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1.
Sci Rep ; 14(1): 10531, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38719880

RESUMO

This study aims to explore the optimal driving speed for ground vibration in suburban railway underground sections. We focused on the ground surface of suburban railway underground sections and developed a 3D finite element dynamic coupling model for the tunnel-soil system. Subsequently, considering factors such as train speed and passenger load, we analyzed the propagation characteristics of ground vibration responses in urban railway underground sections. The research results indicate a significant amplification phenomenon in the peak power spectrum of measurement points near the tunnels in underground sections. The high-frequency components of the power spectrum between measurement points are noticeably higher between the two tunnels. Furthermore, as the train speed increases, this amplification phenomenon becomes more pronounced, and the power spectrum of each measurement point mainly concentrates on several frequency bands, with the amplitude of the power spectrum near the prominent frequencies also increasing. However, when the train speed is between 100 and 120 km/h, the impact on the amplitude of the power spectrum at measurement points above the running tunnel is minimal. Additionally, the amplitude of the middle-to-high frequency components in the power spectrum increases with the increase in passenger numbers. The impact on the peak acceleration amplitude at each measurement point is minimal when the train speed is 80 km/h or below. However, once the train speed exceeds 80 km/h, the peak acceleration amplitude above the running tunnel rapidly increases, reaching its maximum value at 113 km/h, and then gradually decreasing.

2.
Sci Rep ; 14(1): 10754, 2024 05 10.
Artigo em Inglês | MEDLINE | ID: mdl-38730229

RESUMO

Despite the critical role of self-disturbance in psychiatric diagnosis and treatment, its diverse behavioral manifestations remain poorly understood. This investigation aimed to elucidate unique patterns of self-referential processing in affective disorders and first-episode schizophrenia. A total of 156 participants (41 first-episode schizophrenia [SZ], 33 bipolar disorder [BD], 44 major depressive disorder [MDD], and 38 healthy controls [HC]) engaged in a self-referential effect (SRE) task, assessing trait adjectives for self-descriptiveness, applicability to mother, or others, followed by an unexpected recognition test. All groups displayed preferential self- and mother-referential processing with no significant differences in recognition scores. However, MDD patients showed significantly enhanced self-referential recognition scores and increased bias compared to HC, first-episode SZ, and BD. The present study provides empirical evidence for increased self-focus in MDD and demonstrates that first-episode SZ and BD patients maintain intact self-referential processing abilities. These findings refine our understanding of self-referential processing impairments across psychiatric conditions, suggesting that it could serve as a supplementary measure for assessing treatment response in first-episode SZ and potentially function as a discriminative diagnostic criterion between MDD and BD.


Assuntos
Transtorno Bipolar , Transtorno Depressivo Maior , Esquizofrenia , Psicologia do Esquizofrênico , Autoimagem , Humanos , Feminino , Masculino , Adulto , Esquizofrenia/fisiopatologia , Transtorno Bipolar/psicologia , Transtorno Bipolar/fisiopatologia , Transtorno Depressivo Maior/psicologia , Adulto Jovem , Estudos de Casos e Controles , Pessoa de Meia-Idade
3.
BMC Musculoskelet Disord ; 25(1): 368, 2024 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-38730497

RESUMO

BACKGROUND: This systemic review and meta-analysis aimed to evaluate the clinical outcomes of proximal humeral fracture in elderly patient fixation using locked plate with or without cement augmentation. METHODS: The databases of PubMed, Embase, and Cochrane Library were searched in August 2023 for literature comparing the clinical outcomes of patients with PHFs treated with locked plate alone and locked plate augmented with cement. Data describing study design; level of evidence; inclusion criteria; demographic information; final follow-up; revision rate; implant failure rate; avascular necrosis rate; total complication rate; constant score; and disability of arm, shoulder, and hand (DASH) score were collected. RESULTS: Eight studies (one randomized-controlled trial and seven observational studies), involving 664 patients, were identified. Compared with locked plates alone, using cement-augmented locked plates reduced the implant failure rate (odds ratio (OR) = 0.19; 95% confidence interval (CI) 0.10-0.39; P < 0.0001) and total complication rate (OR = 0.45; 95% CI 0.29-0.69; P = 0.0002) and improved DASH scores (mean difference (MD) = 2.99; 95% CI 1.00-4.98; P = 0.003). However, there was no significant difference in clinical outcomes, including revision rate, avascular necrosis rate, and constant score. CONCLUSION: In this review and meta-analysis, fixation of the PHFs in elderly patients using locked plates with or without cement augmentation has no significant difference in revision rate, but the implant failure and total complication rates may be lesser on using the cement-augmented locked plate for fixation than on using a locked plate alone. Good results are expected for most patients treated with this technique. TRIAL REGISTRATION: The Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA)21 guidelines were followed to conduct this systematic review and meta-analysis and was registered as a protocol in PROSPERO (CRD42022318798).


Assuntos
Cimentos Ósseos , Placas Ósseas , Fixação Interna de Fraturas , Fraturas do Ombro , Humanos , Fraturas do Ombro/cirurgia , Fraturas do Ombro/diagnóstico por imagem , Fixação Interna de Fraturas/instrumentação , Fixação Interna de Fraturas/métodos , Fixação Interna de Fraturas/efeitos adversos , Cimentos Ósseos/uso terapêutico , Cimentos Ósseos/efeitos adversos , Idoso , Resultado do Tratamento , Idoso de 80 Anos ou mais , Complicações Pós-Operatórias/etiologia , Complicações Pós-Operatórias/epidemiologia , Reoperação
4.
Int J Biol Macromol ; : 132229, 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38734337

RESUMO

In this study, the effect of hydrothermal treatment with different temperatures (120-180 °C) on the rheological properties of xanthan gum was evaluated. When the temperature of hydrothermal treatment was relatively low (120 °C), the rheological properties of the hydrothermally treated xanthan gum was similar to the untreated xanthan gum (pseudoplastic and solid-like/gel-like behavior). However, as the temperature of hydrothermal treatment was higher, the rheological properties of the hydrothermally treated xanthan gum changed greatly (e.g., a wider range of Newtonian plateaus in flow curves, existence of a critical frequency between the storage modulus (G') and the loss modulus (G") in the dynamic viscoelasticity measurement, variation of complex viscosity). Although the hydrothermal treatment showed little influence on the functional groups of xanthan gum, it altered the micromorphology of xanthan gum from uneven and rough lump-like to thinner and smoother flake-like. In addition, higher concentration (2 %) of hydrothermally treated xanthan gum made its viscosity close to that of the untreated xanthan gum (1 %). Besides, hydrothermal treatment also affected the effect of temperature and salt (CaCl2) adding on the rheological properties of xanthan gum. Overall, this study can provide some useful information on the rheological properties of xanthan gum after hydrothermal treatment.

5.
J Hazard Mater ; 472: 134566, 2024 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-38743973

RESUMO

Three-dimensional separation materials with robust physical/chemical stability have great demand for effective and continuous separation of immiscible oil/water mixtures and water-in-oil emulsions, resulting from chemical leakages and discharge of industrial oily wastewaters. Herein, a superelastic polystyrene-based porous material with superhydrophobicity/superoleophilicity was designed and prepared by high internal phase emulsion polymerization to meet the aforementioned requirements. A flexible and hydrophobic aminopropyl terminated polydimethylsiloxane (NH2-PDMS-NH2) segment was introduced into the rigid styrene-divinylbenzene copolymer through 1, 4-conjugate addition reaction with trimethylolpropane triacrylate. The addition of NH2-PDMS-NH2 simultaneously improved the mechanical and hydrophobic properties of the porous material (the water contact angle from 141.2° to 152.2°). The material exhibited outstanding reversible compressibility (80% strain, even in liquid N2 environments) and superhydrophobic stability, even after being repeatedly compressed 100 times, water contact angle still remained above 150°. Meanwhile, the as-prepared material had outstanding hydrophobic stability in corrosive solutions (strong acidic, alkaline, high-salty, and even strong polar solvent), presence of mechanical interference, strong UV radiations, and high/low temperature environments. More importantly, the material could continuously and efficiently separate immiscible oil/water mixture and water-in-oil emulsions under the above conditions, showing huge potential for the large-scale remediation of complex oily wastewaters.

6.
J Agric Food Chem ; 72(19): 10995-11001, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38701424

RESUMO

The titer of the microbial fermentation products can be increased by enzyme engineering. l-Sorbosone dehydrogenase (SNDH) is a key enzyme in the production of 2-keto-l-gulonic acid (2-KLG), which is the precursor of vitamin C. Enhancing the activity of SNDH may have a positive impact on 2-KLG production. In this study, a computer-aided semirational design of SNDH was conducted. Based on the analysis of SNDH's substrate pocket and multiple sequence alignment, three modification strategies were established: (1) expanding the entrance of SNDH's substrate pocket, (2) engineering the residues within the substrate pocket, and (3) enhancing the electron transfer of SNDH. Finally, mutants S453A, L460V, and E471D were obtained, whose specific activity was increased by 20, 100, and 10%, respectively. In addition, the ability of Gluconobacter oxidans WSH-004 to synthesize 2-KLG was improved by eliminating H2O2. This study provides mutant enzymes and metabolic engineering strategies for the microbial-fermentation-based production of 2-KLG.


Assuntos
Proteínas de Bactérias , Proteínas de Bactérias/genética , Proteínas de Bactérias/metabolismo , Proteínas de Bactérias/química , Gluconobacter/enzimologia , Gluconobacter/genética , Gluconobacter/metabolismo , Açúcares Ácidos/metabolismo , Açúcares Ácidos/química , Fermentação , Engenharia de Proteínas , Engenharia Metabólica , Desidrogenases de Carboidrato/metabolismo , Desidrogenases de Carboidrato/genética , Desidrogenases de Carboidrato/química , Cinética
7.
Nat Prod Bioprospect ; 14(1): 29, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38740677

RESUMO

A catalytic diastereoselective Prins reaction for hydroxymethylation and hydroxylation of 1,3-diarylpropene was successfully utilized to prepare various 1,3-dioxanes 7 in 14-88% yields. Take advantage of the synthetic intermediate 7h, the key B/C rings in brazilin core could be constructed by the sequential of Friedel-Crafts/Ullmann-Ma rather than Ullmann-Ma/Friedel-Crafts reactions.

8.
Virology ; 595: 110091, 2024 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-38718446

RESUMO

Preliminary investigations have demonstrated that the cysteines located at the C-terminus of HEV ORF2 protein exhibits disulfide bonding capability during virus-like particles (VLPs) assembly. However, the effect and mechanism underlying the pairing of disulfide bonds formed by C627, C630, and C638 remains unclear. The p222 protein encompasses C-terminus and serves as a representative of HEV ORF2 to investigate the specific impacts of C627, C630, and C638. The three cysteines were subjected to site-directed mutagenesis and expressed in prokaryotes; Both the mutated proteins and p222 underwent polymerization except for p222A; Surprisingly, only p222 was observed as abundant spherical particles under transmission electron microscope (TEM); Stability and immunogenicity of the p222 exhibited higher than other mutated proteins; LC/MS/MS analysis identified four disulfide bonds in the p222. The novel findings suggest that the three cysteines contribute to structural and functional properties of ORF2 protein, highlighting the indispensability of each cysteine.

9.
Cell Biochem Biophys ; 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38713401

RESUMO

OBJECTIVE: Panax quinquefolius saponins (PQS) and Panax notoginseng saponins (PNS) are key bioactive compounds in Panax quinquefolius L. and Panax notoginseng, commonly used in the treatment of clinical ischemic heart disease. However, their potential in mitigating myocardial ischemia-reperfusion injury remains uncertain. This study aims to evaluate the protective effects of combined PQS and PNS administration in myocardial hypoxia/reoxygenation (H/R) injury and explore the underlying mechanisms. METHODS: To investigate the involvement of HIF-1α/BNIP3 mitophagy pathway in the myocardial protection conferred by PNS and PQS, we employed small interfering BNIP3 (siBNIP3) to silence key proteins of the pathway. H9C2 cells were categorized into four groups: control, H/R, H/R + PQS + PNS, and H/R + PQS + PNS+siBNIP3. Cell viability was assessed by Cell Counting Kit-8, apoptosis rates determined via flow cytometry, mitochondrial membrane potential assessed with the JC-1 fluorescent probes, intracellular reactive oxygen species detected with 2',7'-dichlorodihydrofluorescein diacetate, mitochondrial superoxide production quantified with MitoSOX Red, and autophagic flux monitored with mRFP-GFP-LC3 adenoviral vectors. Autophagosomes and their ultrastructure were visualized through transmission electron microscopy. Moreover, mRNA and protein levels were analyzed via real-time PCR and Western blotting. RESULTS: PQS + PNS administration significantly increased cell viability, reduced apoptosis, lowered reactive oxygen species levels and mitochondrial superoxide production, mitigated mitochondrial dysfunction, and induced autophagic flux. Notably, siBNIP3 intervention did not counteract the cardioprotective effect of PQS + PNS. The PQS + PNS group showed downregulated mRNA expression of HIF-1α and BNIP3, along with reduced HIF-1α protein expression compared to the H/R group. CONCLUSIONS: PQS + PNS protects against myocardial H/R injury, potentially by downregulating mitophagy through the HIF-1α/BNIP3 pathway.

10.
Nat Commun ; 15(1): 3782, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38710678

RESUMO

Thermoelectrics have great potential for use in waste heat recovery to improve energy utilization. Moreover, serving as a solid-state heat pump, they have found practical application in cooling electronic products. Nevertheless, the scarcity of commercial Bi2Te3 raw materials has impeded the sustainable and widespread application of thermoelectric technology. In this study, we developed a low-cost and earth-abundant PbS compound with impressive thermoelectric performance. The optimized n-type PbS material achieved a record-high room temperature ZT of 0.64 in this system. Additionally, the first thermoelectric cooling device based on n-type PbS was fabricated, which exhibits a remarkable cooling temperature difference of ~36.9 K at room temperature. Meanwhile, the power generation efficiency of a single-leg device employing our n-type PbS material reaches ~8%, showing significant potential in harvesting waste heat into valuable electrical power. This study demonstrates the feasibility of sustainable n-type PbS as a viable alternative to commercial Bi2Te3, thereby extending the application of thermoelectrics.

11.
Small ; : e2400408, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38709208

RESUMO

Stent-assisted coiling is a main treatment modality for intracranial aneurysms (IAs) in clinics, but critical challenges remain to be overcome, such as exogenous implant-induced stenosis and reliance on antiplatelet agents. Herein, an endovascular approach is reported for IA therapy without stent grafting or microcatheter shaping, enabled by active delivery of thrombin (Th) to target aneurysms using innovative phase-change material (PCM)-coated magnetite-thrombin (Fe3O4-Th@PCM) FTP nanorobots. The nanorobots are controlled by an integrated actuation system of dynamic torque-force hybrid magnetic fields. With robust intravascular navigation guided by real-time ultrasound imaging, nanorobotic collectives can effectively accumulate and retain in model aneurysms constructed in vivo, followed by controlled release of the encapsulated Th for rapid occlusion of the aneurysm upon melting the protective PCM (thermally responsive in a tunable manner) through focused magnetic hyperthermia. Complete and stable aneurysm embolization is confirmed by postoperative examination and 2-week postembolization follow-up using digital subtraction angiography (DSA), contrast-enhanced ultrasound (CEUS), and histological analysis. The safety of the embolization therapy is assessed through biocompatibility evaluation and histopathology assays. This strategy, seamlessly integrating secure drug packaging, agile magnetic actuation, and clinical interventional imaging, avoids possible exogenous implant rejection, circumvents cumbersome microcatheter shaping, and offers a promising option for IA therapy.

12.
Int J Biol Macromol ; : 131831, 2024 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-38702246

RESUMO

Lately, emulsions with low-fat and natural stabilizers are predominant. This study extracted the nano cellulose crystals (NCs) from Camellia Oleifera shells, and their gallic acid (GA) conjugates were synthesized by free-radical grafting. Pickering emulsions were prepared using NCs 1 %, 1.5 %, 2.5 %, and gallic acid conjugates NC-GA1, NC-GA2, and NC-GA3 as stabilizers. The obtained nano cellulose crystals exhibited 18-25 nm, -40.01 ±â€¯2.45 size, and zeta potential, respectively. The contact angle of 83.4° was exhibited by NC-GA3 conjugates. The rheological, interfacial, and microstructural properties and stability of the Pickering emulsion were explored. NC-GA3 displayed the highest absorption content of 79.12 %. Interfacial tension was drastically reduced with increasing GA concentration in NC-GA conjugates. Rheological properties suggested that the low-fat NC-GA emulsions showed a viscoelastic behavior, increased viscosity, gel-like structure, and increased antioxidant properties. Moreover, NC-GA3 displayed reduced droplet size and improved emulsion temperature and storage stability (28 days) against phase separation. POV and TBARS values were reduced with the NC-GA3 (P < 0.05). This work confirmed that grafting phenolic compounds on NCs could enhance bioactive properties, which can be used in developing low-fat functional foods. NC-GA conjugates can potentially fulfill the increasing demand for sustainable, healthy, and low-fat foods.

14.
Neurol Clin Pract ; 14(3): e200228, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38690148

RESUMO

Objectives: Heterozygous missense variants in MYBPC1 have been recently identified in 13 patients from 6 families with congenital myopathy with tremor. All the patients had mild skeletal myopathy invariably associated with a distinctive myogenic tremor and hypotonia with gradual clinical improvement. However, no phenotypic description has been reported for the neonatal respiratory impairment that patients may suffer. Methods: We report 3 new patients from 2 independent families with congenital myopathy with tremor. Results: Tremors and respiratory distress associated with stridor should raise the diagnosis of congenital myopathy with tremors linked to MYBPC1-dominant variants in children with neonatal hypotonia. Discussion: Neonatal severe respiratory impairment requiring intensive noninvasive ventilation because of stridor is described in 2 patients. Stridor was previously reported in one other case and is part of the clinical features.

15.
Int Immunopharmacol ; 134: 112234, 2024 May 12.
Artigo em Inglês | MEDLINE | ID: mdl-38739976

RESUMO

Ulcerative colitis, a chronic inflammatory condition affecting the rectum and colon to varying degrees, is linked to a dysregulated immune response and the microbiota. Sodium (aS,9R)-3-hydroxy-16,17-dimethoxy-15-oxidotricyclo[12.3.1.12,6]nonadeca-1(18),2,4,6(19),14,16-hexene-9-yl sulfate hydrate (SDH) emerges as a novel diarylheptane compound aimed at treating inflammatory bowel diseases. However, the mechanisms by which SDH modulates these conditions remain largely unknown. In this study, we assessed SDH's impact on the clinical progression of dextran sodium sulfate (DSS)-induced ulcerative colitis. Our results demonstrated that SDH significantly mitigated the symptoms of DSS-induced colitis, reflected in reduced disease activity index scores, alleviation of weight loss, shortening of the colorectum, and reduction in spleen swelling. Notably, SDH decreased the proportion of Th1/Th2/Th17 cells and normalized inflammatory cytokine levels in the colon. Furthermore, SDH treatment modified the gut microbial composition in mice with colitis, notably decreasing Bacteroidetes and Proteobacteria populations while substantially increasing Firmicutes, Actinobacteria, and Patescibacteria. In conclusion, our findings suggest that SDH may protect the colon from DSS-induced colitis through the regulation of Th1/Th2/Th17 cells and gut microbiota, offering novel insights into SDH's therapeutic potential.

16.
Adv Sci (Weinh) ; : e2402645, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38738739

RESUMO

The photocatalytic reduction of CO2 represents an environmentally friendly and sustainable approach for generating valuable chemicals. In this study, a thiophene-modified highly conjugated asymmetric covalent triazine framework (As-CTF-S) is developed for this purpose. Significantly, single-component intramolecular energy transfer can enhance the photogenerated charge separation, leading to the efficient conversion of CO2 to CO during photocatalysis. As a result, without the need for additional photosensitizers or organic sacrificial agents, As-CTF-S demonstrates the highest photocatalytic ability of 353.2 µmol g-1 and achieves a selectivity of ≈99.95% within a 4 h period under visible light irradiation. This study provides molecular insights into the rational control of charge transfer pathways for high-efficiency CO2 photoreduction using single-component organic semiconductor catalysts.

17.
Anal Chem ; 96(19): 7738-7746, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38690966

RESUMO

Telomerase is an important biomarker for early diagnosis of cancers, but current telomerase assays usually rely on measuring the extension products of telomerase substrates, which increases the assay complexity. More evidence indicates that human telomerase RNA (hTR), as a core component of telomerase, is positively correlated with the telomerase activity. Herein, we demonstrate the development of a duplex-specific nuclease (DSN)-propelled 3D quantum dot (QD) nanoassembly with two-step Föster resonance energy transfer (FRET) for the one-step sensing of hTR in breast cancer cells and tissues. This assay involves only one hairpin probe modified with a Cy5 at the sixth base from the 5'-biotin end and a BHQ2 at the 3'-terminus, which integrates three functions of target recognition, target recycling amplification, and signal readout. The anchoring of the hairpin probe on the 605QD surface results in the formation of a 3D 605QD-Cy5-probe-BHQ2 nanoassembly in which two-step FRET occurs among the 605QD, Cy5, and BHQ2 quencher. Notably, the formation of 605QD-Cy5-probe-BHQ2 nanoassembly facilitates the reduction of background signal and the increase of signal-to-background ratio due to its dense, highly oriented nucleic acid shell-induced steric hindrance effect. This assay can achieve one-step and rapid detection of hTR with a detection limit of 2.10 fM, which is the simplest and most rapid hTR assay reported so far. Moreover, this assay can efficiently distinguish single-base mismatched sequences, and it can discriminate the hTR level between breast cancer patients and healthy donors with a high accuracy of 100%, with great prospects for early diagnosis of cancers.


Assuntos
Neoplasias da Mama , Transferência Ressonante de Energia de Fluorescência , Pontos Quânticos , RNA , Telomerase , Humanos , Telomerase/metabolismo , Telomerase/análise , Pontos Quânticos/química , RNA/metabolismo , RNA/análise , Feminino , Carbocianinas/química , Técnicas Biossensoriais/métodos
18.
Inorg Chem ; 63(19): 8948-8957, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38687980

RESUMO

Excellent electrocatalytic CO2 reduction reaction activity has been demonstrated by transition metals and nitrogen-codoped carbon (M-N-C) catalysts, especially for transition-metal porphyrin (MTPP)-based catalysts. In this work, we propose to use one-step low-temperature pyrolysis of the isostructural MTPP-based metal-organic frameworks (MOFs) and electrochemical in situ reduction strategies to obtain a series of hybrid catalysts of Co nanoparticles (Co NPs) and MTPP, named Co NPs/MTPP (M = Fe, Co, and Ni). The in situ introduction of Co NPs can efficiently enhance the electrocatalytic ability of MTPP (M = Fe, Co, and Ni) to convert CO2 to CO, particularly for FeTPP. Co NPs/FeTPP endowed a high CO faradaic efficiency (FECOmax = 95.5%) in the H cell, and the FECO > 90.0% is in the broad potential range of -0.72 to -1.22 VRHE. In addition, the Co NPs/FeTPP achieved 145.4 mA cm-2 at a lower potential of -0.70 VRHE with an FECO of 94.7%, and the CO partial currents increased quickly to reach 202.2 mA cm-2 at -0.80 VRHE with an FECO of 91.6% in the flow cell. It is confirmed that Co NPs are necessary for hybrid catalysts to get superior electrocatalytic activity; Co NPs also can accelerate H2O dissociation and boost the proton supply capacity to hasten the proton-coupled electron-transfer process, effectively adjusting the adsorption strength of the reaction intermediates.

19.
Nat Commun ; 15(1): 3295, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38632230

RESUMO

Van der Waals semiconductors exemplified by two-dimensional transition-metal dichalcogenides have promised next-generation atomically thin optoelectronics. Boosting their interaction with light is vital for practical applications, especially in the quantum regime where ultrastrong coupling is highly demanded but not yet realized. Here we report ultrastrong exciton-plasmon coupling at room temperature in tungsten disulfide (WS2) layers loaded with a random multi-singular plasmonic metasurface deposited on a flexible polymer substrate. Different from seeking perfect metals or high-quality resonators, we create a unique type of metasurface with a dense array of singularities that can support nanometre-sized plasmonic hotspots to which several WS2 excitons coherently interact. The associated normalized coupling strength is 0.12 for monolayer WS2 and can be up to 0.164 for quadrilayers, showcasing the ultrastrong exciton-plasmon coupling that is important for practical optoelectronic devices based on low-dimensional semiconductors.

20.
J Colloid Interface Sci ; 666: 66-75, 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-38583211

RESUMO

Perovskite CsPbBr3 quantum dot shows great potential in artificial photosynthesis, attributed to its outstanding optoelectronic properties. Nevertheless, its photocatalytic activity is hindered by insufficient catalytic active sites and severe charge recombination. In this work, a CsPbBr3@Ag-C3N4 ternary heterojunction photocatalyst is designed and synthesized for high-efficiency CO2 reduction. The CsPbBr3 quantum dots and Ag nanoparticles are chemically anchored on the surface of g-C3N4 sheets, forming an electron transfer tunnel from CsPbBr3 quantum dots to Ag nanoparticles via g-C3N4 sheets. The resulting CsPbBr3@Ag-C3N4 ternary photocatalyst, with spatial separation of photogenerated carriers, achieves a remarkable conversion rate of 19.49 µmol·g-1·h-1 with almost 100 % CO selectivity, a 3.13-fold enhancement in photocatalytic activity as compared to CsPbBr3 quantum dots. Density functional theory calculations reveal the rapid CO2 adsorption/activation and the decreased free energy (0.66 eV) of *COOH formation at the interface of Ag nanoparticles and g-C3N4 in contrast to the g-C3N4, leading to the excellent photocatalytic activity, while the thermodynamically favored CO desorption contributes to the high CO selectivity. This work presents an innovative strategy of constructing perovskite-based photocatalyst by modulating catalyst structure and offers profound insights for efficient CO2 conversion.

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