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1.
Adv Mater ; : e2400059, 2024 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-38684087

RESUMO

Materials that can provide reliable electromagnetic interference (EMI) shielding in highly oxidative atmosphere at elevated temperature are indispensable in the fast-developing aerospace field. However, most of conductor-type EMI shielding materials such as metals can hardly withstand the high-temperature oxidation, while the conventional dielectric-type materials cannot offer sufficient shielding efficiency in gigahertz (GHz) frequencies. Here, a highly deficient medium-entropy (ME) perovskite ceramic as an efficient EMI shielding material in harsh environment, is demonstrated. The synergistic effect of entropy stabilization and aliovalent substitution on A-site generate abnormally high concentration of Ti and O vacancies that are stable under high-temperature oxidation. Due to the clustering of vacancies, the highly deficient perovskite ceramic exhibits giant complex permittivity and polarization loss in GHz, leading to the specific EMI shielding effectiveness above 30 dB/mm in X-band even after 100 h of annealing at 1000 °C in air. Along with the low thermal conductivity, the aliovalent ME perovskite can serve as a bifunctional shielding material for applications in aircraft engines and reusable rockets.

2.
Sci Total Environ ; 929: 172406, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38642745

RESUMO

Little information is known regarding how the lagged pollution of polycyclic aromatic hydrocarbon (PAH) influenced the environment and human health after an e-waste dismantling site was rebuilt. This study investigated the characteristics, sources, and risk assessment of PAHs in a rebuilt e-waste site and its surrounding farmland by analyzing the samples of soil, dust, water, and vegetable. Concentrations of PAHs in soil, vegetable and water in the rebuilt site were relatively higher than in its surrounding farmland. The concentrations in surface soils, soil columns, dust, vegetables, and water varied from 55.4 to 3990 ng g-1, 1.65 to 5060 ng g-1, 2190 to 2420 ng g-1, 2670 to 10,300 ng g-1, and 46.8 to 110 µg L-1 in the e-waste site, respectively. On the farmland, PAH concentrations in surface soils, vegetables, and water ranged from 41.5 to 2760 ng g-1, 506 to 7640 ng g-1, and 56.6 to 89.2 µg L-1, respectively. A higher proportion of high-molecular-weight PAHs (HMW-PAHs) appeared in all multimedia compared with low-molecular-weight PAHs (LMW-PAHs). Diagnostic ratio together with positive matrix factorization (PMF) revealed that vehicle emission was the primary source in this area, and the activity of e-waste disposal was another important source in the rebuilt e-waste site. Based on the deterministic health risks, people working in the reconstructed e-waste site were exposed to low risks, whereas the residents living near the surrounding farmland were exposed to low risk. Sensitivity analyses indicated that exposure frequency and PAH concentrations were the main factors that influenced exposure risk. This study provides valuable insight into the comprehension of the lagging pollution effects of PAH on the environment and human health after the e-waste site was rebuilt.


Assuntos
Resíduo Eletrônico , Monitoramento Ambiental , Hidrocarbonetos Policíclicos Aromáticos , Poluentes do Solo , Hidrocarbonetos Policíclicos Aromáticos/análise , Medição de Risco , Resíduo Eletrônico/análise , Poluentes do Solo/análise , Humanos , Solo/química , China
3.
Proc Natl Acad Sci U S A ; 121(18): e2319751121, 2024 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-38662548

RESUMO

Defect engineering has been widely applied in semiconductors to improve photocatalytic properties by altering the surface structures. This study is about the transformation of inactive WO3 nanosheets to a highly effective CO2-to-CH4 conversion photocatalyst by introducing surface-ordered defects in abundance. The nonstoichiometric WO3-x samples were examined by using aberration-corrected electron microscopy. Results unveil abundant surface-ordered terminations derived from the periodic {013} stacking faults with a defect density of 20.2%. The {002} surface-ordered line defects are the active sites for fixation CO2, transforming the inactive WO3 nanosheets into a highly active catalyst (CH4: O2 = 8.2: 16.7 µmol h-1). We believe that the formation of the W-O-C-W-O species is a critical step in the catalytic pathways. This work provides an atomic-level comprehension of the structural defects of catalysts for activating small molecules.

4.
J Am Chem Soc ; 146(13): 9124-9133, 2024 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-38515273

RESUMO

Single-atom catalysis (SAC) attracts wide interest for zinc-air batteries that require high-performance bifunctional electrocatalysts for oxygen reactions. However, catalyst design is still highly challenging because of the insufficient driving force for promoting multiple-electron transfer kinetics. Herein, we report a superstructure-assisted SAC on tungsten carbides for oxygen evolution and reduction reactions. In addition to the usual single atomic sites, strikingly, we reveal the presence of highly ordered Co superstructures in the interfacial region with tungsten carbides that induce internal strain and promote bifunctional catalysis. Theoretical calculations show that the combined effects from superstructures and single atoms strongly reduce the adsorption energy of intermediates and overpotential of both oxygen reactions. The catalyst therefore presented impressive bifunctional activity with an ultralow potential gap of 0.623 V and delivered a high power density of 188.5 mW cm-2 for assembled zinc-air batteries. This work opens up new opportunities for atomic catalysis.

5.
Adv Mater ; 36(16): e2311937, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38191131

RESUMO

Hybridizing two heterocomponents to construct a built-in electric field (BIEF) at the interface represents a significant strategy for facilitating charge separation in carbon dioxide (CO2)-photoreduction. However, the unidirectional nature of BIEFs formed by various low-dimensional materials poses challenges in adequately segregating the photogenerated carriers produced in bulk. In this study, leveraging zinc oxide (ZnO) nanodisks, a sulfurization reaction is employed to fabricate Z-scheme ZnO/zinc sulfide (ZnS) heterojunctions featuring a multiple-order BIEF. These heterojunctions reveal distinctive interfacial structures characterized by two semicoherent phase boundaries. The cathodoluminescence 2D maps and density functional theory calculation results demonstrate that the direction of the multiple-order BIEF spans from ZnS to ZnO. This directional alignment significantly fosters the spatial separation of photogenerated electrons and holes within ZnS nanoparticles and enhances CO2-to-carbon monoxide photoreduction performance (3811.7 µmol h-1 g-1). The findings present a novel pathway for structurally designing BIEFs within heterojunctions, while providing fresh insights into the migratory behavior of photogenerated carriers across interfaces.

6.
PLoS One ; 19(1): e0296512, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38165985

RESUMO

The rapid increase in the number of older people under the background of population aging has gradually changed the disease spectrum of society, making aging diseases more prevalent, and increasing the demand for health care services, medical and health services, and health insurance among older people, ultimately leading to increasing household and social spending on old age. This study is conducted to assess the impact of those spending burden on the sustainable development of economy and find out some practical and effective solutions. This paper constructs a theoretical model to illustrate the relationship between the old-age dependency ratio and the marginal product of capital (MPK), and then establishes a two-way fixed effect model based on transnational panel data of 81 countries from 1981 to 2017 to verify this relationship empirically. This paper finds that, after controlling a series of variables, an increased burden of old-age dependency leads to a decline in the MPK, a key macroeconomic variable and also a sustainable development criteria, but in which health care, health security systems, and technological innovation play a key and moderating role. The conclusion is also valid after tackling the problem of endogeneity with different methods, like two-stage least squares (TSLS) and the generalized methods of moments (GMM). Overall, before population aging, countries that are old-but-not-rich should encourage more supply-side investments in public health system or technological innovation, and adjust retirement system, or gradually encourage childbearing to strive for time and space for later sustainable development of public health system and economy.


Assuntos
Administração Financeira , Desenvolvimento Sustentável , Humanos , Idoso , Dinâmica Populacional , Investimentos em Saúde , Características da Família
7.
Front Behav Neurosci ; 18: 1329638, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38292326

RESUMO

Background: Despite the increasing global prevalence of depression, existing treatment methods have limitations. Acupuncture has been recognized for its potential to alleviate various diseases by regulating inflammatory cytokines. However, a comprehensive systematic analysis of the effects of acupuncture on depression through inflammatory cytokines is currently lacking. This review aims to evaluate the impact of acupuncture on inflammatory cytokines in animal models of depression. Methods: A comprehensive search was conducted in PubMed, EMBASE, MEDLINE, and the Research Information Service System to identify studies that met predefined inclusion and exclusion criteria. The quality of each included study was assessed using a 10-item checklist adapted from the Cochrane Collaboration methods and animal data review. Meta-analysis was performed using STATA 17.0 software for literature that met the inclusion criteria. Results: The meta-analysis included a total of 21 studies involving 376 rodents. The overall quality of the included reports was rated as moderate or higher. The results demonstrated that acupuncture had a significant effect on the reduction of pro-inflammatory cytokines, including: IL-1ß [SMD = 3.36, 95% CI (2.73, 4.00), I2 = 73.3%, p < 0.05], IL-6 [SMD = 3.05, 95% CI (2.45, 3.64), I2 = 68%, p < 0.05], and TNF-α [SMD = 3.30, 95% CI (2.53, 4.06), I2 = 74.5%, p < 0.05]. Conversely, acupuncture was associated with an increased expression of anti-inflammatory cytokines, notably: IL-4 [SMD = -1.64, 95% CI (-2.46, -0.82), I2 = 4.1%, p = 0.307] and IL-10 [SMD = -1.45, 95% CI (-2.24, -0.66), I2 = 0, p = 0.678]. These results suggest that acupuncture modulates cytokine levels in depressed rodents, including reducing the expression of pro-inflammatory cytokines and increasing the expression of anti-inflammatory cytokines, thereby regulating the immune-related antidepressant pathway. Conclusion: While this study is limited by the number of included studies, the results suggest that acupuncture may be a viable option for the treatment of depression, and this effect is achieved through the regulation of various inflammatory cytokines. Systematic review registration: This research endeavor was duly registered with PROSPERO (ID: CRD42023420919, https://www.crd.york.ac.uk/PROSPERO/display_record.php?RecordID=420919).

8.
3D Print Addit Manuf ; 10(6): 1238-1250, 2023 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-38143713

RESUMO

Inspired by the potential of architected materials for achieving biomimicking functionalities and the advancement of multi-material additive manufacturing to fabricate parts with complex structures and heterogeneous material distributions, this study investigates the feasibility of using a multi-material, flexible chain mail sheet for the design of an additively manufactured artificial spinal disc for reproducing patient-specific anisotropic and nonlinear rotational behaviors. The application of a chain mail-based structure is motivated by its similarities in behaviors compared with a natural disc's fiber network that likewise has negligible bending stiffness and shape-changing ability. The proposed approach for the chain mail sheet design includes an initial characterization of the uniaxial tensile responses of the chain mail unit cell defined as the basic building block of the chain mail sheet, modeling and response calculation, and material optimization. Results show that the additively manufactured chain mail sheet is not only able to exhibit a natural strain-stiffening rotational response but also is able to reproduce natural anisotropy of three natural disc specimens in the six most common rotational scenarios in daily life. This study shows the potential of additively manufactured mechanical-metamaterials-inspired structures for implant design to restore natural mechanics.

9.
Adv Mater ; 35(52): e2309413, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37950585

RESUMO

X-ray imaging plays an increasingly crucial role in clinical radiography, industrial inspection, and military applications. However, current X-ray imaging technologies have difficulty in protecting against information leakage caused by brute force attacks via trial-and-error. Here high-confidentiality X-ray imaging encryption by fabricating ultralong radioluminescence memory films composed of lanthanide-activated nanoscintillators (NaLuF4 : Gd3+ or Ce3+ ) with imperceptible purely-ultraviolet (UV) emission is reported. Mechanistic investigations unveil that ultralong X-ray memory is attributed to the long-lived trapping of thermalized charge carriers within Frenkel defect states and subsequent slow release in the form of imperceptible radioluminescence. The encrypted X-ray imaging can be securely stored in the memory film for more than 7 days and optically decoded by perovskite nanocrystal. Importantly, this encryption strategy can protect X-ray imaging information against brute force trial-and-error attacks through the perception of lifetime change in the persistent radioluminescence. It is further demonstrated that the as-fabricated flexible memory film enables achieving of 3D X-ray imaging encryption of curved objects with a high spatial resolution of 20 lp/mm and excellent recyclability. This study provides valuable insights into the fundamental understanding of X-ray-to-UV conversion in nanocrystal lattices and opens up a new avenue toward the development of high-confidential 3D X-ray imaging encryption technologies.

10.
Food Chem X ; 20: 100904, 2023 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-37817988

RESUMO

This study investigated the effect of electron beam irradiation (EBI) on the lipid stability of oat and barley during long-term storage. Results showed that the initial free fatty acid content in oat was higher than that in barley. This may mean that lipid hydrolysis started under the function of lipase when oat and barley were milled into flours. Both storage and EBI factors influenced lipid-degrading enzyme activity and promoted lipid oxidation in oat and barley. However, it seemed that storage had higher impacts because the DPPH scavenging activity decreased greatly, and the contents of both malondialdehyde and volatile lipid oxidation products increased in all samples. Thus, the antioxidant capacity and level of lipid oxidation after EBI treatment should be considered when producing oat and barley foods. Overall, this study shows the high potential of EBI for use as a non-thermal technique in stabilising the storage quality of oat and barley.

11.
Sci Total Environ ; 905: 167166, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-37730034

RESUMO

Bisphenol S (BPS), being structurally similar to bisphenol A (BPA), has been widely used as an alternative to BPA in industrial applications. However, in-depth studies on the environmental behavior and fate of BPS in various soils have been rarely reported. Here, 14C-labeled BPS was used to investigate its mineralization, bound residues (BRs) formation and extractable residues (ERs) in three soils for 64 days. Significant differences were found in the dissipation rates of BPS in three soils with different pH values. The dissipation of BPS followed pseudo first-order kinetics with half-lives (T1/2) of 15.2 ± 0.1 d, 27.0 ± 0.2 d, 180.4 ± 5.3 d, and 280.5 ± 3.3 d in the alkaline soil (fluvo-aquic soil, FS), the neutral soil (cinnamon soil, CS), the acidic soil (red soil, RS), and sterilized cinnamon soil (CS-S), respectively. The mineralization and BRs formation contributed the most to the dissipation of BPS in soil. BPS was persistent in acidic soil, and may pose a significant threat to plants grown in acidic soils. Additionally, soil microorganisms played a key role in BPS degradation, and the organic matter content might be a major factor that promotes the adsorption and degradation of BPS in soils. Two transformed products, P-hydroxybenzenesulfonic acid and methylated BPS were identified in soils. This study provides new insights into the fate of BPS in various soils, which will be useful for risk assessments of BPS in soil.

12.
Adv Mater ; 35(47): e2305344, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37540191

RESUMO

The integration of hydrogen-bonded organic frameworks (HOFs) into electronic devices holds great promise due to their high crystallinity, intrinsic porosity, and easy regeneration. However, despite their potential, the utilization of HOFs in electronic devices remains largely unexplored, primarily due to the challenges associated with fabricating high-quality films. Herein, a controlled synthesis of HOF nanofilms with smooth surface, good crystallinity, and high orientation is achieved using a solution-processed approach. The memristors exhibit outstanding bipolar switching performance with a low set voltage of 0.86 V, excellent retention of 1.64 × 104 s, and operational endurance of 60 cycles. Additionally, these robust memristors display remarkable thermal stability, maintaining their performance even at elevated temperatures of up to 200 °C. More strikingly, scratched HOF films can be readily regenerated through a simple solvent rinsing process, enabling their reuse for the fabrication of new memristors, which is difficult to achieve with traditional resistive switching materials. Additionally, a switching mechanism based on the reversible formation and annihilation of conductive filaments is revealed. This work provides novel and invaluable insights that have a significant impact on advancing the widespread adoption of HOFs as active layers in electronic devices.

13.
Sensors (Basel) ; 23(12)2023 Jun 14.
Artigo em Inglês | MEDLINE | ID: mdl-37420749

RESUMO

The safety of railway transportation is crucial to social and economic development. Therefore, real-time monitoring of the rail is particularly necessary. The current track circuit structure is complex and costly, posing challenges to monitoring broken tracks using alternative methods. As a non-contact detection technology with a lower environmental impact, electromagnetic ultrasonic transducers (EMATs) have become a concern. However, traditional EMATs have problems such as low conversion efficiency and complex modes, which can limit their effectiveness for long-distance monitoring. Therefore, this study introduces a novel dual-magnet phase-stacked EMAT (DMPS-EMAT) design comprising two magnets and a dual-layer winding coil arrangement. The magnets are positioned at a distance equal to the wavelength of the A0 wave from each other, while the center distance between the two sets of coils beneath the transducer is also equal to the wavelength. After analyzing the dispersion curves of the rail waist, it was determined that the optimal frequency for long-distance rail monitoring is 35 kHz. At this frequency, adjusting the relative positions of the two magnets and the coil directly underneath to be one A0 wavelength can effectively excite a constructive interference A0 wave in the rail waist. The simulation and experimental results show that DMPS-EMAT excited a single-mode A0 wave, resulting in a 1.35-times increase in amplitude.


Assuntos
Imãs , Tecnologia , Simulação por Computador , Transdutores , Meios de Transporte
14.
Angew Chem Int Ed Engl ; 62(37): e202304694, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37162371

RESUMO

In situ photo-deposition of both Pt and CoOx cocatalysts on the facets of poly (triazine imide) (PTI) crystals has been developed for photocatalytic overall water splitting. However, the undesired backward reaction (i.e., water formation) on the noble Pt surface is a spontaneously down-hill process, which restricts their efficiency to run the overall water splitting reaction. Herein, we demonstrate that the efficiency for photocatalytic overall water splitting could be largely promoted by the decoration of Rh/Cr2 O3 and CoOx as H2 and O2 evolution cocatalysts, respectively. Results reveal that the dual cocatalysts greatly extract charges from bulk to surface, while the Rh/Cr2 O3 cocatalyst dramatically restrains the backward reaction, achieving an apparent quantum efficiency (AQE) of 20.2 % for the photocatalytic overall water splitting reaction.

15.
J Hazard Mater ; 445: 130583, 2023 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-37055988

RESUMO

As a best-selling triazolinthione fungicide, prothioconazole (PTZ) has been widely used worldwide and has aroused concern about its environmental effect. This study used phenyl-UL-14C-labeled PTZ and an improved fate model to investigate the fate and metabolism of this fungicide in aerobic soil. During 120 d of incubation, PTZ rapidly transformed into metabolites and bound residues, with a half-life (DT50) of less than 1 d. After 120 d, approximately 45-55% of PTZ formed bound residues, and the extractable metabolite residues were gradually degraded over time. Approximately 19%, 44% and 27% of phenyl-UL-14C-PTZ was mineralized in red soil, fluvo-aquic soil and cinnamon soil, respectively, but only approximately 3% was mineralized in black soil. Five metabolites were identified and confirmed, and a possible metabolic pathway for phenyl-UL-14C-PTZ in soil was proposed. Based on the correlation analysis between soil properties and model rate constants, soil properties exerted important effects on PTZ transformation. These results will provide basic data for environmental risk assessments and removal of the PTZ pollutant and suggest that the soil type should be considered in the selection and application of pesticides.


Assuntos
Fungicidas Industriais , Praguicidas , Poluentes do Solo , Fungicidas Industriais/química , Solo/química , Poluentes do Solo/análise
16.
Sci Total Environ ; 880: 163312, 2023 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-37030363

RESUMO

Dufulin is a promising chiral antiviral agent, but little is known about its fate in soils. In this study, the fate of dufulin enantiomers in aerobic soils was investigated using radioisotope tracing techniques. The result of the four-compartment model showed no significant differences in dissipation, generation of bound residues (BR) and mineralization between S-dufulin and R-dufulin during incubation. Dufulin dissipated most quickly in cinnamon soils, followed by fluvo-aquic and black soils and the half-lives of dufulin in these soils obtained by the modified model were 4.92-5.23, 32.39-33.32 and 60.80-61.34 d, respectively. After 120 d incubation, the percentage of radioactivity of BR increased to 18.2-38.4 % in the three soils. Dufulin formed most bound residues in the black soil, least in the cinnamon soil, and BRs rapidly formed in the cinnamon soil during the early culture period. In these three soils, the cumulative mineralization of 14CO2 ranged from 25.0 to 26.7 %, 42.1 to 43.4 % and 33.8 to 34.4 %, respectively, which indicated that the environmental fate of dufulin was primarily influenced by soil characteristics. The study of microbial community structure revealed that the phyla Ascomycota, Proteobacteria and genus Mortierella might be related to the degradation of dufulin. These findings provide a reference for assessing the environmental impact and ecological safety of dufulin application.


Assuntos
Praguicidas , Poluentes do Solo , Praguicidas/química , Solo/química , Poluentes do Solo/análise , Benzotiazóis/análise
17.
ACS Appl Mater Interfaces ; 15(13): 17134-17143, 2023 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-36972382

RESUMO

The self-assembly mechanism of alternating AlN/TiN nano-lamellar structures in AlTiN coating is still a mystery, though this coating has been widely used in industry. Here, by using the phase-field crystal method, we studied the atomic-scale mechanisms of the formation of nano-lamellar structures during spinodal decomposition transformation of an AlTiN coating. The results show that the formation of a lamella is characterized by four distinct stages including the generation of dislocations (stage I), formation of islands (stage II), merging of islands (stage III), and flattening of lamellae (stage IV). The locally periodic fluctuation of the concentration along the lamella leads to the generation of periodically distributed misfit dislocations and then AlN/TiN islands, while the fluctuation of the composition in the direction normal to the lamella is responsible for the merging of islands and flattening of a lamella and more importantly the cooperative growth between neighboring lamellae. Moreover, we found that misfit dislocations play a crucial role in all the four stages, promoting the cooperative growth of TiN and AlN lamellae. Our results demonstrate that the TiN and AlN lamellae could be produced through the cooperative growth of AlN/TiN lamellae in spinodal decomposition of the AlTiN phase.

18.
Med Sci Monit Basic Res ; 29: e938849, 2023 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-36883230

RESUMO

BACKGROUND Postoperative tracheal extubation requires optimal timing to ensure patient safety and normal muscle function. The train-of-four ratio (TOFR) of the fourth muscle response compared with the first indicates a non-depolarizing neuromuscular block, and a ratio ≥0.9 can be used as an objective measurement of neuromuscular reversal. This study of 60 adult patients who underwent elective surgery with general anesthesia that included the neuromuscular blocking agent cisatracurium aimed to compare standard postoperative clinical assessment with the TOFR ≥0.9 on patient outcomes using postoperative neuromuscular function assessed by grip strength and ability to sit up unaided and spirometry measurements following extubation. MATERIAL AND METHODS The 30 patients extubated postoperatively in the TOF group were required to have a TOFR ≥0.9, while the 30 patients in the clinical assessment group were awake and following simple commands and had a 5-second head lift and spontaneous breathing with acceptable oxygenation. The main outcomes were the incentive spirometry and grip strength and ability to sit up unaided measured at 10, 30, 50 min and 24 h after extubation. RESULTS The groups had no difference in recovery path of incentive spirometry volume (P=0.072) and no difference in postoperative incentive spirometry decrease from baseline except at 10 min after extubation (P=0.005). There was no difference in handgrip strength and independent sitting between groups. CONCLUSIONS The findings showed that using the TOF ratio ≥0.9 before extubation did not improve early postoperative strength quantified by spirometry volume, handgrip strength, and proportion of unaided sitting.


Assuntos
Extubação , Força da Mão , Humanos , Adulto , Espirometria
19.
Angew Chem Int Ed Engl ; 62(14): e202216434, 2023 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-36748541

RESUMO

Poly (triazine imide) photocatalysts prepared via molten salt methods emerge as promising polymer semiconductors with one-step excitation capacity of overall water splitting. Unveiling the molecular conjugation, nucleation, and crystallization processes of PTI crystals is crucial for their controllable structure design. Herein, microscopy characterization was conducted at the PTI crystallization front from meso to nano scales. The heptazine-based precursor was found to depolymerize to triazine monomers within molten salts and KCl cubes precipitate as the leading cores that guide the directional stacking of PTI molecular units to form aggregated crystals. Upon this discovery, PTI crystals with improved dispersibility and enhanced photocatalytic performance were obtained by tailoring the crystallization fronts. This study advances insights into the directional assembling of PTI monomers on salt templates, placing a theoretical foundation for the ordered condensation of polymer crystals.

20.
Adv Mater ; 35(15): e2209955, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36692193

RESUMO

The photo-electrochemical (PEC) oxidation of glycerol (GLY) to high-value-added dihydroxyacetone (DHA) can be achieved over a BiVO4 photoanode, while the PEC performance of most BiVO4 photoanodes is impeded due to the upper limits of the photocurrent density. Here, an enhanced Mie scattering effect of the well-documented porous BiVO4 photoanode is obtained with less effort by a simple annealing process, which significantly reduces the reflectivity to near zero. The great light absorbability increases the basic photocurrent density by 1.77 times. The selective oxidation of GLY over the BiVO4 photoanode results in a photocurrent density of 6.04 mA cm-2 and a DHA production rate of 325.2 mmol m-2 h-1 that exceeds all reported values. This work addresses the poor ability of nanostructured BiVO4 to harvest light, paving the way for further improvements in charge transport and transfer to realize highly efficient PEC conversion.

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