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2.
Anal Chem ; 2024 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-38755966

RESUMO

Nanogap-based plasmonic metal nanocrystals have been applied in surface-enhanced Raman scattering detection, while the closed and insufficient electromagnetic fields as well as the nonreproducible Raman signal of the substrate greatly restrict the actual application. Herein, a highly uniform Au/AgAu monolayer with abundant nanogaps and huge electromagnetic enhancement is prepared, which shows ultrasensitive and reproducible SERS detection. Au/AgAu with an inner nanogap is first prepared based on Au nanotriangles, and the nanogap is opened from the three tips via a subsequent etching process. The open-gap Au/AgAu displays much higher SERS efficiency than Au and Au/AgAu with an inner nanogap on detecting crystal violet due to the open-gap induced electromagnetic enhancement and improved molecular absorption. Furthermore, the open-gap Au/AgAu monolayer is prepared via interfacial self-assembly, which shows further improved SERS due to the dense and strong hotspots in the nanocavities induced by the electromagnetic coupling between adjacent open gaps. The monolayer possesses excellent signal stability, uniformity, and reproducibility. The analytic enhancement factor and relative standard deviation reach to 2.12 × 108 and 4.65% on detecting crystal violet, respectively. Moreover, the monolayer achieves efficient detection of thiram in apple juice, biphenyl-4-thiol, 4-mercaptobenzoic, melamine, and a mixed solution of four different molecules, showing great promise in practical detection.

3.
Postgrad Med ; : 1-8, 2024 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-38773675

RESUMO

BACKGROUND: Whether there is a longitudinal association between long-term blood pressure variability (BPV) and subsequent depression among Chinese adults remains inconclusive. METHODS: This study utilized data from a nationwide cohort of the China Health and Retirement Longitudinal Study, which included participants aged > 45 years without prevalent psychiatric or memory-related diseases. The intra-individual coefficient of variation (CV) and standard deviation (SD) across 3 visits from 2011 to 2015 were used to examine the long-term variability in systolic BP (SBP) and diastolic BP (DBP). The depressive symptoms were examined using the 10-item Center for Epidemiologic Studies Depression Scale (CES-D-10), and moderate-to-severe depression was defined as CES-D-10 ≥ 15. RESULTS: A total of 5,249 participants (mean age: 61.4 ± 8.1 years, 46.5% were men) were included in the current analysis. Individuals in the highest quartile of both BP CV and SD were independently correlated with a higher total CES-D-10 score compared to those in the lowest quartile after multivariable adjustment. 1,070 participants (20.4%) had moderate-to-severe depression during the 3-year follow-up period. Participants in the Q4 of SBP and DBP CV had 1.23-fold higher odds (95% CI: 1.01, 1.49) and 1.20-fold higher odds (95% CI: 1.01, 1.41) of moderate-to-severe depression compared to those in Q1. Subgroup analyses revealed that men with higher BP CVs had a greater risk of severe depressive symptoms (p for SBP CV-by-sex interaction = 0.050, p for SBP CV-by-sex interaction = 0.025). CONCLUSIONS: Depression was common among Chinese middle-aged and older adults and long-term visit-to-visit BPV was positively associated with depressive symptoms, highlighting the importance of implementing intensive prevention strategies for depression and enhancing blood pressure monitors in China.

4.
Retina ; 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38564760
5.
Langmuir ; 40(16): 8327-8351, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38606587

RESUMO

High emission of carbon dioxide (CO2) has caused CO2 levels to reach more than 400 ppm in air and led to a serious climate problem. In addition, in confined spaces such as submarines and aircraft, the CO2 concentration increase in the air caused by human respiration also affects human health. In order to protect the environment and human health, the search for high-performance adsorbents for carbon capture from high and low concentration gas is particularly important. Porous carbon materials, possessing the advantages of low cost and renewability, have set off a boom in the research of porous adsorbents, which have the opportunity to be utilized on a large scale for industrial carbon capture in the future. In this review, we summarize the recent research progress of porous carbons for carbon capture from flue gas and directly from air in the last five years, including activated carbon (AC), heteroatom-modified porous carbon, carbon molecular sieves (CMS), and other porous carbon materials, with a focus on the effects of temperature, water content, and gas flow rate of industrial flue gas on the performance of porous carbon adsorbents. We summarize the preparation strategies of various porous carbons and seek environmental friendly porous carbon materials preparation strategies under the premise of improving the CO2 adsorption capacity and selectivity of porous carbon adsorbents. Based on the effects of real industrial flue gas on adsorbents, we provide new ideas and evaluation methods for the development and preparation of porous carbon materials.

6.
BMC Cancer ; 24(1): 411, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38566028

RESUMO

BACKGROUND: Deleterious BRCA1/2 (BRCA) mutation raises the risk for BRCA mutation-related malignancies, including breast, ovarian, prostate, and pancreatic cancer. Germline variation of BRCA exhibits substantial ethnical diversity. However, there is limited research on the Chinese Han population, constraining the development of strategies for BRCA mutation screening in this large ethnic group. METHODS: We profile the BRCA mutational spectrum, including single nucleotide variation, insertion/deletion, and large genomic rearrangements in 2,080 apparently healthy Chinese Han individuals and 522 patients with BRCA mutation-related cancer, to determine the BRCA genetic background of the Chinese Han population, especially of the East Han. Incident cancer events were monitored in 1,005 participants from the healthy group, comprising 11 BRCA pathogenic/likely pathogenic (PLP) variant carriers and 994 PLP-free individuals, including 3 LGR carriers. RESULTS: Healthy Chinese Han individuals demonstrated a distinct BRCA mutational spectrum compared to cancer patients, with a 0.53% (1 in 189) prevalence of pathogenic/likely pathogenic (PLP) variant, alongside a 3 in 2,080 occurrence of LGR. BRCA1 c. 5470_5477del demonstrated high prevalence (0.44%) in the North Han Chinese and penetrance for breast cancer. None of the 3 LGR carriers developed cancer during the follow-up. We calculated a relative risk of 135.55 (95% CI 25.07 to 732.88) for the development of BRCA mutation-related cancers in the BRCA PLP variant carriers (mean age 42.91 years, median follow-up 10 months) compared to PLP-free individuals (mean age 48.47 years, median follow-up 16 months). CONCLUSION: The unique BRCA mutational profile in the Chinese Han highlights the potential for standardized population-based BRCA variant screening to enhance BRCA mutation-related cancer prevention and treatment.


Assuntos
Proteína BRCA1 , Neoplasias da Mama , Masculino , Humanos , Adulto , Pessoa de Meia-Idade , Proteína BRCA1/genética , Mutação em Linhagem Germinativa , Proteína BRCA2/genética , Predisposição Genética para Doença , Detecção Precoce de Câncer , China/epidemiologia , Neoplasias da Mama/diagnóstico , Neoplasias da Mama/epidemiologia , Neoplasias da Mama/genética , Mutação
7.
J Colloid Interface Sci ; 667: 362-370, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38640655

RESUMO

In this study, we employed a straightforward phosphorylation approach to achieve a dual objective: constructing c-a heterostructures consisting of crystalline Ni12P5 and amorphous FeOOH, while simultaneously enhancing oxygen vacancies. The resulting oxygen evolution reaction (OER) catalyst, Ni12P5/FeOOH/NF, exhibited remarkable performance with current densities of 500 mA cm-2 in both 1 M KOH and 1 M KOH + seawater, requiring low overpotentials of only 288 and 365 mV, respectively. Furthermore, Ni12P5/FeOOH/NF exhibited only a slight increase in overpotential, with increments of 18 mV and 70 mV in 1 M KOH after 15 and 150 h, and 32 mV and 108 mV in 1 M KOH + seawater at 500 mA cm-2 after 15 and 150 h, respectively. This minimal change can be attributed to the stabilized c-a structure, the protective coating of Ni12P5, and superhydrophilic. Through in-situ Raman and ex-situ XPS analysis, we discovered that Ni12P5/FeOOH/NF can undergo a reconfiguration into an oxygen vacancy-rich (Fe/Ni)OOH phase during OER process. The elevated OER activity is mainly due to the contribution of the oxygen vacancy-rich (Fe/Ni)OOH phase from the reconfigure of the Ni12P5/FeOOH/NF. This finding emphasizes the critical role of oxygen vacancies in facilitating the production of OO species and overcoming the limitations associated with OOH formation, ultimately enhancing the kinetics of the OER.

8.
Plant Physiol Biochem ; 208: 108509, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38461751

RESUMO

Melatonin (MT) and reduced glutathione (GSH) roles in mitigating chromium (Cr) toxicity in sweetpotato were explored. Plants, pre-treated with varying MT and GSH doses, were exposed to Cr (40 µM). Cr severely hampered growth by disrupting leaf photosynthesis, root system, and oxidative processes and increased Cr absorption. However, the exogenous application of 1 µM of MT and 2 mM of GSH substantially improved growth parameters by enhancing chlorophyll content, gas exchange (Pn, Tr, Gs, and Ci), and chlorophyll fluorescence (Fv/Fm, ETR, qP, and Y(II)). Furthermore, malondialdehyde (MDA), hydrogen peroxide (H2O2), superoxide ion (O2•-), electrolyte leakage (EL), and Cr uptake by roots (21.6 and 27.3%) and its translocation to shoots were markedly reduced by MT and GSH application, protecting the cell membrane from oxidative damage of Cr-toxicity. Microscopic analysis demonstrated that MT and GSH maintained chloroplast structure and integrity of mesophyll cells; they also enhanced stomatal length, width, and density, strengthening the photosynthetic system and plant growth and biomass. MT and GSH improved osmo-protectants (proline and soluble sugars), gene expression, and enzymatic and non-enzymatic antioxidant activities, mitigating osmotic stress and strengthening plant defenses under Cr stress. Importantly, the efficiency of GSH pre-treatment in reducing Cr-toxicity surpassed that of MT. The findings indicate that MT and GSH alleviate Cr detrimental effects by enhancing photosynthetic organ stability, component accumulation, and resistance to oxidative stress. This study is a valuable resource for plants confronting Cr stress in contaminated soils, but further field validation and detailed molecular exploration are necessary.


Assuntos
Melatonina , Melatonina/farmacologia , Cromo/toxicidade , Peróxido de Hidrogênio/metabolismo , Antioxidantes/metabolismo , Glutationa/metabolismo , Estresse Oxidativo , Fotossíntese , Clorofila/metabolismo
9.
J Phys Condens Matter ; 36(30)2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38330447

RESUMO

Decoupling conductivity(σ)and Seebeck coefficient(S)by electronic topological transitions (ETT) under high pressure (2-4 GPa) is a promising method for bismuth telluride (Bi2Te3) to optimize thermoelectric (TE) performance. However, theScannot dramatically increase with increasingσwhen ETT occurs in Bi2Te3, which impedes optimizing TE performance by utilizing ETT in Bi2Te3. A new strategy of enhanced ETT by combining lattice distortions and high pressure is proposed in this work. The lattice distortions in Bi2Te3were introduced by high pressure and high temperature (HPHT) treatment to generate surplus dislocations. Thein-situmeasurements ofσandSat HPHT in Bi2Te3with lattice distortions show an enhanced ETT effect at 2 GPa, which causes decoupleσandSwith an anomalous increase in its|S|about 22%. The ETT effect causes the figure of merit (ZT) of Bi2Te3can be improved to 0.275 at 1.50-2.62 GPa, 460 K, it is more than 62% compared with 0.79 GPa, at 450 K. The excellent TE performance of Bi2Te3arising from the lattice distortions can result in local non-hydrostatic pressure which enhances ETT under high pressure. This work provides a new strategy to enhance ETT to decoupleσandS, and search for better TE materials from the pressure dimension in the future.

10.
Plant Biotechnol J ; 2024 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-38348566

RESUMO

Heavy metal pollution poses a significant risk to human health and wreaks havoc on agricultural productivity. Phytoremediation, a plant-based, environmentally benign, and cost-effective method, is employed to remove heavy metals from contaminated soil, particularly in agricultural or heavy metal-sensitive lands. However, the phytoremediation capacity of various plant species and germplasm resources display significant genetic diversity, and the mechanisms underlying these differences remain hitherto obscure. Given its potential benefits, genetic improvement of plants is essential for enhancing their uptake of heavy metals, tolerance to harmful levels, as well as overall growth and development in contaminated soil. In this study, we uncover a molecular cascade that regulates cadmium (Cd2+ ) tolerance in cotton, involving GhRCD1, GhbHLH12, GhMYB44, and GhHMA1. We identified a Cd2+ -sensitive cotton T-DNA insertion mutant with disrupted GhRCD1 expression. Genetic knockout of GhRCD1 by CRISPR/Cas9 technology resulted in reduced Cd2+ tolerance in cotton seedlings, while GhRCD1 overexpression enhanced Cd2+ tolerance. Through molecular interaction studies, we demonstrated that, in response to Cd2+ presence, GhRCD1 directly interacts with GhbHLH12. This interaction activates GhMYB44, which subsequently activates a heavy metal transporter, GhHMA1, by directly binding to a G-box cis-element in its promoter. These findings provide critical insights into a novel GhRCD1-GhbHLH12-GhMYB44-GhHMA1 regulatory module responsible for Cd2+ tolerance in cotton. Furthermore, our study paves the way for the development of elite Cd2+ -tolerant cultivars by elucidating the molecular mechanisms governing the genetic control of Cd2+ tolerance in cotton.

11.
Chemistry ; 30(19): e202304081, 2024 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-38288909

RESUMO

Optically pure sulfoxides are valuable organosulfur compounds extensively employed in medicinal and organic synthesis. In this study, we present a biocatalytic oxidation-reduction cascade system designed for the preparation of enantiopure sulfoxides. The system involves the cooperation of a low-enantioselective chimeric oxidase SMO (styrene monooxygenase) with a high-enantioselective reductase MsrA (methionine sulfoxide reductase A), facilitating "non-selective oxidation and selective reduction" cycles for prochiral sulfide oxidation. The regeneration of requisite cofactors for MsrA and SMO was achieved via a cascade catalysis process involving three auxiliary enzymes, sustained by cost-effective D-glucose. Under the optimal reaction conditions, a series of heteroaryl alkyl, aryl alkyl and dialkyl sulfoxides in R configuration were synthesized through this "one-pot, one step" cascade reaction. The obtained compounds exhibited high yields of >90 % and demonstrated enantiomeric excess (ee) values exceeding 90 %. This study represents an unconventional and efficient biocatalytic way in utilizing the low-enantioselective oxidase for the synthesis of enantiopure sulfoxides.


Assuntos
Metionina Sulfóxido Redutases , Sulfóxidos , Biocatálise , Oxirredução , Catálise , Estereoisomerismo
12.
Anal Chim Acta ; 1287: 342103, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38182346

RESUMO

BACKGROUND: PLS-DA of high-dimensional metabolomics data is frequently employed to capture the most pertinent features to sample classification. But the presence of numerous insignificant input features could distort the PLS-DA model, blow up and scramble the selected differential features. Usually, univariate filtration is subsequently complemented to refine the selected features, but often giving unstable results. Whereas by precluding insignificant features through univariate data prefiltration assessed by FDR adjusted p-value, PLS-DA can generate more stable and reliable differential features. We explored and compared these two data analysis procedures to gain insights into the underlying mechanisms responsible for the disparate results. RESULTS: The effect of univariate data filtration preceding and succeeding PLS-DA analysis on the identified discriminative features/metabolites was investigated using LC-MS data acquired on the samples of human serum and C. elegans extracts, with and without metabolite standards spiked to simulate the treated and control groups of biological samples. It was shown that the univariate data prefiltration before PLS-DA usually gave less but more stable and likely more reliable and meaningful differential features, while PLS-DA applied directly to the original data could be affected by the presence of insignificant features and orthogonal noise. Large number of insignificant variables and orthogonal noise could distort the generated PLS-DA model and affect the p(corr) value, and artificially inflate the calculated VIP values of relevant features due to the increased total number of input features for model construction, thus leading to more false positives selected by the conventional VIP threshold of 1.0. SIGNIFICANCE AND NOVELTY: Univariate data filtration preceding PLS-DA was important for the identification of reliable differential features if using a conventional threshold of VIP of 1.0. Presence of insignificant features could distort the PLS-DA model and inflate VIP values. Appropriate VIP threshold is associated with the numbers of input features and the model components. For PLS-DA without univariate prefiltration, threshold of VIP larger than 1.0 is recommended for the selection of discriminative features to reduce the false positives.


Assuntos
Caenorhabditis elegans , Espectrometria de Massa com Cromatografia Líquida , Humanos , Animais , Cromatografia Líquida , Espectrometria de Massas em Tandem , Análise de Dados
13.
Artigo em Inglês | MEDLINE | ID: mdl-38252582

RESUMO

Nowadays, Deepfake videos are widely spread over the Internet, which severely impairs the public trustworthiness and social security. Although more and more reliable detectors have recently sprung up for resisting against that new-emerging tampering technique, some challengeable issues still need to be addressed, such that most of Deepfake video detectors under the framework of the supervised mechanism require a large scale of samples with accurate labels for training. When the amount of the training samples with the true labels are not enough or the training data are maliciously poisoned by adversaries, the supervised classifier is probably not reliable for detection. To tackle that tough issue, it is proposed to design a fully unsupervised Deepfake detector. In particular, in the whole procedure of training or testing, we have no idea of any information about the true labels of samples. First, we novelly design a pseudo-label generator for labeling the training samples, where the traditional hand-crafted features are used to characterize both types of samples. Second, the training samples with the pseudo-labels are fed into the proposed enhanced contrastive learner, in which the discriminative features are further extracted and continually refined by iteration on the guidance of the contrastive loss. Last, relying on the inter-frame correlation, we complete the final binary classification between real and fake videos. A large scale of experimental results empirically verify the effectiveness of our proposed unsupervised Deepfake detector on the benchmark datasets including FF++, Celeb-DF, DFD, DFDC, and UADFV. Furthermore, our proposed well-performed detector is superior to the current unsupervised method, and comparable to the baseline supervised methods. More importantly, when facing the problem of the labeled data poisoned by malicious adversaries or insufficient data for training, our proposed unsupervised Deepfake detector performs its powerful superiority. Our source codes have been released at https://github.com/bestalllen/Unsupervised_DF_Detection/.

14.
Chemosphere ; 350: 141120, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38199502

RESUMO

Salt stress profoundly impacts sweetpotato production. Exogenous glutathione (GSH) and melatonin (MT) promoted plant growth under stress, but their specific roles and mechanisms in sweetpotato salt tolerance need exploration. This study investigated GSH and MT's regulatory mechanisms in sweetpotato under salt stress. Salt stress significantly reduces both growth and biomass by hindering photosynthesis, root traits, K+ content, and K+/Na+ balance, leading to oxidative stress and excessive hydrogen peroxide (H2O2), superoxide ion (O2•-), and malondialdehyde (MDA) production and Na+ accumulation. Nevertheless, GSH (2 mM) and MT (25 µM) pre-treatments effectively mitigated salt-induced oxidative damage and protected the plasma membrane. They reduced osmotic pressure by enhancing K+ uptake, K+/Na+ regulation, osmolyte accumulation, and reducing Na+ accumulation. Improved stomatal traits, chloroplast and grana lamella preservation, and maintenance of mesophyll cells, cell wall, and mitochondrial structure were observed with GSH and MT pre-treatments under salt stress, therefore boosting the photosynthetic system and enhancing plant growth and biomass. Moreover, the findings also indicate that the positive outcomes of GSH and MT pre-treatments result from elevated antioxidant levels, enhanced enzymatic activity, and upregulated expression of sodium hydrogen exchanger 2 (NHX2), K+transporter 1 (AKT1), and cation/H+exchanger (CHX), CBL-interacting protein kinase 1 (CIPK1), and antioxidant enzyme genes. These mechanisms enhance structural stability in photosynthesis and reduce salt stress. Evidently, MT pre-treatment exhibited superior effects compared to GSH. These findings provide a firm theoretical basis for employing GSH and MT to enhance salt tolerance in sweetpotato cultivation.


Assuntos
Melatonina , Melatonina/metabolismo , Antioxidantes/metabolismo , Espécies Reativas de Oxigênio/farmacologia , Tolerância ao Sal , Peróxido de Hidrogênio/metabolismo , Glutationa/metabolismo , Fotossíntese
15.
Small ; 20(14): e2308473, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-37972267

RESUMO

Decorating platinum (Pt) with a single atom offers a promising approach to tailoring their catalytic activity. In this study, for the first time, an innovative assistive active sites (AAS) strategy is proposed to construct high-loading (3.46wt.%) single Fe─N4 as AAS, which are further hybridized with small Pt nanoparticles to enhance both oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activities. For ORR, the target catalyst (Pt/HFeSA-HCS) exhibits a higher mass activity (MA) of 0.98 A mgPt -1 and specific activity (SA) of 1.39 mA cmPt -2 at 0.90 V versus RHE. As for MOR, Pt/HFeSA-HCS shows exceptional MA (3.21 A mgPt -1) and SA (4.27 mA cmPt -2) at peak values, surpassing commercial Pt/C by 15.3 and 11.5 times, respectively. The underlying mechanism behind this AAS strategy is to find that in MOR, Fe─N4 promotes water dissociation, generating more *OH to accelerate the conversion of *CO to CO2. Meanwhile, in ORR, Fe─N4 acts as a competitor to adsorb *OH, weakening Pt─OH bonding and facilitating desorption of *OH on the Pt surface. Constructing AAS that can enhance dual functionality simultaneously can be seen as a successful "kill two birds with one stone" strategy.

16.
Environ Sci Pollut Res Int ; 31(1): 1576-1588, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-38048003

RESUMO

Extensive coral bleaching events can result in catastrophic degradation of coral reefs and reorganization of coral communities. In the present study, we analyzed the spatial differences in coral bleaching and possible reasons of large-scale coral bleaching, based on the results of a survey carried out in the northern South China Sea in 2020. In addition, we have continuously monitored the sea surface temperature (SST) of the northernmost Weizhou Island for more than six years. The living coral cover at Weizhou Island (W), Xuwen Nature Reserve (X), and Haihua Island (H) was relatively high at 24.6% ± 4.8%, 12.1% ± 3.8%, and 8.1% ± 2.6%, respectively, whereas their bleaching rates were 9.7% ± 2.6%, 9.7% ± 3.3%, and 6.9% ± 2.1%, respectively. Among them, the living coral cover of W was significantly different from those of X and H, whereas the bleaching rate was not significantly different among the three areas. In all three areas, the massive and encrusting corals predominate and exhibit relatively high bleaching rates, with Porites lutea and Bernardpora stutchburyi being the dominant species. In addition, the temperature monitoring results of Weizhou Island for six consecutive years showed that the critical SST of coral bleaching was 31.5 ℃. The monitoring results also showed that the average SST of Weizhou Island was 32.1 ℃, exceeding 32 ℃ in July 2020 for up to 533 h. The longest continuous time when the SST exceeded 32 ℃ was 97 h. These findings indicated that the coral bleaching event that occurred in the Beibu Gulf during 2020 was a large-scale and high-temperature transient event that presented a relatively homogeneous threat to the coral communities. We inferred that this sudden heat stress event was caused by the enclosed tidal current in the Beibu Gulf, which prevented the southern upwelling from reaching the north, as well as by the inability of the SST to decrease without rainfall caused by typhoon cyclones. Our findings suggested that abnormal heat waves can result in coral bleaching at high latitudes and even coral reef degradation. Furthermore, our study provides a new perspective for investigating the self-recovery and reorganization of coral communities following accumulated coral bleaching.


Assuntos
Antozoários , Recifes de Corais , Animais , Temperatura , Clima , China
17.
Chemistry ; 30(7): e202302520, 2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-37877456

RESUMO

Triplet-triplet annihilation upconversion (TTA-UC) has the potential to enhance photoredox catalysis yield. It includes a sensitizer and an annihilator. Efficient and stable annihilators are essential for photoredox catalysis, yet only a few examples are reported. Herein, we designed four novel pyrene annihilators (1, 2, 3 and 4) via introducing aryl-alkynyl groups onto pyrene to systematically modulate their singlet and triplet energies. Coupled with platinum octaethylporphyrin (PtOEP), the TTA-UC efficiency is enhanced gradually as the number of aryl-alkynyl group increases. When combining 4 with palladium tetraphenyl-tetrabenzoporphyrin (PdTPTBP), we achieved the highest red-to-green upconversion efficiency (22.4±0.3 %) (out of a 50 % maximum) so far. Then, this pair was used to activate photooxidation of aryl boronic acid under red light (630 nm), which achieved a great improved reaction yield compared to that activated by green light directly. The results not only provide a design strategy for efficient annihilators, but also show the advantage of applying TTA-UC into improving the photoredox catalysis yield.

18.
Small ; 20(21): e2309202, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38100237

RESUMO

Histone deacetylases (HDACs) are a class of epigenetic enzymes that are closely related to tumorigenesis and suppress the expression of tumor suppressor genes. Whereas the HDACs inhibitors can release DNA into the cytoplasm and trigger innate immunity. However, the high density of chromatin limits DNA damage and release. In this study, suitable nanosized CycNHOH NPs (150 nm) and CypNHOH NPs (85 nm) efficiently accumulate at the tumor site due to the enhanced permeability and retention (EPR) effect. In addition, robust single-linear oxygen generation and good photothermal conversion efficiency under NIR laser irradiation accelerated the DNA damage process. By effectively initiating immune cell death, CypNHOH NPs activated both innate and adaptive immunity by maturing dendritic cells, infiltrating tumors with natural killer cells, and activating cytotoxic T lymphocytes, which offer a fresh perspective for the development of photo-immunotherapy.


Assuntos
Epigênese Genética , Imunoterapia , Raios Infravermelhos , Nanopartículas , Neoplasias , Imunoterapia/métodos , Epigênese Genética/efeitos dos fármacos , Nanopartículas/química , Animais , Neoplasias/terapia , Fototerapia/métodos , Humanos , Morte Celular/efeitos dos fármacos , Camundongos , Linhagem Celular Tumoral
19.
Environ Res ; 239(Pt 2): 117406, 2023 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-37839529

RESUMO

The growing global concern about environmental threats due to environmental pollution requires the development of environmentally friendly and efficient removal/detection materials and methods. Porphyrin/phthalocyanine (Por/Pc) based porous organic polymers (POPs) as a newly emerging porous material are prepared through polymerizing building blocks with different structures. Benefiting from the high porosity, adjustable pore structure, and enzyme-like activities, the Por/Pc-POPs can be the ideal platform to study the removal and detection of pollutants. However, a systematic summary of their application in environmental treatment is still lacking to date. In this review, the development of various Por/Pc-POPs for pollutant removal and detection applications over the past decade was systematically addressed for the first time to offer valuable guidance on environmental remediation through the utilization of Por/Pc-POPs. This review is divided into two sections (pollutants removal and detection) focusing on Por/Pc-POPs for organic, inorganic, and gaseous pollutants adsorption, photodegradation, and chemosensing, respectively. The related removal and sensing mechanisms are also discussed, and the methods to improve removal and detection efficiency and selectivity are also summarized. For the future practical application of Por/Pc-POPs, this review provides the emerging research directions and their application possibility and challenges in the removal and detection of pollutants.


Assuntos
Poluentes Ambientais , Porfirinas , Poluentes Ambientais/química , Porosidade , Polímeros/química
20.
Heliyon ; 9(10): e20518, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37790962

RESUMO

Fragile karst areas of Guangxi are the key areas of vegetation protection and restoration work of the government. It is of great significance to study the effects of meteorological disasters on vegetation change for disaster prevention and reduction and ecological protection in the karst areas. The Normalized Differential Vegetation Index (NDVI), as a tool for monitoring vegetation growth, has a strong responsiveness to vegetation and can qualitatively and quantitatively evaluate the vegetation cover and its growth vitality. Therefore, in this study, we analyzed the trend of vegetation change and the impacts of multiple meteorological hazards, such as drought, torrential rainfall, high temperature, and low temperature, on the vegetation of the karst region in Guangxi by using the linear trend method, GIS spatial analysis, and correlation analysis, using the MODIS NDVI and temperature and precipitation information from 2000 to 2020 in the karst region of Guangxi. The results show that: (1) NDVI increased significantly in the karst areas, and 32.2% of the areas had significant improvement in vegetation. The improvement was the most obvious mainly in the central part of the study area, while the vegetation degradation trend was obvious in partial scattered areas in northeast and southwest. (2) On the interannual scale, NDVI was negatively correlated with some meteorological disaster indexes, such as relative humidity index, the number of drought days, the amount of extremely heavy rainstorm, the amount of heavy rainstorm, the number of days with high temperature of ≥35 °C, the number of days with high temperature of 35-37 °C, the number of days with high temperature of ≥37 °C, the minimum temperature, and the effective accumulated temperature of ≤0 °C. The obvious negative effect area of drought on vegetation was mainly concentrated in the middle of the study area, and that of rainfall was mainly distributed in the southwest, northeast and northwest; that of high temperature was mainly distributed in the northwest and northeast, and that of low temperature was mainly concentrated in the southwest and north. (3) On the multi-year monthly scale, the responses of NDVI to drought, high temperature and low temperature disaster indexes had a lag effect, but had no lag effect on rainfall disaster indexes. The lag time of vegetation to drought was 1 month, and the lag time to high temperature and low temperature was 3 months.

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