginal branch (OM) were calculated to assess CAD severity. RESULTS: T2DM patients showed higher significant CAC scores, coronary plaque prevalence, total SSSs and LMCA-SSSs, LAD-SSSs, LCX-SSSs, RCA-SSSs and D/I-SSSs compared with NGM controls. In contrast to NGM controls, EAT volume was significantly increased in T2DM patients, whereas EAT attenuation was similar. In T2DM patients, EAT attenuation was associated with discrete CAD risk factors, the presence of coronary and triple-vessel plaques, as well as LAD-SSSs, LCX-SSSs, RCA-SSSs and total SSSs. In addition, EAT attenuation was only associated with the total SSS of calcified plaques, but not with noncalcified plaques. CONCLUSION: In T2DM patients, high EAT attenuation is associated with the presence and severity of CAD in general and with coronary stenosis caused by calcified plaques in particular.


Assuntos
Doença da Artéria Coronariana , Estenose Coronária , Diabetes Mellitus Tipo 2 , Placa Aterosclerótica , Humanos , Doença da Artéria Coronariana/etiologia , Doença da Artéria Coronariana/complicações , Diabetes Mellitus Tipo 2/complicações , Diabetes Mellitus Tipo 2/diagnóstico , Angiografia Coronária/métodos , Pericárdio/diagnóstico por imagem , Estenose Coronária/diagnóstico por imagem , Estenose Coronária/complicações , Vasos Coronários/diagnóstico por imagem , Constrição Patológica , Tecido Adiposo/diagnóstico por imagem
8.
Anal Chim Acta ; 1220: 340040, 2022 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-35868701

RESUMO

Aromatic esters have been widely used in daily life with non-ignorable dangers, such as plasticizer, flavor, and preservative. Their wide applications and corresponding hazards caused by overuse have promoted the rapid development of sensitively analytical method for effective regulation. However, the variety makes it challenging for broad-spectrum and simultaneous extraction of diverse aromatic esters from the highly complex cosmetic samples. To our delight, a covalent organic framework, named DaTp (1, 3, 5-triformylphloroglucinol-2, 6-diaminoanthracene), possessing high specific surface, excellently thermochemical stability, and abundant electron-rich heteroatoms, has been synthesized and fabricated as a competitive solid phase microextraction coating for extracting the trace analytes with diverse polarity, through the hydrophobic interaction, π-π conjugation and hydrogen bond. Herein, this self-made SPME fiber has been further coupled with gas chromatography-tandem mass spectrometry (GC-MS) to determine the multi-polar aromatic esters in cosmetics packaged with plastic. This developed analytical method showed wide liner ranges, low limits of detection, good repeatability and reproducibility. Finally, the aromatic esters in four cosmetic samples were quantified precisely with satisfactory recoveries (80.7%-118%).


Assuntos
Cosméticos , Estruturas Metalorgânicas , Cosméticos/análise , Ésteres/análise , Cromatografia Gasosa-Espectrometria de Massas/métodos , Limite de Detecção , Estruturas Metalorgânicas/química , Reprodutibilidade dos Testes , Microextração em Fase Sólida/métodos
9.
ACS Macro Lett ; 11(3): 347-353, 2022 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-35575373

RESUMO

Development of soft actuators with complex practical functions is significant for imitating the behaviors of living organisms. However, it is still a challenge to fabricate artificial soft actuators with jellyfish-like synergistic deformation and fluorescence color change (SDFC) and autonomous dynamic behavior, but such a system could obviously endow the classic soft actuators with more functions. Herein, we proposed to utilize tetra(4-pyridylphenyl)ethylene (TPE-4N) luminogen with pH-responsive aggregation-induced emission (AIE) to fabricate the AIE active hydrogel, which could be further employed to obtain an anisotropic bilayer soft actuator based on strong interfacial adhesion with acrylic acid (AA) gels. Furthermore, artificial flower-shape actuators showing SDFC behaviors were demonstrated. On the basis of these findings, jellyfish-inspired autonomous gel actuators driven by a pH oscillator have been fabricated, in which periodical SDFC behaviors completely regulated by the system itself without repetitive on/off switches of external stimuli were well synchronized with the pH oscillator. The described combination of nonlinear chemistry and responsive hydrogels actuator opens pathways toward out-of-equilibrium SDFC devices with autonomous behavior useful for biomimetic fields.


Assuntos
Biomimética , Hidrogéis , Anisotropia , Fluorescência , Hidrogéis/química , Concentração de Íons de Hidrogênio
10.
J Chromatogr A ; 1669: 462959, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35303573

RESUMO

Perfluorinated alkyl substances (PFASs) were ubiquitously in the surface and groundwater. It is crucial and urgent to develop a rapid and ultrasensitive analysis method for the quantification of trace-level PFASs. Herein, a highly hydrophobic sorbent by capping phenylsilane groups on the surfaces of NH2-UiO-66(Zr) nanocrystals was used for efficient solid-phase microextraction (SPME) of PFASs in water samples. It was found that the superficially capped nanocrystals (NH2-UiO-66(Zr)-hp) exhibited both faster extraction kinetics and higher enrichment capacity than the non-capped nanocrystals. The extraction of eleven kinds of PFASs by NH2-UiO-66(Zr)-hp fiber reached equilibrium in 20 min. The enrichment factors of the NH2-UiO-66(Zr)-hp fiber ranged from 6.5 to 48, with a preference for long-chain PFASs over short-chain PFASs. It was proposed that superficial capping eliminated competitive moisture adsorption on the surfaces of the non-capped nanocrystals, thus facilitating the adsorption of PFASs through hydrophobic interaction. By using this new sorbent, the limits of detection of the SPME method as low as 0.035 to 0.616 ng·L-1 were achieved for the target PFASs. The recoveries of PFASs in the environmental water samples were 80.9%-120%. This study presents a new strategy for developing an efficient sorbent for PFASs by surface hydrophobic modification.


Assuntos
Estruturas Metalorgânicas , Ácidos Ftálicos , Poluentes Químicos da Água , Estruturas Metalorgânicas/química , Microextração em Fase Sólida/métodos , Poluentes Químicos da Água/análise
11.
Taiwan J Obstet Gynecol ; 60(6): 1078-1083, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-34794741

RESUMO

OBJECTIVE: High-intensity focused ultrasound (HIFU) therapy is a noninvasive alternative to conventional abdominal surgery in obstetrics and gynecology. The aim of this study is to evaluate the reduction of pain intensity with bowel manipulation before ultrasound-guided HIFU treatment in women with posterior wall uterine fibroids and/or adenomyosis. MATERIALS AND METHODS: This is a multicenter retrospective observational study. Data from all patients who underwent HIFU therapy at three HIFU clinics (Sichuan Maternal and Child Health Hospital, Xiangya Hospital of Central South University, and Kuo General Hospital) between January 2019 and December 2019 were analyzed. We compared pain intensity with and without bowel manipulation during the HIFU treatment and evaluated tolerability without intravenous sedation. The presence of discomfort or pain during the HIFU procedure was evaluated using the visual analog scale (VAS). RESULTS: A total of 86 women were included in this study. All women underwent HIFU therapy with the PRO-2008 system in the supine position for posterior wall uterine fibroids and/or adenomyosis. Thirty-seven women received pretreatment anal catheterization with a condom and 49 women were not subjected to bowel manipulation. All patients received pretreatment condom-catheter device were well tolerated during the procedure of bowel manipulation. During the HIFU procedure, the women who had received bowel manipulation experienced lower pain intensity, especially less sacrococcygeal pain (VAS score 1.56 ± 1.46 vs 2.89 ± 1.61), target region pain (1.54 ± 1.30 vs 2.53 ± 1.29), and radiating pain (0.13 ± 0.34 vs 0.41 ± 0.54), compared with the women without bowel manipulation. CONCLUSION: Bowel manipulation with anal catheterization before HIFU therapy for posterior wall uterine masses can be safely performed and is effective as a low risk intervention to aid in reducing potential HIFU complications related to nerve involvement.


Assuntos
Adenomiose/terapia , Tratamento por Ondas de Choque Extracorpóreas , Ablação por Ultrassom Focalizado de Alta Intensidade/efeitos adversos , Leiomioma/terapia , Ultrassonografia de Intervenção/métodos , Neoplasias Uterinas/terapia , Adenomiose/patologia , Criança , Feminino , Humanos , Leiomioma/patologia , Gravidez , Estudos Retrospectivos , Resultado do Tratamento , Ultrassonografia Doppler em Cores , Neoplasias Uterinas/patologia , Escala Visual Analógica
12.
Chem Commun (Camb) ; 56(96): 15169-15172, 2020 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-33215183

RESUMO

A dissipative aggregation-induced emission (DAIE) system is successfully fabricated by coupling a stimuli-responsive AIE luminogens (AIEgens) with a pH oscillator. The novel DAIE system exhibits reversible, autonomous and sustainable AIE behaviour. Moreover, the DAIE behaviour can be regulated with the system temperature. The novel strategy will boost the development of bioinspired intelligent systems for real-world applications.

13.
Talanta ; 219: 121175, 2020 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-32887097

RESUMO

Headspace solid-phase microextraction (HS-SPME) of low volatile analytes from complex aqueous samples can be substantially facilitated by elevating the temperature of the samples. However, many SPME coatings prepared from novel sorptive materials may suffer from low stabilities in hot water steam. Herein, a superhydrophobic metal-organic framework (MOF) derived from decorating the metal-oxo nodes of the amino-functionalized UiO-66(Zr) with phenylsilane was prepared and successfully developed into a novel SPME fiber coating. The highest extraction efficiencies towards the semi-volatile ultraviolet (UV) filters were achieved when the aqueous samples were heated up to 100 °C. It was notable that the lab-made coating exhibited extraordinary stability towards hot water steam, probably because the hydrophobic groups capped on the MOF prevented water molecules from entering and deconstructing its lattice. Even after being treated with water steam under 100 °C for 21 h, the extraction performance of the coating remained unchanged, and the crystal structure of the MOF maintained. Furthermore, a negligible matrix effect was observed even in the samples containing humic acid. Under the optimal extraction and thermal desorption conditions, a method for determining UV filters in aqueous samples was established, which possessed low detection limits (0.6-2.1 ng L-1), wide linear ranges (10-50000 ng L-1), good inter-fiber reproducibility (2.3-6.0%, n = 6), and satisfying intra-fiber repeatability (1.8-5.8%, n = 3). The method was successfully applied in quantifying UV filters in environmental water samples. In addition, the lab-made NH2-UiO-66(Zr)-shp-coated fiber was also suitable for the analysis of polycyclic aromatic hydrocarbons (PAHs). This study provided an effective strategy for preparing MOF coatings that can maintain their crystalline structures and high extraction performances in high-temperature steam.

14.
Talanta ; 217: 121088, 2020 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-32498859

RESUMO

The development of carbon sorbents with high specific surface areas remains a hot research field in analytical community. In the current study, a novel three-dimensional hierarchical flower-like magnesium glycollate sphere was synthesized. Then, the obtained magnesium glycollate sphere was carbonized to obtain magnesia-carbon composite material with enhanced performance. The flower-like carbon material exhibited good adsorption capacity towards polycyclic aromatic hydrocarbons due to the large surface area, the strong π-π interaction force and hydrophobic forces. The flower-like MgO&C material was used as a solid-phase microextraction fiber coating for the analysis of polycyclic aromatic hydrocarbons in real river water samples. Good linearity (5-1000 ng L-1), satisfactory relatively recoveries (86.2-113.5%) and low limits of detections (0.01-0.20 ng L-1) were obtained under the optimized conditions.

15.
Soft Matter ; 16(12): 2928-2932, 2020 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-32154538

RESUMO

A diversified and biocompatible rhythmic deformation (RD) system is successfully fabricated by coupling a heterogeneous hydrogel with a pH oscillator. By tailoring the geometry of the building blocks, a heterogeneous hydrogel actuator with diversity could be easily constructed through interfacial adhesion. Moreover, the RD behaviour can be regulated by the system temperature and actuator shape.

16.
Atherosclerosis ; 284: 230-236, 2019 05.
Artigo em Inglês | MEDLINE | ID: mdl-30777338

RESUMO

BACKGROUND AND AIMS: Density may indicate some tissue characteristics and help reveal the role of epicardial adipose tissue (EAT) in coronary artery disease (CAD). Therefore, we assessed the association of EAT density with the coronary artery plaque burden in patients presenting with chest pain. METHODS: This retrospective cohort study comprised 614 patients (mean age 61 ±â€¯9 years, 61% males) with a high cardiovascular disease risk, who underwent cardiac computed tomography angiography. Density was reflected as attenuation. RESULTS: EAT attenuation was significantly associated with EAT volume with a negative Pearson's correlation coefficient and gradually increased across coronary artery calcium (CAC) scores of 0, 1-100, 101-400 and > 400. EAT attenuation was tightly associated with CAD risk factors, including age, sex, BMI, total cholesterol, neutrophil to lymphocyte ratios and CAC score. The association between EAT attenuation and CAC score was strengthened after adjusting for multivariable indices (OR 1.21, 95% CI 1.05-1.40, p = 0.01) and further adjusting for EAT volume (OR 1.26 95% CI 1.06-1.51, p<0.01). However, EAT attenuation was associated only with CAD presence (OR 1.32, 95% CI 1.02-1.69, p<0.05), CAC presence (OR 1.28, 95% CI 1.02-1.60, p<0.05), segment involvement score (OR 1.19, 95% CI 1.01-1.40, p<0.05) and segment stenosis score (OR 1.19, 95% CI 1.01-1.40, p<0.05) in the EAT volume- and multivariable-adjusted model. Additionally, EAT attenuation was not associated with significant coronary artery lesions and triple-vessel plaques. CONCLUSIONS: Higher EAT attenuation is associated with a higher risk of CAD.


Assuntos
Tecido Adiposo/patologia , Angiografia por Tomografia Computadorizada , Doença da Artéria Coronariana/diagnóstico por imagem , Doença da Artéria Coronariana/patologia , Pericárdio/patologia , Idoso , Estudos de Coortes , Doença da Artéria Coronariana/epidemiologia , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Tamanho do Órgão , Estudos Retrospectivos , Medição de Risco
17.
J Mater Chem B ; 7(12): 1996-2000, 2019 03 28.
Artigo em Inglês | MEDLINE | ID: mdl-32254803

RESUMO

A novel and facile dynamic interfacial adhesion (DIA) strategy has been successfully applied in the reversible fabrication of complex 3D hydrogel constructs based on dynamic covalent bonds (DCBs). By tailoring the geometry of gel building blocks (GBBs) and incorporating stimuli-responsive units, various shapes could be easily achieved.


Assuntos
Hidrogéis/química , Adesividade
18.
Talanta ; 178: 629-635, 2018 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-29136873

RESUMO

The introduction of functional groups into metal organic frameworks has great potential for enhancement in adsorption performance of nitrosamines using solid phase microextraction (SPME). However, pre-functionalization and post-modification generally suffer from the same limitation that the additional functional groups occupy the free volume and thereby decreasing pore volume and special surface area. Herein, we use a modulator-induced defect-formation strategy to prepare the 8-aminocaprylic acid doped UIO-66 (Am-UIO-66) with high adsorption capacity of nitrosamines. Then, the as-synthesized UIO-66 and Am-UIO-66 were fabricated as SPME fibers exhibiting good adsorption capacity towards nitrosoamines. The reason was that the 8-aminocaprylic acid creates structural defects and additional pore spaces of Am-UIO-66, thus increases the specific surface area as well as pore volume. Finally, the Am-UIO-66-coated SPME fiber was successfully applied to the determination of nitrosamines migration from latex gloves and achieved good linearity (20-2000ngL-1), satisfactory recoveries (85.2-112.8%) and rather low LODs (2.61-6.12ngL-1), by coupling with gas chromatography-mass spectrometry (GC-MS).

19.
Anal Chim Acta ; 989: 21-28, 2017 Oct 09.
Artigo em Inglês | MEDLINE | ID: mdl-28915939

RESUMO

Adsorption capacity is the major sensitivity-limited factor in solid-phase microextraction. Due to its light-weight properties, large specific surface area and high porosity, especially tunable pore structures, the utilization of porous organic polymers as solid-phase microextraction adsorbents has attracting researchers' attentions. However, these works mostly concentrated on the utilization of specific porous organic polymers for preparing high-performance solid-phase microextraction coatings. The relationship between pore structures and adsorption performance of the porous organic polymers still remain unclear. Herein, three porous organic polymers with similar properties but different pore distributions were prepared by condensation polymerization reaction of phloroglucinol and terephthalaldehyde, which were fabricated as solid-phase microextraction coatings subsequently. The adsorption capacity of the porous organic polymers-coated fibers were evaluated by using benzene and its derivatives (i.e.,benzene, toluene, ethylbenzene and m-xylene) and polycyclic aromatic hydrocarbons as the target analytes. The results showed that the different adsorption performance of these porous organic polymers was mainly caused by their different pore volumes instead of their surface areas or pore sizes. Finally, the proposed method by using the mesoporous organic polymer coating was successfully applied to the determination of benzene and its derivatives in environmental water samples. As for analytical performance, high pre-concentration factors (74-2984), satisfactory relative recoveries (94.5 ± 18.5-116.9 ± 12.5%), intraday precision (2.44-5.34%), inter-day precision (4.62-7.02%), low limit of detections (LODs, 0.10-0.29 ng L-1) and limit of quantifications (LOQs, 0.33-0.96 ng L-1) were achieved under the optimal conditions. This study provides an important idea in the rational design of porous organic polymers for solid-phase microextraction or other adsorption applications.

20.
Environ Sci Technol ; 51(9): 5137-5145, 2017 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-28379014

RESUMO

Although nanotechnology has offered effective and efficient solutions for environmental remediation, the full utilization of sustainable energy and the avoidance of secondary pollution are still challenges. Herein, we report a two-step modification strategy for TiO2 nanoparticles by first forming a thin, surface-adherent polydopamine (PDA) shell onto the nanoparticles and then assembling core-shell nanoparticles as a photodegradation coating. The composite coating modified from TiO2 could not only realize the highly efficient utilization of photons from the visible region but also avoid the secondary pollution of nanoparticles during application. Additionally, improvements in the adsorption ability after modification greatly facilitated the photocatalytic process of the modified materials. A preliminary in vivo study on Daphnia magna and a wastewater treatment experiment suggest that treatment with the composite coating can effectively eliminate fluorene and significantly reduce its lethality. We believe the two-step modification scheme can open new avenues for the facile modification of nanomaterials for designed purposes, especially in the field of environmental remediation.


Assuntos
Poluentes Ambientais , Titânio/efeitos da radiação , Luz , Nanoestruturas , Fotólise
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