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1.
Clin Oral Investig ; 28(6): 306, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38727727

ABSTRACT

OBJECTIVES: Recent evidence suggested a link between periodontitis (PD) and dental caries, but the trends and nature of this association remained unclear. The overall aim of this study was to critically assess the correlation of two disorders. METHODS: A comprehensive search was conducted within the PUBMED and EMBASE databases including grey literatures up to July 5th, 2023. The Newcastle-Ottawa scale was used to qualitatively evaluate the risk of bias. RESULTS: Overall, 18 studies were included. In terms of caries risk in PD patients, the prevalence of caries was increased by PD (OR = 1.57, 95%CI:1.20-2.07), both in crown (OR = 1.03, 95%CI:1.01-1.05) and root caries (OR = 2.10, 95%CI:1.03-4.29). Odds of caries were also raised by PD severity (OR moderate = 1.38, 95%CI:1.15-1.66; OR severe = 2.14, 95%CI:1.74-2.64). Besides, patients with PD exhibited a higher mean number of decayed, missing and filled teeth (DMFT) and decayed and filled root teeth (DFR) [weighted mean difference (WMD)DMFT = 0.87, 95%CI: -0.03-1.76; WMDDFR = 1.13, 95%CI: 0.48-1.78]. Likewise, patients with caries had an elevated risk of PD (OR = 1.79, 95%CI:1.36-2.35). However, Streptococcus mutans, one of the main pathogens of caries, was negatively correlated with several main pathogens of periodontitis. CONCLUSIONS: This study indicated a positive correlation between dental caries and periodontitis clinically, while the two disease-associated pathogens were antagonistic. CLINICAL RELEVANCE: Further research, including clinical cohort studies and mechanisms of pathogens interaction is needed on this link for better prevention and treatment of PD and caries. In addition, innovative prevention strategies need to be developed and incorporated in dental practices to prevent these two highly prevalent oral diseases.


Subject(s)
Dental Caries , Periodontitis , Humans , Dental Caries/epidemiology , Periodontitis/complications , Periodontitis/epidemiology , Periodontitis/microbiology , Prevalence , Risk Factors
2.
Angew Chem Int Ed Engl ; 63(16): e202319732, 2024 Apr 15.
Article in English | MEDLINE | ID: mdl-38367015

ABSTRACT

Bio-catalysis represents a highly efficient and stereoselective method for the synthesis of valuable chiral compounds, however, the poor stability and limited reaction types of free enzymes restrict their wide application in industrial production. In this work, to overcome these problems, a multifunctional photoenzymatic nanoreactor CALB@COF-Ir was developed through the encapsulation of Candida antarctica lipase B (CALB) in a photosensitive covalent organic framework COF-Ir. This bio-nanocluster serves as efficient catalysts in asymmetric dynamic kinetic resolution (DKR) of secondary amines to give a series of chiral amines in high yields (up to 99 %) and enantioselectivities (up to 99 % ee). The well-designed COF-Ir not only acts as safety cover to prevent CALB from deactivation but promotes racemization of secondary amines via photo-induced hydrogen atom transfer (HAT) process. Photoelectric characterization and TDDFT calculation revealed that (ppy)2Ir units in COF-Ir play crucial role in this photocatalytic system which enhance its photo-redox properties through facilitating the separation between photoelectrons (e-) and holes (h+). Furthermore, the heterogeneous photoenzymatic nanoreactor could be recycled for five rounds with slight decline of catalytic reactivity.

3.
Angew Chem Int Ed Engl ; 63(11): e202319909, 2024 Mar 11.
Article in English | MEDLINE | ID: mdl-38243685

ABSTRACT

Benzoxazole-linked covalent organic frameworks (BO-COFs), despite their exceptional chemical stability, are still in their infancy. This is primarily because the current prevalent methods require the use of special ortho-hydroxyl-substituted aromatic amines as monomers. Herein, we report an innovative strategy to access BO-COFs directly from imine-linked COFs (Im-COFs) without pre-embedded OH groups, using a two-step sequential oxidation/cyclization process. The two-step process included the oxidation of Im-COFs into amide-linked COFs, followed by a copper-catalyzed oxidative cyclization. Five representative BO-COFs were synthesized with retained crystallinity and high oxidization efficiency, offering the potential to convert a significant portion of Im-COFs into BO-COFs. The structural advantages of the newly designed BO-COFs were demonstrated through their application to photocatalytic organic transformations.

4.
Chem Commun (Camb) ; 60(13): 1782-1785, 2024 Feb 08.
Article in English | MEDLINE | ID: mdl-38252554

ABSTRACT

Inspired by the bidentate coordination chemistry of metal ions, we incorporated hydroxyl (OH) and methoxy (OMe) groups into the skeleton of imine-linked COFs to improve their protonation ability via intramolecular hydrogen bonds (O-H⋯NC). In comparison with the pristine COFs possessing monodentate nitrogen coordination sites, OH and OMe functionalized COFs with (N,O)-bidentate chelating sites exhibited up to 13.8 times faster photocatalytic hydrogen evolution rates (HERs).

5.
BMC Oral Health ; 23(1): 932, 2023 11 27.
Article in English | MEDLINE | ID: mdl-38012618

ABSTRACT

PURPOSE: To characterize the bacterial community in the primarily infected root canals. METHODS: A total of 13 samples were collected from the primarily infected root canals. 16 S rDNA sequencing was performed to define bacterial community. Taxonomic annotation, bacterial hierarchical structures, community richness and diversity, and inter-subject variability of the bacterial community in the root canal samples were analyzed. Gender, age, and duration of the toothache-specific bacterial community associated with the patient groups were analyzed. RESULTS: A total of 359 Species were annotated and identified in the whole study cohort. The Alpha diversity analysis showed that the species diversity and detection rate of the 13 samples were high, which reflected the authenticity of sequencing results. The Beta diversity analysis was used to compare the degree of difference between different root canal samples. The 13 samples were divided into two groups according to the results, group A was samples I1-I12, and group B was samples I13. The bacterial species of group A samples were analyzed with the clinical characteristics of patients, and it was found that gender, and duration specific differences in bacterial species, and there was no significant difference in species types among different ages of patients. CONCLUSION: There were a wide diversity and inter-subject variability in the bacterial community in the primary infected root canals. While Porphyromonas gingivalis was the most abundant species, Fusobacterium nucleatum was the most variable species in the bacterial community of the root canal. The bacterial community at different taxonomic levels varied from sample to sample, despite consistent disease diagnoses. There was gender, duration-specific differences in the bacterial species in the primary infected root canals.


Subject(s)
Dental Pulp Cavity , Periapical Periodontitis , Humans , Dental Pulp Cavity/microbiology , East Asian People , Fusobacterium nucleatum/genetics , Fusobacterium nucleatum/isolation & purification , Periapical Periodontitis/microbiology , Porphyromonas gingivalis/genetics , Porphyromonas gingivalis/isolation & purification , Root Canal Therapy , DNA, Ribosomal
6.
Angew Chem Int Ed Engl ; 62(51): e202313520, 2023 Dec 18.
Article in English | MEDLINE | ID: mdl-37921489

ABSTRACT

Covalent organic frameworks (COFs) have emerged as efficient heterogeneous photocatalysts for a wide range of relatively simple organic reactions, whereas their application in complex organic transformations, like site-selective functionalization of unactivated C-H bonds, is underexplored, which can be mainly attributed to the lack of highly active organophotocatalytic cores. Herein through bonding oxygen atoms at the N-terminus of quinolines in nonsubstituted quinoline-linked COFs (NQ-COFs), we successfully realized the embedding of active hydrogen atom transfer (HAT) moieties into the skeleton of COFs. This novel designed COF (NQ-COFE5 -O), serving as both an excellent photosensitizer and HAT catalyst, exhibited much higher efficiency in C-H functionalization than the corresponding NQ-COFE5 . Specially, we evaluated the photocatalytic performance of NQ-COFE5 -O on ten different substrates, including quinolines, benzothiazole, and benzoxazole, all of which were transferred to desired products in moderate to high yields (up to 93 %). Furthermore, the as-synthesized NQ-COFE5 -O displayed excellent photostability and could be reused with negligible loss of activity for five catalytic cycles.

7.
Chem Sci ; 14(6): 1543-1550, 2023 Feb 08.
Article in English | MEDLINE | ID: mdl-36794200

ABSTRACT

Irreversible locking of imine linkages into stable linkages represents a promising strategy to improve the robustness and functionality of covalent organic frameworks (COFs). We report, for the first time, a multi-component one-pot reaction (OPR) for imine annulation to construct highly stable nonsubstituted quinoline-bridged COFs (NQ-COFs), and that equilibrium regulation of reversible/irreversible cascade reactions by addition of MgSO4 desiccant is crucial to achieve high conversion efficiency and crystallinity. The higher long-range order and surface area of NQ-COFs synthesized by this OPR than those of the reported two-step post-synthetic modification (PSM) facilitate charge carrier transfer and photogeneration ability of superoxide radicals (O2˙-), which makes these NQ-COFs more efficient photocatalysts for O2˙- mediated synthesis of 2-benzimidazole derivatives. The general applicability of this synthetic strategy is demonstrated by fabricating 12 other crystalline NQ-COFs with a diversity of topologies and functional groups.

8.
ChemSusChem ; 16(5): e202202082, 2023 Mar 08.
Article in English | MEDLINE | ID: mdl-36479983

ABSTRACT

In this work, an efficient visible light promoted aerobic dehydro-coupling of amines, oxidation of thioethers and hydroxylation of arylboronic acids under benign conditions by using pyrene-based donor-acceptor (D-A) conjugated organic molecules was described. Donor-acceptor structure influences their π-conjugation and band gap a lot, and thereby enhances their visible light absorption ability, single electron transfer and oxidative behaviors. Alkynyl units in PS-IV play a crucial role in the catalyst which could serve as electron transferring bridge to strengthen electron delocalization, thus facilitating the single electron transfer from photosensitizer to substrates, and making it an efficient ⋅O2 - generator. While PS-III without alkynyl units tends to produce 1 O2 . Therefore, these molecules can serve as efficient catalysts for different kinds of visible-light-induced aerobic organic reactions. More importantly, the simply structured molecule is insoluble and stable in various solvents, and thus could be recycled as heterogeneous catalyst for many rounds with slight catalytic activity degradation. Besides, large scale (1 mol) reaction of benzylamine coupling proceeded smoothly under the standard conditions.

9.
Sci Bull (Beijing) ; 67(1): 61-70, 2022 01.
Article in English | MEDLINE | ID: mdl-36545961

ABSTRACT

Photocatalytic oxidative organic reactions are important synthetic transformations, and research on reaction selectivity by reactive oxygen species (ROS) is significant. To date, however, there has rarely been any focus on the directed generation of ROSs. Herein, we report the first identification of tunable molecular oxygen activation induced by polymeric conjugation in nonmetallic conjugated microporous polymers (CMP). The conjugation between these can be achieved by the introduction of alkynyl groups. CMP-A with an alkynyl bridge facilitates the intramolecular charge mobility while CMP-D, lacking an alkynyl group enhances the photoexcited carrier build-up on the surface from diffusion. These different processes dominate the directed ROS generation of the superoxide radical (O2-) and singlet oxygen (1O2), respectively. This theory is substantiated by the different performances of these CMPs in the aerobic oxidation of sulfides and the dehydrogenative coupling of amines, and could provide insight into the rational design of CMPs for various heterogeneous organic photosynthesis.


Subject(s)
Oxygen , Photosynthesis , Reactive Oxygen Species , Chemical Phenomena , Diffusion
10.
Angew Chem Int Ed Engl ; 61(41): e202208833, 2022 Oct 10.
Article in English | MEDLINE | ID: mdl-35999182

ABSTRACT

Exploring new routes to lock the dynamic C=N bonds in imine-linked covalent organic frameworks (COFs) is highly desired for enhancing their stability and functionality. Herein, a novel C=N bridge locking strategy via rhodium-catalyzed [4+2] annulation is developed to construct nonsubstituted quinoline-linked COFs (NQ-COFs). The notable feature of this strategy includes high C=N conversion efficiency, oxidant-free, and generality for synthesis of a variety of NQ-COFs with high chemical stability. Particularly, after post-synthetic modification, the crystallinity, topology, and porosity of pristine imine-linked COFs are well retained. When used as photocatalysts, NQ-COFs display better visible light absorption and carriers' separation efficiency due to enhanced in-plane π conjugation ability, as well as more facile generation of superoxide anion radicals than their counterparts, thus leading to efficient synthesis of 2,4,6-tris(aryl)pyridines, benzimidazole, and sulfoxide derivatives.

11.
Food Chem ; 397: 133742, 2022 Dec 15.
Article in English | MEDLINE | ID: mdl-35940091

ABSTRACT

Water loss is a key factor for the postharvest senescence of fruit. It has been reported that natural cuticular wax at high concentrations has better performance than commercial coating in water retention of fruit, which can prevent postharvest water loss without the accumulation of off-flavor. Here, we analyzed the correlation between epicuticular wax and postharvest water loss with 75 citrus varieties from a natural population. The water loss rate of the fruit was little influenced by the wax microstructure (stomata and wax crystal morphology), but strongly affected by epicuticular wax components. Further, C24 and C26 aliphatic aldehydes showed the greatest impact on fruit water loss rate, whose correlation coefficients reached -0.63 and -0.67, respectively. These two substances could significantly reduce the fruit water loss rate, indicating that they are potential natural additives to be used in the coating for citrus fruit water retention.


Subject(s)
Citrus , Aldehydes/analysis , Fruit/chemistry , Water/analysis , Waxes/chemistry
12.
Nat Commun ; 11(1): 1149, 2020 03 02.
Article in English | MEDLINE | ID: mdl-32123173

ABSTRACT

Photoreduction of CO2 to fuels offers a promising strategy for managing the global carbon balance using renewable solar energy. But the decisive process of oriented photogenerated electron delivery presents a considerable challenge. Here, we report the construction of intermolecular cascaded π-conjugation channels for powering CO2 photoreduction by modifying both intramolecular and intermolecular conjugation of conjugated polymers (CPs). This coordination of dual conjugation is firstly proved by theoretical calculations and transient spectroscopies, showcasing alkynyl-removed CPs blocking the delocalization of electrons and in turn delivering the localized electrons through the intermolecular cascaded channels to active sites. Therefore, the optimized CPs (N-CP-D) exhibiting CO evolution activity of 2247 µmol g-1 h-1 and revealing a remarkable enhancement of 138-times compared to unmodified CPs (N-CP-A).

13.
ACS Appl Mater Interfaces ; 12(1): 1867-1876, 2020 Jan 08.
Article in English | MEDLINE | ID: mdl-31840502

ABSTRACT

Construction of the semimetal/semiconductor composite interface is widely used to promote the O2 molecule adsorption and charge transfer for boosting solar-driven molecular oxygen activation (MOA). Herein, a Bi@Bi2MoO6 heterostructure is fabricated via a two-step wet chemical method as a typical photocatalyst to investigate the underlying mechanism of Bi-coordinated facet-dependent MOA under visible-light illumination. Density functional theory and systematical characterization methods reveal the distinct charge transfer and O2 activation processes on the surface of Bi nanoparticle-deposited Bi2MoO6 nanosheets with different facets exposed. By virtue of a particular and efficient [Bi2O2]2+ → Bi → MoO42- interfacial charge-transfer channel, Bi deposited on the (001) facet of Bi2MoO6 can observably intensify MOA, thereby giving birth to more generation of reactive oxygen species and endowing the Bi@Bi2MoO6 with excellent photocatalytic performance in sodium pentachlorophenate (NaPCP) removal. The decomposition pathway of NaPCP is also proposed based on the intermediate determination and mineralization analysis. This work provides deep insights into the mechanism of facet-dependent MOA over a semimetal-semiconductor system and also sheds light on designing effective molecular oxygen-activated interface for environmental remediation.

14.
Chemistry ; 25(13): 3362-3368, 2019 Mar 01.
Article in English | MEDLINE | ID: mdl-30645005

ABSTRACT

Donor-acceptor (D-A) conjugated polymers have proved to be desired candidates to couple with inorganic semiconductors for enhanced photocatalytic activity. Herein, the matched energy levels between polymer BFB and TiO2 make them form BFB-TiO2 composites with moderate photocatalytic H2 evolution rate (HER). To further enhance the interfacial interaction, BFB was modified with a carboxylic acid end group, which reacted with surface OH of TiO2 to form an ester bond. As a result, the functionalized BFBA-TiO2 composites exhibited superior photocatalytic activity. Especially, HER of 4 % BFBA-TiO2 can reach up to 228.2 µmol h-1 under visible light irradiation (λ>420 nm), which is about 2.02 times higher than that of BFB-TiO2 . The enhanced photocatalytic activity originated from the formed ester bond between polymer and TiO2 , and photogenerated electrons injection from lowest unoccupied molecular orbital (LUMO) of the exited polymer to conduction band of TiO2 were accelerated. Therefore, based on an intermolecular interaction mechanism, more suitable D-A conjugated polymers with anchoring groups could be designed to couple with other semiconductors for enhancing photocatalytic activity.

15.
Macromol Rapid Commun ; 40(6): e1800494, 2019 Mar.
Article in English | MEDLINE | ID: mdl-30556197

ABSTRACT

To take advantage of high surface area of network conjugated microporous polymers, four linear or network conjugated polymers L-PDBT, L-PDBT-O, N-PDBT, and N-PDBT-O are designed in terms of water-compatibility, and it turned out that microporous network N-PDBT-O exhibited the highest hydrogen evolution rate (HER) at 366 µmol h-1 under visible light irradiation (λ > 420 nm, one of best reported pristine polymer-based photocatalysts), which is three times higher than the corresponding linear L-PDBT-O. Water contact angle measurements revealed that benzothiophene-sulfone-based conjugated polymers display better water compatibility and adsorption, and the synergic effect of better hydrophilic surface and higher surface area of N-PDBT-O might eventually lead to more exposed active sites in comparison to linear L-PDBT-O in the H2 evolution suspension system. The hydrophilicity-controlled strategy could be applied to design of other network conjugated microporous polymer photocatalysts in an attempt to improve the activity.


Subject(s)
Hydrogen/chemistry , Light , Polymers/chemistry , Catalysis , Hydrophobic and Hydrophilic Interactions , Particle Size , Photochemical Processes , Polymers/chemical synthesis , Porosity , Sulfones/chemistry , Surface Properties , Thiophenes/chemistry
16.
Mater Sci Eng C Mater Biol Appl ; 87: 155-166, 2018 Jun 01.
Article in English | MEDLINE | ID: mdl-29549945

ABSTRACT

For successful theranosis of brain diseases, limited access of therapeutic molecules across blood-brain barrier (BBB) needs be overcome in brain delivery. Currently, peptide derivatives of rabies virus glycoprotein (RVG) have been exploited as delivery ligands to transport nanocarriers across BBB and specifically into the brain. The targeting peptides usually conjugate to the nanocarrier surface, and the cargoes, including siRNA, miRNA, DNA, proteins and small molecular chemicals, are complexed or encapsulated in the nanocarriers. The peptide ligand of the RVG-modified nanocarriers introduces the conjugated targeted-delivery into the brain, and the cargoes are involved in disease theranosis. The peptide-modified nanocarriers have been applied to diagnose and treat various brain diseases, such as glioma, Alzheimer's disease, ischemic injury, protein misfolding diseases etc. Since the targeting delivery system has displayed good biocompatibility and desirable therapeutic effect, it will raise a potential application in treating brain diseases.


Subject(s)
Blood-Brain Barrier/metabolism , Brain Diseases/drug therapy , Drug Carriers , Glycoproteins , Peptides , Rabies virus/chemistry , Theranostic Nanomedicine/methods , Viral Proteins , Animals , Blood-Brain Barrier/pathology , Brain Diseases/metabolism , Brain Diseases/pathology , Drug Carriers/chemistry , Drug Carriers/pharmacokinetics , Drug Carriers/therapeutic use , Glycoproteins/chemistry , Glycoproteins/pharmacokinetics , Glycoproteins/therapeutic use , Humans , Peptides/chemistry , Peptides/pharmacokinetics , Peptides/therapeutic use , Viral Proteins/chemistry , Viral Proteins/pharmacokinetics , Viral Proteins/therapeutic use
17.
Adv Mater ; 29(31)2017 Aug.
Article in English | MEDLINE | ID: mdl-28614603

ABSTRACT

Solar-driven reduction of dinitrogen (N2 ) to ammonia (NH3 ) is severely hampered by the kinetically complex and energetically challenging multielectron reaction. Oxygen vacancies (OVs) with abundant localized electrons on the surface of bismuth oxybromide-based semiconductors are demonstrated to have the ability to capture and activate N2 , providing an alternative pathway to overcome such limitations. However, bismuth oxybromide materials are susceptible to photocorrosion, and the surface OVs are easily oxidized and therefore lose their activities. For realistic photocatalytic N2 fixation, fabricating and enhancing the stability of sustainable OVs on semiconductors is indispensable. This study shows the first synthesis of self-assembled 5 nm diameter Bi5 O7 Br nanotubes with strong nanotube structure, suitable absorption edge, and many exposed surface sites, which are favorable for furnishing sufficient visible light-induced OVs to realize excellent and stable photoreduction of atmospheric N2 into NH3 in pure water. The NH3 generation rate is as high as 1.38 mmol h-1 g-1 , accompanied by an apparent quantum efficiency over 2.3% at 420 nm. The results presented herein provide new insights into rational design and engineering for the creation of highly active catalysts with light-switchable OVs toward efficient, stable, and sustainable visible light N2 fixation in mild conditions.

18.
Drug Discov Today ; 22(9): 1318-1335, 2017 09.
Article in English | MEDLINE | ID: mdl-28428056

ABSTRACT

Sustained gene delivery is of particular importance today because it circumvents the need for repeated therapeutic administration and provides spatial and temporal control of the release profile. Better understanding of the genetic basis of diseases and advances in gene therapy have propelled significant research on biocompatible gene carriers for therapeutic purposes. Varied biodegradable polymer-based architectures have been used to create new compositions with unique properties suitable for sustained gene delivery. This review presents the most recent advances in various polymeric systems: hydrogels, microspheres, nanospheres and scaffolds, having complex architectures to encapsulate and deliver functional genes. Through the recombination of different existing polymer systems, the multicomplex systems can be further endowed with new properties for better-targeted biomedical applications.


Subject(s)
Gene Transfer Techniques , Animals , Genetic Vectors , Humans , Polymers
19.
Mater Sci Eng C Mater Biol Appl ; 70(Pt 2): 1156-1162, 2017 Jan 01.
Article in English | MEDLINE | ID: mdl-27772717

ABSTRACT

Relatively electron-deficient perylenediimide (PDI) and relatively electron-rich porphyrin (Por) were introduced into the middle of 16-mer glycol nucleic acid (GNA), and up to five consecutive chromophores were arranged in the zipper-like interstrand alternating fashion. Remarkable variation for the CD spectra ascribed to chromophores was observed, and bathochromic shift in the UV/Vis absorption region of chromophores occurred upon duplex formation. Interestingly, zipper-like heteroaggregates of chromophores inside had marvelous positive effects on the stabilization of the duplex, Tm of Por-PDI-Por sandwich-type modified GNA duplex was increased by 24°C in comparison with three A-T base pairs, moreover, Por-PDI-Por-PDI-Por interstrand modified GNA duplex was even stabilized by 25°C in replacement of five A-T base pairs. The specificity of high duplex stability might be driven by the strong hydrophobic electrostatic complementarity between PDI and Por face-centered stacking.


Subject(s)
Imides/chemistry , Perylene/analogs & derivatives , Porphyrins/chemistry , Static Electricity , Base Pairing , Circular Dichroism , Computer Simulation , Perylene/chemistry , Spectrophotometry, Ultraviolet , Temperature
20.
Zhongguo Yi Liao Qi Xie Za Zhi ; 40(1): 35-7, 2016 Jan.
Article in Chinese | MEDLINE | ID: mdl-27197495

ABSTRACT

This article introduces a cerebral thrombus protection device for the cerebral interventional treatment, also introduces the principle, design and manufacturing process of the device, and confirmes the effectiveness in vitro experiment.


Subject(s)
Thrombosis/prevention & control , Equipment Design , Humans
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