Your browser doesn't support javascript.
loading
Show: 20 | 50 | 100
Results 1 - 20 de 45
Filter
1.
Cell Mol Biol Lett ; 29(1): 69, 2024 May 13.
Article in English | MEDLINE | ID: mdl-38741032

ABSTRACT

BACKGROUND: Pulmonary hypertension (PH) is a progressive disease characterized by pulmonary vascular remodeling. Increasing evidence indicates that endothelial-to-mesenchymal transition (EndMT) in pulmonary artery endothelial cells (PAECs) is a pivotal trigger initiating this remodeling. However, the regulatory mechanisms underlying EndMT in PH are still not fully understood. METHODS: Cytokine-induced hPAECs were assessed using RNA methylation quantification, qRT-PCR, and western blotting to determine the involvement of N6-methyladenosine (m6A) methylation in EndMT. Lentivirus-mediated silencing, overexpression, tube formation, and wound healing assays were utilized to investigate the function of METTL3 in EndMT. Endothelial-specific gene knockout, hemodynamic measurement, and immunostaining were performed to explore the roles of METTL3 in pulmonary vascular remodeling and PH. RNA-seq, RNA Immunoprecipitation-based qPCR, mRNA stability assay, m6A mutation, and dual-luciferase assays were employed to elucidate the mechanisms of RNA methylation in EndMT. RESULTS: The global levels of m6A and METTL3 expression were found to decrease in TNF-α- and TGF-ß1-induced EndMT in human PAECs (hPAECs). METTL3 inhibition led to reduced endothelial markers (CD31 and VE-cadherin) and increased mesenchymal markers (SM22 and N-cadherin) as well as EndMT-related transcription factors (Snail, Zeb1, Zeb2, and Slug). The endothelial-specific knockout of Mettl3 promoted EndMT and exacerbated pulmonary vascular remodeling and hypoxia-induced PH (HPH) in mice. Mechanistically, METTL3-mediated m6A modification of kruppel-like factor 2 (KLF2) plays a crucial role in the EndMT process. KLF2 overexpression increased CD31 and VE-cadherin levels while decreasing SM22, N-cadherin, and EndMT-related transcription factors, thereby mitigating EndMT in PH. Mutations in the m6A site of KLF2 mRNA compromise KLF2 expression, subsequently diminishing its protective effect against EndMT. Furthermore, KLF2 modulates SM22 expression through direct binding to its promoter. CONCLUSIONS: Our findings unveil a novel METTL3/KLF2 pathway critical for protecting hPAECs against EndMT, highlighting a promising avenue for therapeutic investigation in PH.


Subject(s)
Adenosine , Endothelial Cells , Epithelial-Mesenchymal Transition , Hypertension, Pulmonary , Kruppel-Like Transcription Factors , Methyltransferases , Adenosine/analogs & derivatives , Adenosine/metabolism , Animals , Hypertension, Pulmonary/genetics , Hypertension, Pulmonary/metabolism , Humans , Methyltransferases/metabolism , Methyltransferases/genetics , Mice , Endothelial Cells/metabolism , Epithelial-Mesenchymal Transition/genetics , Kruppel-Like Transcription Factors/metabolism , Kruppel-Like Transcription Factors/genetics , Pulmonary Artery/metabolism , Pulmonary Artery/pathology , Methylation , Mice, Inbred C57BL , Cadherins/metabolism , Cadherins/genetics , Male , Vascular Remodeling/genetics , Cells, Cultured
2.
JBI Evid Implement ; 2024 Apr 02.
Article in English | MEDLINE | ID: mdl-38557502

ABSTRACT

INTRODUCTION AND OBJECTIVES: Kidney transplantation is an effective treatment for end-stage kidney disease. Kidney transplant recipients (KTRs) are prone to experiencing reduced physical function, depression, fatigue, and lack of exercise motivation due to their sedentary lifestyle before surgery. Exercise is an effective intervention for KTRs, but it has not been properly implemented in many practice settings. This project aimed to promote evidence-based exercises as part of KTRs' rehabilitation to improve their health outcomes. METHODS: This project was informed by the JBI Evidence Implementation Framework. The project was conducted in the organ transplant ward of a tertiary comprehensive hospital in Changsha, China. Based on a summary of best evidence, 12 audit criteria were developed for the baseline and follow-up audits involving 30 patients and 20 nursing staff. The JBI Practical Application of Clinical Evidence System (PACES) and Getting Research into Practice (GRiP) tool were used to identify barriers and facilitators and develop targeted strategies to improve issues. RESULTS: Compared with the baseline audit, significant improvements were achieved in most of the criteria in the follow-up audit, with 9 of the 12 criteria reaching 100% compliance. Notably, the 6-minute walk distance test results were significantly higher, while the Self-Rating Depression Scale and Self-Rating Anxiety Scale scores were significantly lower (p < 0.05). CONCLUSIONS: This project demonstrates that evidence-based practice can improve the clinical practice of rehabilitation exercises for KTRs. The GRiP strategies proved to be extremely useful, notably, the formulation of a standardized rehabilitation exercise protocol, training, and enhancement of the exercising environment. Head nurses' leadership and decision-making also played an important role in the success of this project. SPANISH ABSTRACT: http://links.lww.com/IJEBH/A180.

3.
J Am Chem Soc ; 146(15): 10785-10797, 2024 Apr 17.
Article in English | MEDLINE | ID: mdl-38573588

ABSTRACT

The anti-Stokes shift represents the capacity of photon upconversion to convert low-energy photons to high-energy photons. Although triplet exciton-mediated photon upconversion presents outstanding performance in solar energy harvesting, photoredox catalysis, stereoscopic 3D printing, and disease therapeutics, the interfacial multistep triplet exciton transfer leads to exciton energy loss to suppress the anti-Stokes shift. Here, we report near infrared-II (NIR-II) excitable triplet exciton-mediated photon upconversion using a hybrid photosensitizer consisting of lead sulfide quantum dots (PbS QDs) and new surface ligands of thiophene-substituted diketopyrrolopyrrole (Th-DPP). Under 1064 nm excitation, this photon upconversion revealed a record-corrected upconversion efficiency of 0.37% (normalized to 100%), with the anti-Stokes shift (1.07 eV) approaching the theoretical limit (1.17 eV). The observation of this unexpected result is due to our discovery of the presence of a weak interaction between the sulfur atom on Th-DPP and Pb2+ on the PbS QDs surface, facilitating electronic coupling between PbS QDs and Th-DPP, such that the realization of triplet exciton transfer efficiency is close to 100% even when the energy gap is as small as 0.04 eV. With this premise, this photon upconversion as a photocatalyst enables the production of standing organic gel via photopolymerization under 1064 nm illumination, displaying NIR-II photon-driven photoredox catalysis. This research not only establishes the foundation for enhancing the performance of NIR-II excitable photonic upconversion but also promotes its development in photonics and photoredox catalysis.

4.
ACS Appl Mater Interfaces ; 16(6): 7512-7521, 2024 Feb 14.
Article in English | MEDLINE | ID: mdl-38318769

ABSTRACT

Near-infrared light excitable triplet-triplet annihilation upconversion (NIR TTA-UC) materials have attracted interest in a variety of emerging applications such as photoredox catalysis, optogenetics, and stereoscopic 3D printing. Currently, the practical application of NIR TTA-UC materials requires substantial improvement in photostability. Here, we found that the new annihilator of π-expanded diketopyrrolopyrrole (π-DPP) cannot activate oxygen to generate superoxide anion via photoinduced electron transfer, and its electron-deficient characteristics prevent the singlet oxygen-mediated [2 + 2] cycloaddition reaction; thus, π-DPP exhibited superior resistance to photobleaching. In conjunction with the NIR photosensitizer PdTNP, the upconversion efficiency of π-DPP is as high as 8.9%, which is eight times of the previously reported PdPc/Furan-DPP. Importantly, after polystyrene film encapsulation, less than 10% photobleaching was observed for this PdTNP/π-DPP-based NIR TTA-UC material after four hours of intensive NIR light exposure. These findings provide a type of annihilator with extraordinary photostability, facilitating the development of NIR TTA-UC materials for practical photonics.

5.
Int J Oncol ; 63(5)2023 11.
Article in English | MEDLINE | ID: mdl-37681483

ABSTRACT

Osteosarcoma (OS) prevailing in children and adolescents mainly occurs at the metaphysis of long bones. As it is associated with a high invasive and metastatic ability, resistance to chemotherapy, and a low 5­year survival rate, the diagnosis and treatment of OS post a global healthy issue. Over the past decades, RNA biology has shed new light onto the pathogenesis of OS. As a type of non­coding RNAs, circular RNAs (circRNAs) have been found to play crucial roles in cellular activities. Recently, a large number of circRNAs have been identified in OS and some of them have been validated to be functional in OS. In the present review, abnormally expressed and different types of circRNAs in OS are summarized. Functional studies on circRNAs have revealed that circRNAs can regulate gene expression at different levels, such as gene transcription, precursor mRNA splicing, miRNA sponges and translation into proteins/peptides. Mechanistic analyses on circRNAs show that circRNAs can regulate JAK­STAT3, NF­κB, PI3K­AKT, Wnt/ß­catenin signaling pathways during the occurrence and development of OS. Furthermore, the potential clinical applications of circRNAs are also emphasized. The present review focus on the current knowledge on the functions and mechanisms of circRNAs in the pathogenesis of OS, aiming to provide new insight into the OS diagnosis and treatment of OS.


Subject(s)
Bone Neoplasms , MicroRNAs , Osteosarcoma , Adolescent , Child , Humans , RNA, Circular/genetics , Phosphatidylinositol 3-Kinases , MicroRNAs/genetics , Osteosarcoma/genetics , Bone Neoplasms/genetics
6.
Clin Kidney J ; 16(8): 1316-1329, 2023 Aug.
Article in English | MEDLINE | ID: mdl-37529646

ABSTRACT

Background: Kidney transplant has become the preferred therapy for end-stage renal disease. However, kidney transplant recipients (KTRs) still face several challenges, such as physical inactivity. The purpose of this study was to explore the effects of a nurse-led physical exercise program in Chinese KTRs. Methods: A total of 106 participants were enrolled from the Third Xiangya Hospital of Central South University between July 2021 and June 2022 and randomly assigned to the control or intervention groups. Participants in the control group were provided with routine nursing care and participants in the intervention group received a nurse-led rigorous physical exercise program that was divided into two stages: the pre-discharge stage and the post-discharge stage. The pre-discharge stage included the non-ambulatory and ambulatory stages. The Chinese traditional exercise Baduanjin was incorporated into the physical exercise during the ambulatory stage. The post-discharge stage continued the same exercise as the ambulatory stage at home. After 3 months of intervention, both groups received the same follow-up for 3 months. The primary and secondary outcomes of all participants were collected. The data were analysed with repeated measures analysis of variance to examine the effectiveness of the intervention. Results: Compared with the control group, the intervention group had less fatigue and more motivation to be active in primary outcomes. Moreover, patients in the intervention group had a higher phase angle, a longer 6-minute walk distance, more 30-second chair stand times and decreased anxiety and depression levels in secondary outcomes. No adverse events were observed during the intervention. There were no significant differences in all dimensions of the quality-of-life questionnaire between the intervention and the control group. Conclusion: Chinese KTRs could benefit from the nurse-led physical exercise program post-operatively. Trial registration: ChiCTR2100048755.

7.
Molecules ; 28(14)2023 Jul 18.
Article in English | MEDLINE | ID: mdl-37513346

ABSTRACT

Triplet-triplet annihilation upconversion (TTA-UC) has considerable potential for emerging applications in bioimaging, optogenetics, photoredox catalysis, solar energy harvesting, etc. Fluoroboron dipyrrole (Bodipy) dyes are an essential type of annihilator in TTA-UC. However, conventional Bodipy dyes generally have large molar extinction coefficients and small Stokes shifts (<20 nm), subjecting them to severe internal filtration effects at high concentrations, and resulting in low upconversion quantum efficiency of TTA-UC systems using Bodipy dyes as annihilators. In this study, a Bodipy dimer (B-2) with large Stokes shifts was synthesized using the strategy of dimerization of an already reported Bodipy annihilator (B-1). Photophysical characterization and theoretical chemical analysis showed that both B-1 and B-2 can couple with the red light-activated photosensitizer PdTPBP to fulfill TTA-UC; however, the higher fluorescence quantum yield of B-2 resulted in a higher upconversion efficiency (ηUC) for PdTPBP/B-2 (10.7%) than for PdTPBP/B-1 (4.0%). This study proposes a new strategy to expand Bodipy Stokes shifts and improve TTA-UC performance, which can facilitate the application of TTA-UC in photonics and biophotonics.

8.
Biomimetics (Basel) ; 8(3)2023 Jul 09.
Article in English | MEDLINE | ID: mdl-37504187

ABSTRACT

The unique drive principle and strong manipulation ability of spider legs have led to several bionic robot designs. However, some parameters of bionic actuators still need to be improved, such as torque. Inspired by the hydraulic drive principle of spider legs, this paper describes the design of a bionic actuator characterized by the use of air pressure on each surface and its transmittance in the direction of movement, achieving a torque amplification effect. The produced torque is as high as 4.78 N m. In addition, its torque characteristics during folding motions are similar to those during unfolding motions, showing that the bionic actuator has stable bidirectional drive capability.

9.
Nat Commun ; 14(1): 4002, 2023 Jul 06.
Article in English | MEDLINE | ID: mdl-37414824

ABSTRACT

The ability to deliver electrons is vital for dye-based photocatalysts. Conventionally, the aromatic stacking-based charge-transfer complex increases photogenerated electron accessibility but decreases the energy of excited-state dyes. To circumvent this dilemma, here we show a strategy by tuning the stacking mode of dyes. By decorating naphthalene diimide with S-bearing branches, the S···S contact-linked naphthalene diimide string is created in coordination polymer, thereby enhancing electron mobility while simultaneously preserving competent excited-state reducing power. This benefit, along with in situ assembly between naphthalene diimide strings and exogenous reagent/reactant, improves the accessibility of short-lived excited states during consecutive photon excitation, resulting in greater efficiency in photoinduced electron-transfer activation of inert bonds in comparison to other coordination polymers with different dye-stacking modes. This heterogeneous approach is successfully applied in the photoreduction of inert aryl halides and the successive formation of CAr-C/S/P/B bonds with potential pharmaceutical applications.


Subject(s)
Chalcogens , Inorganic Chemicals , Polymers/chemistry , Electron Transport , Naphthalenes/chemistry
10.
Sci Total Environ ; 892: 164662, 2023 Sep 20.
Article in English | MEDLINE | ID: mdl-37277044

ABSTRACT

Owing to its biotoxicity and inductive effect on photochemical pollution, atmospheric peroxyacetyl nitrate (PAN), which is a typical product of atmospheric photochemical reactions, has attracted much research attention. However, to the best of our knowledge, few comprehensive studies have been conducted on the seasonal variation and key influencing factors of PAN concentrations in southern China. In this study, PAN, ozone (O3), precursor volatile organic compound (VOC), and other pollutant concentrations were measured online for 1 year (from October 2021 to September 2022) in Shenzhen, a megacity in the Greater Bay Area of China. The average concentrations of PAN and peroxypropionyl nitrate (PPN) were 0.54 and 0.08 parts per billion (ppb), and the maximum hourly concentrations reached 10.32 and 1.01 ppb, respectively. The results of the generalized additive model (GAM) showed that the atmospheric oxidation capacity and precursor concentration were the most important factors affecting the PAN concentration. According to the steady-state model, the average cumulative contribution to the peroxyacetyl (PA) radical formation rate by six major carbonyl compounds was calculated at 4.2 × 106 molecules cm-3 s-1, and acetaldehyde (63.0 %) and acetone (13.9 %) contributed the most. Furthermore, the photochemical-age-based parameterization method was used to analyze the source contributions of carbonyl compounds and PA radicals. The results showed that although the primary anthropogenic (40.2 %), biogenic (27.8 %), and secondary anthropogenic (16.4 %) sources were the most important contributors of PA radicals, the biogenic and secondary anthropogenic source contributions both increased considerably in summer, and the cumulative proportion of both sources reached ~70 % in July. In addition, a comparison of PAN pollution processes in different seasons revealed that in summer and winter, the PAN concentration was predominantly limited by precursors and meteorological parameters, such as light intensity, respectively.


Subject(s)
Air Pollutants , Ozone , Volatile Organic Compounds , Seasons , Air Pollutants/analysis , China , Ozone/analysis , Volatile Organic Compounds/analysis , Environmental Monitoring
11.
Angew Chem Int Ed Engl ; 62(25): e202303093, 2023 Jun 19.
Article in English | MEDLINE | ID: mdl-37070679

ABSTRACT

Triplet-triplet annihilation upconversion (TTA-UC) with near-infrared (NIR) photosensitizers is highly desirable for a variety of emerging applications. However, the development of NIR-to-blue TTA-UC with a large anti-Stokes shift is extremely challenging because of the energy loss during the intersystem crossing (ISC). Here, we develop the first NIR-absorbing B,N-heteroarene-based sensitizer (BNS) with multi-resonance thermally activated delayed fluorescence (MR-TADF) characters to achieve efficient NIR-to-blue TTA-UC. The small energy gap between the singlet and triplet excited states (0.14 eV) of BNS suppresses the ISC energy loss, and its long-delayed fluorescence lifetime (115 µs) contributes to efficient triplet energy transfer. As a result, the largest anti-Stokes shift (1.03 eV) among all heavy-atom-free NIR-activatable TTA-UC systems is obtained with a high TTA-UC quantum yield of 2.9 % (upper limit 50 %).


Subject(s)
Cytoskeleton , Photosensitizing Agents , Photosensitizing Agents/pharmacology , Energy Transfer , Fluorescence , Vibration
12.
Nat Commun ; 14(1): 1102, 2023 Feb 27.
Article in English | MEDLINE | ID: mdl-36843133

ABSTRACT

Selective photoactivation of inert aryl halides is a fundamental challenge in organic synthesis. Specially, the long-wavelength red light is more desirable than the widely-applied blue light as the excitation source for photoredox catalysis, due to its superior penetration depth. However, the long-wavelength red light-driven photoactivation of inert aryl halides remains a challenge, mainly because of the low energy of the single long-wavelength red photon. Herein, we report the photoreduction of aryl bromides/chlorides with 656 nm LED via triplet-triplet annihilation (TTA) strategy. This method is based on our discovery that the commonly used chromophore of perylene can serve as an efficient and metal-free photocatalyst to enable the photoreduction of inert aryl halides without the conventional need for electronic sacrificial agents. By introducing a red light-absorbing photosensitizer to this perylene system, we accomplish the long-wavelength red light-driven photoreduction of aryl halides via sensitized TTA mechanism. Moreover, the performance of such a TTA-mediated photoreduction can be significantly enhanced when restricting the rotation freedom of phenyl moiety for perylene derivatives to suppress their triplet nonradiative transition, in both small and large-scale reaction settings.

13.
Angew Chem Int Ed Engl ; 62(11): e202218341, 2023 03 06.
Article in English | MEDLINE | ID: mdl-36634030

ABSTRACT

Metal-free long-wavelength light-driven prodrug photoactivation is highly desirable for applications such as neuromodulation, drug delivery, and cancer therapy. Herein, via triplet fusion, we report on the far-red light-driven photo-release of an anti-cancer drug by coupling the boron-dipyrromethene (BODIPY)-based photosensitizer with a photocleavable perylene-based anti-cancer drug. Notably, this metal-free triplet fusion photolysis (TFP) strategy can be further advanced by incorporating an additional functional dopant, i.e. an immunotherapy medicine inhibiting the indoleamine 2,3-dioxygenase (IDO), with the far-red responsive triplet fusion pair in an air-stable nanoparticle. With this IDO inhibitor-assisted TFP system we observed efficient inhibition of primary and distant tumors in a mouse model at record-low excitation power, compared to other photo-assisted immunotherapy approaches. This metal-free TFP strategy will spur advancement in photonics and biophotonics fields.


Subject(s)
Antineoplastic Agents , Immune Checkpoint Inhibitors , Animals , Mice , Photolysis , Light , Immunotherapy , Indoleamine-Pyrrole 2,3,-Dioxygenase
14.
Acc Chem Res ; 55(18): 2604-2615, 2022 09 20.
Article in English | MEDLINE | ID: mdl-36074952

ABSTRACT

Photon upconversion, the process of converting low-energy photons into high-energy ones, has been widely applied for solar energy conversion, photoredox catalysis, and various biological applications such as background-free bioimaging, cancer therapy, and optogenetics. Upconversion materials that are based on triplet-triplet annihilation (TTA) are of particular interest due to their low excitation power requirements (e.g., ambient sunlight) and easily tunable excitation and emission wavelengths. Despite advances that have been made with respect to TTA upconversion (TTA-UC) in the past decade, several challenges remain for near-infrared light-activatable triplet-triplet annihilation upconversion (NIR TTA-UC). These challenges include low upconversion quantum yield, small anti-Stokes shift, and incompatibility with oxygen, the latter of which seriously limits the practical applications of NIR TTA-UC.This Account will summarize the recent research endeavors to address the above-mentioned challenges and the recent new applications. The first part of this Account highlights recent strategies of molecular design to modulate the excited states of photosensitizers and annihilators, two key factors to determine TTA-UC performance. Novel molecular engineering strategies such as the resonance energy transfer method, dimerization of dye units, and the helix twist molecular structure have been proposed to tune the excited states of photosensitizers. The obtained photosensitizers exhibited enhanced absorption of deep tissue penetrable near-infrared (NIR) light, produced a triplet excited state with elevated energy level and prolonged lifetime, and promoted intersystem crossing, leading to an upgraded TTA-UC system with significantly expanded anti-Stokes shift. With respect to the annihilator, the perylene derivatives were systematically explored, and their attached aromatic groups were found to be the key to adjusting the energy levels of both the triplet and singlet excited states. The resultant optimal TTA-UC system exhibits the highest recorded efficiency among NIR TTA-UC systems.Moreover, to resolve the oxygen-induced TTA-UC quenching, enzymatic reactions were recently introduced. More specifically, the glucose oxidase-catalyzed glucose oxidation reaction showed the ability to rapidly consume oxygen to turn on the TTA-UC luminescence in an aqueous solution. The resultant TTA-UC nanoparticle was able to detect glucose and an enzyme related to glucose metabolism in a highly specific, sensitive, and background-free manner. Further, the upconverted singlet excited state of the annihilator was directly utilized as the catalyst or the excited substrate. For example, the modification of annihilators and drug molecules with photolabile linkages can realize the long wavelength light-induced photolysis. Compared to direct short-wavelength-driven photolysis, this sensitized TTA photolysis (TTAP) exhibits superior reaction yield and lower photodamage, which are important in the release of drugs for tumor treatment in vivo. Moreover, the improved upconversion efficiency can enable the successful coupling of NIR TTA-UC with a visible light absorbing photocatalyst for NIR-driven photoredox catalysis. Compared to direct visible-light photocatalysis, TTA-UC mediated NIR photoredox catalysis showed superior product yield especially in large scale reaction systems owing to the deep penetration power of NIR light. More interestingly, among a few promising technology applications, three-dimensional (3D) printing based on photopolymerization can operate with faster speed and energy-input several orders of magnitude lower when the two-photon polymerization is replaced with TTA-UC mediated polymerization. We believe this Account will spur interest in the further development and application of TTA-UC in the areas of energy, chemistry, material science, and biology.


Subject(s)
Perylene , Photosensitizing Agents , Glucose , Glucose Oxidase , Infrared Rays , Oxygen/chemistry , Photosensitizing Agents/chemistry
15.
Adv Drug Deliv Rev ; 189: 114479, 2022 10.
Article in English | MEDLINE | ID: mdl-35932906

ABSTRACT

Phototherapy is a noninvasive cancer treatment that relies on the interaction between light and photoactive agents. These photoactive agents are typically organic dyes, but their hydrophobic nature and self-aggregation tendency in biological media greatly restricts the development of highly effective phototherapeutic systems. In the past decade, functional dye-doped metal-organic framework (MOF)-based phototherapy has attracted enormous interest because organic dyes can be encapsulated and isolated within the MOF structure to show superior treatment efficacy. In addition to incorporating the reported phototherapeutic dyes into MOF as the ligand or the guest in the pores, the construction of an MOF-based phototherapy agent can also be extended to these dye units that are previously inactive for phototherapy. Thus, this review focuses on the emerging development of phototherapeutic MOFs that exhibited better performance than the involving dye units due to the controlled dye aggregation within the MOF. The related mechanisms and some emerging future directions of dye-doped MOF-based phototherapy are also discussed and summarized.


Subject(s)
Metal-Organic Frameworks , Coloring Agents , Humans , Ligands , Phototherapy
16.
Inorg Chem ; 61(35): 13768-13774, 2022 Sep 05.
Article in English | MEDLINE | ID: mdl-35998355

ABSTRACT

A new metal-organic framework (MOF) with tetrazole-derived triphenylamine (TPA) as the ligand, namely Mn-TPA, has been successfully prepared and thoroughly characterized via thermogravimetric analysis, IR spectroscopy, elemental analysis, UV-vis absorption, fluorescence analysis, bond valence sum calculations, and single-crystal and powder X-ray diffraction analysis. The undulating monolayer of Mn-TPA can hinder the interaction and tight stacking among analytes, which creates a bionic microenvironment for the electrochemical recognition process. Mn-TPA exhibits high specific surface area, stable film-forming capacity, excellent electrochemical activity, and good biocompatibility. Furthermore, the developed Mn-TPA-based immunosensing system exhibits an excellent limit of detection of 0.50 pg·mL-1 toward vomitoxin, which is more outstanding than that of the reported vomitoxin-sensing system. Thus, this work shows the great potential of a well-designed MOF as an easy-to-make and highly sensitive electrochemical platform for biosensing in food safety detection and other fields.


Subject(s)
Biosensing Techniques , Metal-Organic Frameworks , Biosensing Techniques/methods , Food Inspection , Metal-Organic Frameworks/chemistry , Tetrazoles
17.
Molecules ; 27(13)2022 Jun 23.
Article in English | MEDLINE | ID: mdl-35807299

ABSTRACT

Near-infrared (NIR) light-triggered photoredox catalysis is highly desirable because NIR light occupies almost 50% of solar energy and possesses excellent penetrating power in various media. Herein we utilize a metal-free boron dipyrromethene (BODIPY) derivative as the photocatalyst to achieve NIR light (720 nm LED)-driven oxidation of benzylamine derivatives, sulfides, and aryl boronic acids. Compared to blue light-driven photooxidation using Ru(bpy)3Cl2 as a photocatalyst, NIR light-driven photooxidation exhibited solvent independence and superior performance in large-volume (20 mL) reaction, presumably thanks to the neutral structure of a BODIPY photocatalyst and the deeper penetration depth of NIR light. We further demonstrate the application of this metal-free NIR photooxidation to prodrug activation and combination with Cu-catalysis for cross coupling reaction, exhibiting the potential of metal-free NIR photooxidation as a toolbox for organic synthesis and drug development.


Subject(s)
Infrared Rays , Light , Boronic Acids , Catalysis , Oxidation-Reduction , Sulfides
18.
ACS Appl Mater Interfaces ; 14(6): 7980-7989, 2022 Feb 16.
Article in English | MEDLINE | ID: mdl-35119261

ABSTRACT

Anthraquinone (AQ) as an effective hydrogen atom transfer catalyst was limited in photocatalysis application due to the dimerization of reduced AQ. Sr-NDI@AQ, encapsulating AQ into the channel of Sr-NDI, paved a new way for solving the problem of dimerization of reduced AQ and improving the catalytic efficiency owing to the fast electron transfer from reduced AQ to the ligand through host-guest interaction. The structure of Sr-NDI@AQ was determined by single-crystal X-ray diffraction, and the value for distance and torsion angle between the ligand and AQ was calculated. The photochemical and electrochemical properties for Sr-NDI@AQ were characterized through a series of experiments. The coupling reaction between aldehyde and phenyl vinyl sulfone and photoacetalization reaction were carried out, displaying the improving catalytic efficiency of Sr-NDI@AQ compared to Sr-NDI and AQ. The reaction mechanisms were proposed through radical capture and electron paramagnetic resonance experiments.

19.
Adv Mater ; 34(14): e2107962, 2022 Apr.
Article in English | MEDLINE | ID: mdl-34877721

ABSTRACT

Persistent luminescence is a unique optical process where long-lasting afterglow persists after the cessation of excitation. Nanoscale persistent luminescent materials are getting increased research interest from various fields due to their unique optical property. In recent years, inspiring achievements have been made to produce uniform persistent luminescence nanoparticles (PLNPs) in a controllable manner, unleashing their fascinating potential, surpassing other types of luminescent materials in a wide variety of application such as high-contrast bioimaging and high-resolution X-ray detection. In this review, the evolution of uniform PLNPs, from their bulk phosphor counterparts, to the "top-down" preparation of nanoscale persistent luminescent materials, to the recent "bottom-up" synthesis of uniform PLNPs is first summarized. The respective milestones of uniform PLNPs prepared by templated synthesis, aqueous synthesis, and colloidal synthesis are highlighted. The key optical properties that can be enhanced in uniform PLNPs, including increasing the persistent luminescence intensity, tuning the excitation irradiance, as well as the emission wavelengths are then analyzed. Detailed strategies to enhance each optical property are also discussed in various sections. Finally, future challenges are highlighted with respect to the perspectives on the development of next-generation PLNPs with novel applications.


Subject(s)
Luminescence , Nanoparticles , X-Rays
20.
Angew Chem Int Ed Engl ; 60(44): 23569-23573, 2021 10 25.
Article in English | MEDLINE | ID: mdl-34347334

ABSTRACT

Organic self-assembled co-crystals have garnered considerable attention due to their facile synthesis and intriguing properties, but supramolecular interactions restrict their stability in aqueous solution, which is especially important for biological applications. Herein, we report on the first biological application of aqueous dispersible self-assembled organic co-crystals via the construction of metal-organic framework (MOF) -stabilized co-crystals. In particular, we built an electron-deficient MOF with naphthalene diimide (NDI) as the ligand and biocompatible Ca2+ as the metal nodes. An electron donor molecule, pyrene, was encapsulated to form the host-guest MOF self-assembled co-crystal. We observed that such MOF structure leads to uniquely high-density ordered arrangement and the close intermolecular distance (3.47 Å) of the charge transfer pairs. Hence, the concomitant superior charge transfer interaction between pyrene/NDI can be attained and the resultant photothermal conversion efficiency of Py@Ca-NDI in aqueous solution can thus reach up to 41.8 %, which, to the best of our knowledge, is the highest value among the reported organic co-crystal materials; it is also much higher than that of the FDA approved photothermal agent ICG as well as most of the reported MOFs. Based on this realization, as a proof of concept, we demonstrated that such a self-assembled organic co-crystal platform can be used in biological applications that are exemplified via highly effective long wavelength light photothermal therapy.


Subject(s)
Biocompatible Materials/chemistry , Calcium/chemistry , Imides/chemistry , Metal-Organic Frameworks/chemical synthesis , Naphthalenes/chemistry , Phototherapy , Pyrenes/chemistry , Catalysis , Metal-Organic Frameworks/chemistry
SELECTION OF CITATIONS
SEARCH DETAIL
...