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1.
Small ; : e2401485, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38712455

RESUMO

Dual channel photo-driven H2O2 production in pure water on small-scale on-site setups is a promising strategy to provide low-concentrated H2O2 whenever needed. This process suffers, however, strongly from the fast recombination of photo-generated charge carriers and the sluggish oxidation process. Here, insoluble Keggin-type cesium phosphomolybdate Cs3PMo12O40 (abbreviated to Cs3PMo12) is introduced to carbonized cellulose (CC) to construct S-scheme heterojunction Cs3PMo12/CC. Dual channel H2O2 photosynthesis from both H2O oxidation and O2 reduction in pure water has been thus achieved with the production rate of 20.1 mmol L-1 gcat. -1 h-1, apparent quantum yield (AQY) of 2.1% and solar-to-chemical conversion (SCC) efficiency of 0.050%. H2O2 accumulative concentration reaches 4.9 mmol L-1. This high photocatalytic activity is guaranteed by unique features of Cs3PMo12/CC, namely, S-scheme heterojunction, electron reservoir, and proton reservoir. The former two enhance the separation of photo-generated charge carriers, while the latter speeds up the torpid oxidation process. In situ experiments reveal that H2O2 is formed via successive single-electron transfer in both channels. In real practice, exposing the reaction system under natural sunlight outdoors successfully results in 0.24 mmol L-1 H2O2. This work provides a key practical strategy for designing photocatalysts in modulating redox half-reactions in photosynthesis.

2.
J Colloid Interface Sci ; 668: 666-677, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38703514

RESUMO

Silicon is considered as the next-generation anode material for lithium-ion batteries due to its high theoretical specific capacity and abundant crustal abundance. However, its poor electrical conductivity results in slow diffusion of lithium ions during battery operation. Simultaneously, the alloying process of silicon undergoes a 300 % volume change, leading to structural fractures in silicon during the cycling process. As a result, it loses contact with the current collector, continuously exposing active sites, and forming a sustained solid electrolyte interface (SEI) membrane. This paper presents the design of a fluorine-ion-regulated yolk-shell carbon-silicon anode material, highlighting the following advantages: (a) Alleviating volume changes through the design of a yolk-shell structure, thereby maintaining material structural integrity during cycling. (b) Carbon shell prevents silicon from coming into contact with the electrolyte, simultaneously improving silicon's electrical conductivity and increasing ion/electron conductivity. (c) Utilizing fluorine-ion interface modification to obtain an SEI membrane rich in fluorine components (such as LiF), thereby enhancing its long cycling performance. The F-Si@Void@C exhibits outstanding electrochemical performance, with a reversible capacity of 1166 mAh/g after 900 cycles at a current density of 0.5 A/g.

3.
Transl Oncol ; 45: 101973, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38705052

RESUMO

OBJECTIVE: High-grade glioma (HGG) patients frequently encounter treatment resistance and relapse, despite numerous interventions seeking enhanced survival outcomes yielding limited success. Consequently, this study, rooted in our prior research, aimed to ascertain whether leveraging circadian rhythm phase attributes could optimize radiotherapy results. METHODS: In this retrospective analysis, we meticulously selected 121 HGG cases with synchronized rhythms through Cosinor analysis. Post-surgery, all subjects underwent standard radiotherapy alongside Temozolomide chemotherapy. Random allocation ensued, dividing patients into morning (N = 69) and afternoon (N = 52) radiotherapy cohorts, enabling a comparison of survival and toxicity disparities. RESULTS: The afternoon radiotherapy group exhibited improved overall survival (OS) and progression-free survival (PFS) relative to the morning cohort. Notably, median OS extended to 25.6 months versus 18.5 months, with P = 0.014, with median PFS at 20.6 months versus 13.3 months, with P = 0.022, post-standardized radiotherapy. Additionally, lymphocyte expression levels in the afternoon radiation group 32.90(26.10, 39.10) significantly exceeded those in the morning group 31.30(26.50, 39.20), with P = 0.032. CONCLUSIONS: This study underscores the markedly prolonged average survival within the afternoon radiotherapy group. Moreover, lymphocyte proportion demonstrated a notable elevation in the afternoon group. Timely and strategic adjustments of therapeutic interventions show the potential to improve therapeutic efficacy, while maintaining vigilant systemic immune surveillance. A comprehensive grasp of physiological rhythms governing both the human body and tumor microenvironment can refine treatment efficacy, concurrently curtailing immune-related damage-a crucial facet of precision medicine.

4.
J Colloid Interface Sci ; 661: 544-563, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38308894

RESUMO

The realization of 2D/2D Van der Waals (VDW) heterojunctions represents an advanced approach to achieving superior photocatalytic efficiency. However, electron transfer through Van der Waals heterojunctions formed via ex-situ assembly encounters significant challenges at the interface due to contrasting morphologies and potential barriers among the nanocomposite substituents. Herein, a novel approach is presented, involving the insertion of a phosphate group between copper phthalocyanine (CuPc) and B-doped and N-deficient g-C3N4 (BDCNN), to design and construct a Van der Waals heterojunction labeled as xCu[acs]/yP-BDCNN. The introduction of phosphate as a charge modulator and efficient conduit for charge transfer within the heterojunction resulted in the elimination of spatial barriers and induced electron movement from BDCNN to CuPc in the excited states. Consequently, the catalytic central Cu2+ in CuPc captured the photoelectrons, leading to the conversion of CO2 to C2H4, CO and CH4. Remarkably, this approach resulted in a 78-fold enhancement in photocatalytic efficiency compared to pure BDCNN. Moreover the findings confirm that the 2D-2D 4Cu[acs]/9P-BDCNN sheet-like heterojunction effectively boosts photocatalytic activity for persistent pollutants such as methyl orange (MO), methylene blue (MB), rhodamine B (RhB), and tetracycline antibiotics (TCs). The introduction of "interfacial interacting" substances to establish an electron transfer pathway presents a novel and effective strategy for designing photocatalysts capable of efficiently reducing CO2 into valuable products.

5.
J Colloid Interface Sci ; 660: 192-202, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38241867

RESUMO

Interfacial solar steam generation is considered a promising approach to address energy and drinking water shortages. However, designing efficient light-absorbing and photothermal-converting materials remains challenging. In this study, we describe a detailed method for synthesising a three-dimensional (3D) hierarchical oxygen defect-rich WO3/Ag/PbS/Ni foam (termed WO3-x/Ag/PbS/NF) composite to realise efficient exciton separation and enhanced photothermal conversion. The 3D heterogeneous ternary photothermal material combines the individual benefits of WO3-x, Ag and PbS, improving charge transfer and promoting photogenerated electron-hole pairs. This enhances light absorption and energy conversion. Theoretical calculations indicate that the increased photothermal conversion efficiency primarily results from the heterojunction between Ag, WO3-x and PbS, facilitating exciton separation and electron transfer. Consequently, the WO3-x/Ag/PbS/NF solar evaporator exhibits exceptional light absorption (98% within the sunlight spectrum), a high evaporation rate of 1.90 kg m-2h-1 under 1 sun and a light-to-heat conversion efficiency of 94%. The WO3-x/Ag/PbS/NF evaporator also exhibits excellent capabilities in seawater desalination and wastewater treatment. This approach introduces a synergistic concept for creating novel multifunctional light-absorbing materials suitable for various energy-related applications.

6.
ACS Appl Mater Interfaces ; 16(1): 889-897, 2024 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-38153800

RESUMO

Achieving effective hydrogen evolution/oxidation reaction (HER/HOR) across a wide pH span is of critical importance in unlocking the full potential of hydrogen energy but remains intrinsically challenging. Here, we engineer the N-coordinated Ir-Mo dual atoms on a carbon matrix by ultrafast high-temperature sintering, creating an efficient bifunctional electrocatalyst for both HER and HOR in both acidic and alkaline electrolytes. The optimized catalyst, Ir-Mo DAC/NC, demonstrates exceptional performance, with a significantly reduced HER overpotential of 11.3 mV at 10 mA/cm2 and a HOR exchange current (i0,m) of 3972 mA/mgIr in acidic conditions, surpassing the performance of Pt/C and Ir/C catalysts. In alkaline conditions, Ir-Mo DAC/NC also outperforms Pt/C, as evidenced by its low HER overpotential of 23 mV at 10 mA/cm2 and a high i0,m of 1308 mA/mgIr. Furthermore, our catalyst exhibits remarkable stability in both acidic and alkaline environments. DFT calculations results reveal that the superior electrochemical performance of Ir-Mo DAC/NC arises from the electronic synergy between Ir and Mo pairs, which regulates the interaction between the intermediates and active sites. These findings present a promising strategy for the development of dual-atom catalysts (DACs), with potential applications in the polymer fuel cells and water electrolyzers.

7.
Nat Commun ; 14(1): 8384, 2023 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-38104169

RESUMO

Electrocatalytic acetylene semi-hydrogenation to ethylene powered by renewable electricity represents a sustainable pathway, but the inadequate current density and single-pass yield greatly impedes the production efficiency and industrial application. Herein, we develop a F-modified Cu catalyst that shows an industrial partial current density up to 0.76 A cm-2 with an ethylene Faradic efficiency surpass 90%, and the maximum single-pass yield reaches a notable 78.5%. Furthermore, the Cu-F showcase the capability to directly convert acetylene into polymer-grade ethylene in a tandem flow cell, almost no acetylene residual in the production. Combined characterizations and calculations reveal that the Cuδ+ (near fluorine) enhances the water dissociation, and the generated active hydrogen are immediately transferred to Cu0 (away from fluorine) and react with the locally adsorbed acetylene. Therefore, the hydrogen evolution reaction is surpassed and the overall acetylene semi-hydrogenation performance is boosted. Our findings provide new opportunity towards rational design of catalysts for large-scale electrosynthesis of ethylene and other important industrial raw.

8.
RSC Adv ; 13(40): 27705-27713, 2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37731826

RESUMO

Fe-N-C material, known for its high efficiency, cost-effectiveness, and environmental friendliness, is a promising electrocatalyst in the field of the oxygen reduction reaction (ORR). However, the influence of defects and coordination structures on the catalytic performance of Fe-N-C has not been completely elucidated. In our present investigation, based on density functional theory, we take an Fe adsorbed graphene structure containing a 5-8-5 divacancy (585DV) defect as a research model and investigate the influence of the coordination number of N atoms around Fe (Fe-NxC(4-x)) on the ORR electrocatalyst behavior in alkaline conditions. We find that the Fe-N4 structure exhibits superior ORR catalytic performance than other N coordination structures Fe-NxC4-x (x = 0-3). We explore the reasons for the improved catalytic performance through electronic structure analysis and find that as the N coordination number in the Fe-NxC(4-x) structure increases, the magnetic moment of the Fe single atom decreases. This reduction is conducive to the ORR catalytic performance, indicating that a lower magnetic moment is more favorable for the catalytic process of the ORR within the Fe-NxC(4-x) structure. This study is of great significance for a deeper understanding of the structure-performance relationship in catalysis, as well as for the development of efficient ORR catalysts.

9.
Adv Sci (Weinh) ; 10(26): e2303110, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37435625

RESUMO

Simultaneously optimizing elementary steps, such as water dissociation, hydroxyl transferring, and hydrogen combination, is crucial yet challenging for achieving efficient hydrogen evolution reaction (HER) in alkaline media. Herein, Ru single atom-doped WO2 nanoparticles with atomically dispersed Ru-W pair sites (Ru-W/WO2 -800) are developed using a crystalline lattice-confined strategy, aiming to gain efficient alkaline HER. It is found that Ru-W/WO2 -800 exhibits remarkable HER activity, characterized by a low overpotential (11 mV at 10 mA cm-2 ), notable mass activity (5863 mA mg-1 Ru at 50 mV), and robust stability (500 h at 250 mA cm-2 ). The highly efficient activity of Ru-W/WO2 -800 is attributed to the synergistic effect of Ru-W sites through ensemble catalysis. Specifically, the W sites expedite rapid hydroxyl transferring and water dissociation, while the Ru sites accelerate the hydrogen combination process, synergistically facilitating the HER activity. This study opens a promising pathway for tailoring the coordination environment of atomic-scale catalysts to achieve efficient electro-catalysis.

10.
Am J Transl Res ; 15(4): 2716-2726, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37193188

RESUMO

OBJECTIVES: Lymphoepithelial carcinoma (LEC) of the oral cavity and pharynx is a rare cancer, with poorly understood clinicopathological characteristics and prognosis. Only a few case reports or small case series have been reported, so the characteristics and survival of patients with this disease remains unclear. The present study aimed to describe the clinicopathological characteristics and determine the factors associated with survival of this uncommon cancer. METHODS: A population-based study was carried out to investigate clinical characteristics and prognosis of LEC of the oral cavity and pharynx using the data from Surveillance, Epidemiology and End Results (SEER) database. Log-Rank test and Cox regression analysis were performed to determine the prognostic factors, and a prognostic nomogram was further constructed. The propensity-matched analysis was conducted to compare the survival of nasopharyngeal LEC and non-nasopharyngeal LEC patients. RESULTS: Totally, 1025 patients were identified, including 769 nasopharyngeal LEC patients and 256 non-nasopharyngeal LEC patients. The median OS of all patients was 232.0 months (95% CI 169.0-258.0). The 1-, 5-, 10- and 20-year survival rates were 92.9%, 72.9%, 59.3%, and 46.8%, respectively. Surgery significantly prolonedg the survival of LEC patients (P<0.01, mOS: 190 m vs. 255 m). Radiotherapy, as well as radiotherapy after surgery, prolonged the mOS (P<0.01 for both). The survival analysis demonstrated that old age (>60 years), lymph node (N3) and distant metastases were independent factors for poor survival, whereas radiotherapy and surgery were independent factors for favorable survival. The prognostic nomogram was established base on these five independent prognostic factors (C-index = 0.70; 95% CI 0.66-0.74). In addition, no significant difference in survival time between nasopharyngeal LEC and non-nasopharyngeal LEC patients were observed. CONCLUSIONS: LEC of the oral cavity and pharynx is a rare disease, and old age, lymph node and distant metastases, surgery and radiotherapy were significantly associated with prognosis. The prognostic nomogram could be used to make individual predictions of OS.

11.
Oral Dis ; 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37183989

RESUMO

OBJECTIVE: Oral squamous cell carcinoma (OSCC) is the most common malignant tumour in the oral cavity. OSCC is aggressive and prone to metastasis; it is associated with high mortality and short survival. In this study, we investigated the function of the long non-coding RNA LINC00525 in OSCC progression and the molecular mechanisms through in vitro and in vivo experiments. MATERIALS AND METHODS: CCK8 assay was used to detect the effect of LINC00525 on cell viability; transwell migration and invasion assays and scratch assay were used to examine the role of LINC00525 in cell migration and invasion. Flow cytometry, RT-PCR and western blot were used to detect apoptosis indexes. Tumorigenic effects were investigated using mouse xenograft tumour models. RESULTS: LINC00525 was associated with OSCC survival and prognosis. LINC00525 knockdown decreased cell viability and epithelial-mesenchymal transition (EMT) properties and increased apoptosis and also shortened the cell cycle of OSCC cells in vitro. The downregulation of LINC00525 reduced the growth of OSCC tumour in vivo. LINC00525 can regulate OSCC cells via the apoptotic signalling pathway. CONCLUSION: Our results indicate that LINC00525 exhibits oncogenic functions in OSCC. LINC00525 may be a new promising and potential target for the treatment of OSCC.

12.
Adv Sci (Weinh) ; 10(12): e2206166, 2023 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-36861951

RESUMO

Understanding the dynamical evolution from metal ions to single atoms is of great importance to the rational development of synthesis strategies for single atom catalysts (SACs) against metal sintering during pyrolysis. Herein, an in situ observation is disclosed that the formation of SACs is ascertained as a two-step process. There is initially metal sintering into nanoparticles (NPs) (500-600 °C), followed by the conversion of NPs into metal single atoms (Fe, Co, Ni, Cu SAs) at higher temperature (700-800 °C). Theoretical calculations together with control experiments based on Cu unveil that the ion-to-NP conversion can arise from the carbon reduction, and NP-to-SA conversion being steered by generating more thermodynamically stable Cu-N4 configuration instead of Cu NPs. Based on the evidenced mechanism, a two-step pyrolysis strategy to access Cu SACs is developed, which exhibits excellent ORR performance.

13.
ACS Appl Mater Interfaces ; 15(12): 16079-16089, 2023 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-36921354

RESUMO

Dielectric capacitors with an ultrahigh power density have received extensive attention due to their potential applications in advanced electronic devices. However, their inherent low energy density restricts their application for miniaturization and integration of advanced dielectric capacitors. Herein, a novel composite entirely incorporated with two-dimensional (2D) nanosheets with a topological trilayered construction is prepared by a solution casting and hot-pressing method. The 2D boron nitride nanosheets (BNNS) with a wide band gap that are oriented in a poly(vinylidene fluoride) (PVDF) matrix to form the upper and bottom outer layers would efficiently suppress the leakage current in composites, thus significantly improving the overall breakdown strength. Meanwhile, the 2D anatase-type TiO2 nanosheets (TONS) uniformly distributed in the middle layer can enhance their interfacial compatibility and polarization with the PVDF matrix, leading to a synergistic improvement in both the breakdown strength and dielectric constant of the composite. In particular, a significantly improved dielectric constant of ∼11.42, a reduced dielectric loss of 0.03 at 100 Hz, and a maximum discharge energy density (Udis) of 10.17 J cm-3 at an electric field of 370.1 MV m-1 can be obtained from the trilayered composite containing 3 wt % 2D TONS in the middle layer and 2 wt % 2D BNNS on the outer layer. The finding of this research offers an effective strategy for the preparation of advanced polymer-based composites with an outstanding discharge energy density performance.

14.
ACS Appl Mater Interfaces ; 15(8): 10718-10725, 2023 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-36802467

RESUMO

Single-atom catalysts with a tunable coordination structure have shown grand potential in flexibly altering the selectivity of oxygen reduction reaction (ORR) toward the desired pathway. However, rationally mediating the ORR pathway by modulating the local coordination number of the single-metal sites is still challenging. Herein, we prepare the Nb single-atom catalysts (SACs) with an external-shell oxygen-modulated unsaturated NbN3 site in carbon nitride and the NbN4 site anchored in nitrogen-doped carbon carriers, respectively. Compared with typical NbN4 moieties for 4e- ORR, the as-prepared NbN3 SACs exhibit excellent 2e- ORR activity in 0.1 M KOH, with the onset overpotential close to zero (9 mV) and the H2O2 selectivity above 95%, making it one of the state-of-the-art catalysts in the electrosynthesis of hydrogen peroxide. Density functional theory (DFT) theoretical calculations indicate the unsaturated Nb-N3 moieties and the adjacent oxygen groups optimize the interface bond strength of pivotal intermediates (OOH*) for producing H2O2, thus accelerating the 2e- ORR pathway. Our findings may provide a novel platform for developing SACs with high activity and tunable selectivity.

15.
J Headache Pain ; 24(1): 4, 2023 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-36641423

RESUMO

BACKGROUND: While new genetic analysis methods are widely used in the clinic, few researchers have focused on trigeminal neuralgia (TN) with familial clustering (≥ 2 TN patients in one kindred family). Previous literature suggests that familial trigeminal neuralgia (FTN) may be associated with inherited genetic factors. To date, few next-generation sequencing studies have been reported for FTN. This study investigated the pathogenic mechanism of FTN by using whole-exome sequencing (WES) technology, which may enhance our understanding of human TN pathophysiology.  METHOD: We performed WES for 7 probands from families of FTN. Sanger sequencing was performed for two control groups (FTN family members group and nonfamilial TN subject group) to potentially identify new FTN-related gene mutations. In families where FTN probands carried potentially pathogenic gene mutations, the ribonucleic acid (RNA) of FTN probands and related family members, as well as nonfamilial TN patients were analysed by RNA sequencing (RNA-seq) to confirm differential gene expression. RESULTS: Seven probands were derived from 3 Chinese families. WES and Sanger sequencing identified MARS1 mutation c.2398C > A p.(Pro800Thr) in Family 1. MARS1 mutation was confirmed in 14/26 [53.8%] members of Family 1 in FTN family member group, while none of nonfamilial TN subjects had this MARS1 mutation. RNA-seq showed that 3 probands in Family 1 had higher expression of Fosl1 (Fos-like antigen 1) and NFE2 (Nuclear factor, erythroid 2) than 3 subjects in the nonfamilial TN subject group. Fosl1 and NFE2 are genes related to integrated stress response (ISR). CONCLUSION: MARS1 mutations may cause chronic activation of ISR, contribute to ISR pathophysiological changes in FTN, and cause/accelerate peripheral nerve degeneration. The findings of this study can enrich our knowledge of the role of molecular genetics in TN in humans.


Assuntos
Metionina tRNA Ligase , Neuralgia do Trigêmeo , Humanos , Mutação , Linhagem , Neuralgia do Trigêmeo/genética , Metionina tRNA Ligase/genética
16.
Neurosurg Rev ; 46(1): 42, 2023 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-36707467

RESUMO

The occurrence of bleeding events after stent-assisted embolization of a ruptured artery requiring continuous double antiplatelet therapy may seriously affect the prognosis of this group of patients. A nomogram can provide a personalized, more accurate risk estimate based on predictors. We, therefore, developed a nomogram to predict the probability of bleeding events in patients with stent-assisted ruptured aneurysm embolization. We performed a single-center retrospective analysis of data collected from patients undergoing stent-assisted ruptured aneurysm embolization between January 2018 and December 2021. Forward stepwise logistic regression was performed to identify independent predictors of adverse events of bleeding after stent-assisted embolization and to establish nomograms. Discrimination and calibration of this model were performed using the area under the ROC curve (AUC-ROC) and the calibration plot. The model is internally validated by using resampling (1000 replicates). A total of 131 patients were identified, and a total of 118 patients met the study criteria. The predictors included in the nomogram were body mass index (BMI), AAi, and MA-ADP. The model showed good resolving power with a ROC area of 0.893 (95% CI: 0.834 ~ 0.952) for this model with good calibration. The nomogram can be used to individualize, visualize, and accurately predict the risk probability of bleeding events after stent-assisted embolization of ruptured aneurysms.


Assuntos
Aneurisma Roto , Embolização Terapêutica , Aneurisma Intracraniano , Humanos , Nomogramas , Estudos Retrospectivos , População do Leste Asiático , Alta do Paciente , Aneurisma Intracraniano/cirurgia , Aneurisma Intracraniano/etiologia , Resultado do Tratamento , Hemorragia/etiologia , Stents/efeitos adversos , Embolização Terapêutica/efeitos adversos , Aneurisma Roto/etiologia
17.
ACS Appl Mater Interfaces ; 14(34): 39311-39321, 2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-35977386

RESUMO

In recent years, high-energy-density polymer-based capacitors have received extensive attention because of their potential applications in advanced power systems and electronic equipment. However, their development is severely hampered by the inherent features of polymers such as low polarization and low charge-discharge efficiency (η). In this study, a new strategy for core-shell Na0.5Bi0.5TiO3(NBT)@TiO2(TO) whiskers combined with sandwich-structured poly(vinylidene fluoride) (PVDF)-based dielectric composites is proposed, in which the middle layer is the PVDF-based composites filled with different fractions of NBT@TO whiskers and the outer layers are pristine PVDF. The experimental results show that the loading of NBT@TO whiskers can simultaneously optimize electrical displacement and breakdown strength of the sandwich-structured composite due to the additional interfacial polarization and the contribution of the barrier effect between adjacent layers. Thus, a significantly improved electric displacement of ∼13.99 µC cm-2, a maximum discharge energy density (Ud) of ∼15.42 J cm-3 at a low electric field of 314 MV m-1, and a high charging-discharging efficiency (η ∼ 66.12%) can be obtained from the composite with the middle layer containing 6 wt % NBT@TO whiskers. This research provides a strategy for the preparation of advanced polymer-based composites with a superior discharge energy density in the future.

18.
ACS Appl Mater Interfaces ; 14(8): 10337-10343, 2022 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-35179878

RESUMO

Exploring highly active and cost-effective catalysts for styrene epoxidation is of great significance, but it remains challenging to simultaneously achieve excellent conversion and selectivity toward styrene oxide. In this work, the structures and performance of Co, Fe, and Cu single-atom catalysts (SACs) in styrene epoxidation with tert-butyl hydroperoxide (TBHP) are predicted using density functional theory (DFT) calculations. The results reveal that the Co-N structure prefers that of styrene oxide over Fe-N and Cu-N structures. This predicted result is verified via catalytic evaluations, where the Co SACs displayed significantly higher styrene oxide selectivity than Fe and Cu SACs. Moreover, the activity of Co SAC can be further improved by the construction of unsaturated vacancy-defect cobalt single sites. As a result, excellent performance with styrene conversion of 99.9% and styrene oxide selectivity of 71% is achieved after a reaction time of 8 h on the optimal Co SAC.

19.
J Colloid Interface Sci ; 602: 767-777, 2021 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-34198141

RESUMO

Solar steam generation is considered to be an effective strategy to alleviate the global water shortage problem. Therefore, exploring highly efficient and thermal stability photothermal conversion materials is highly essential and urgent. In this work, we develop a three-dimensional (3D) oxygen vacancy-rich WO3 with ''nanorod array grown on nanosheet array" unique architecture decorated on Ni foam (denoted as WO3-x/NF) through a simple and effective hydrothermal method followed by an annealing route, which is applied as light-absorbing material. The 3D hierarchical porous unique structure of the WO3-x/NF evaporator can supply a channel steam escaping and enhance the light trapping due to the multi-scattering effect, and the localized surface plasmon resonance (LSPR) effects of WO3-x also contribute to increase the light absorption in the full solar spectrum. The as-prepared WO3-x/NF evaporator reveals a high solar absorption (95%), an evaporation rate of 1.50 kg m-2 h-1 under one sun illumination, and a light-to-heat conversion efficiency of about 88%, as well as stable salt-resistance performance. The water purification results show that WO3-x/NF evaporator has a significant effect on seawater desalination without significant salt accumulation and purification of heavy metal wastewater. Furthermore, the first-principles calculations reveal that WO3 with oxygen vacancies has a narrower bandgap, which is more conducive to absorb solar energy from the whole spectrum. This work can provide a new avenue toward the design of other high photothermal conversion system.

20.
J Colloid Interface Sci ; 592: 77-86, 2021 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-33647564

RESUMO

Owing to the shortage of clean water as the global problem, the exploration of photothermal substances with high performance solar steam generation for sustainable water purification is essential and urgent. Herein, we demonstrate the assembly of two-dimensional graphene into one-dimensional rough, loose, and porous fibers and further use the assembled fibers to fabricate Janus membrane evaporator. The specific configuration guarantees an enhanced light harvesting property through multiple reflections, and improves the vapor transport ability through the constructed interlaced network. As a result, the as-obtained evaporator exhibits high solar absorbance, superior photothermal property and energy conversion efficiency, which is much higher than those of other reported Janus membrane evaporators and also better than the fabricated carbon nanotube-, and graphene sheet-based Janus membrane evaporator. The water purification results indicate that the fabricated graphene fiber-based Janus membrane is highly effective in seawater desalination without obvious salt accumulation and heavy metal wastewater purification. This study proposes a neotype graphene assembly for the fabrication of Janus membrane evaporator, which has potential applications in desalination and wastewater decontamination.

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