Reversible Covalent Assembly of Nanoparticles through On-Surface Diels-Alder Reaction.

We demonstrate here a controlled assembly of individual nanoscale building blocks into defined architectures based on chemospecific covalent bonding interactions. For this purpose, α-Fe2O3, γ-Fe2O3, and SiO2 nanoparticles decorated with surface-conjugated organic ligands were used for performing on-surface Diels-Alder reactions. Driven through their chemical affinity and surface-grafted complementary functionalities, nanoparticles underwent click-reactions to produce covalently organized nanostructures. An advantage of using the Diels-Alder reaction is its reversible nature, which was used to click and unclick the nanoparticles on demand. The efficiency and chemical specificity of this approach opens up another synthetic access to unify materials with complementary properties, where the thermoresponsive nature of particle assemblies imparts to them a fully reversible character. The covalent conjugation strategies demonstrated in this work potentially allow the use of a diverse range of particles and ligands for their applications in different disciplines such as medicine, optics, or photonics. The nanoparticles morphology and crystalline nature were investigated by TEM and XRD analysis, while the presence of surface attached groups was verified by NMR, FTIR, UV-vis, and ζ potential measurements.

Potential and perspectives of halide perovskites in light emitting devices.

Light emitting diodes (LEDs) have become part of numerous electrical and electronic systems such as lighting, displays, status indicator lamps and wearable electronics. Owing to their excellent optoelectronic properties and deposition via simple solution process, metal halide perovskites possess unique potential for developing halide perovskite-based LEDs (PeLEDs) with superior photoluminescence efficiencies leading to external quantum efficiencies beyond 20% for PeLEDS. However, the limited durability, high operative voltages, and challenges of scale-up are persisting barriers in achieving required technology readiness levels. To build up the existing knowledge and raise the device performance this review provides a state-of-the-art study on the properties, film and device fabrication, efficiency, and stability of PeLEDs. In terms of commercialization, PeLEDs need to overcome materials and device challenges including stability, ion migration, phase segregation, and joule heating, which are discussed in this review. We hope, discussions about the strategies to overcome the stability issues and enhancement the materials intrinsic properties towards development more stable and efficient optoelectronic devices can pave the way for scalability and cost-effective production of PeLEDs.

Thermally-induced drift of A-site cations at solid-solid interface in physically paired lead halide perovskites.

The promise of hybrid organic-inorganic halide perovskite solar cells rests on their exceptional power conversion efficiency routinely exceeding 25% in laboratory scale devices. While the migration of halide ions in perovskite thin films has been extensively investigated, the understanding of cation diffusion remains elusive. In this study, a thermal migration of A­site cations at the solid-solid interface, formed by two physically paired MAPbI3 and FAPbI3 perovskite thin films casted on FTO, is demonstrated through continuous annealing at comparably low temperature (100 °C). Diffusion of methylammonium (CH3NH3+, MA+) cations into the low­symmetry yellow δ­FAPbI3 phase triggers a transition from the yellow (δ) to black (α) phase evident in the distinctive color change and verified by shifts in absorption bands and X­ray diffraction patterns. Intermixing of the A­site cations MA+ and FA+ (CH(NH2)2+) occurred for both systems, α­MAPbI3/δ­FAPbI3 and α­MAPbI3/α­FAPbI3. The structural and compositional changes in both cases support a thermally activated ion drift unambiguously demonstrated through changes in the absorption and X-ray photoelectron spectra. Moreover, the physical contact annealing (PCA) leads to healing of defects and pinholes in α­MAPbI3 thin films, which was correlated to longer recombination lifetimes in mixed MAxFA1-xPbI3 thin films obtained after PCA and probed by ultrafast transient absorption spectroscopy.

Fabrication of Antibacterial, Osteo-Inductor 3D Printed Aerogel-Based Scaffolds by Incorporation of Drug Laden Hollow Mesoporous Silica Microparticles into the Self-Assembled Silk Fibroin Biopolymer.

In this study, the novel biomimetic aerogel-based composite scaffolds through a synergistic combination of wet chemical synthesis and advanced engineering approaches have successfully designed. To this aim, initially the photo-crosslinkable methacrylated silk fibroin (SF-MA) biopolymer and methacrylated hollow mesoporous silica microcapsules (HMSC-MA) as the main constituents of the novel composite aerogels were synthesized. Afterward, by incorporation of drug-loaded HMSC-MA into the self-assembled SF-MA, printable gel-based composite inks are developed. By exploiting micro-extrusion-based three-dimensional (3D) printing, SF-MA-HMSC composite gels are printed by careful controlling their viscosity to provide a means to control the shape fidelity of the resulted printed gel constructs. The developed scaffold has shown a multitude of interesting biophysical and biological performances. Namely, thanks to the photo-crosslinking of the gel components during the 3D printing, the scaffolds become mechanically more stable than the pristine SF scaffolds. Also, freeze-casting the printed constructs generates further interconnectivity in the printed pore struts resulting in the scaffolds with hierarchically organized porosities necessary for cell infiltration and growth. Importantly, HMSC incorporated scaffolds promote antibacterial drug delivery, cellular ingrowth and proliferation, promoting osteoblastic differentiation by inducing the expression of osteogenic markers and matrix mineralization. Finally, the osteoconductive, -inductive, and anti-infective composite aerogels are expected to act as excellent bone implanting materials with an extra feature of local and sustained release of drug for efficient therapy of bone-related diseases.

18F-Labeled magnetic nanovectors for bimodal cellular imaging.

Surface modification of nanocarriers enables selective attachment to specific molecular targets within a complex biological environment. Besides the enhanced uptake due to specific interactions, the surface ligands can be utilized for radiolabeling applications for bimodal imaging ensured by positron emission topography (PET) and magnetic resonance imaging (MRI) functions in one source. Herein, we describe the surface functionalization of magnetite (Fe3O4) with folic acid as a target vector. Additionally, the magnetic nanocarriers were conjugated with appropriate ligands for subsequent copper-catalyzed azide-alkyne cycloaddition or carbodiimide coupling reactions to successfully achieve radiolabeling with the PET-emitter 18F. The phase composition (XRD) and size analysis (TEM) confirmed the formation of Fe3O4 nanoparticles (6.82 nm ± 0.52 nm). The quantification of various surface functionalities was performed by Fourier-transform infrared spectroscopy (FT-IR) and ultraviolet-visible microscopy (UV-Vis). An innovative magnetic-HPLC method was developed in this work for the determination of the radiochemical yield of the 18F-labeled NPs. The as-prepared Fe3O4 particles demonstrated high radiochemical yields and showed high cellular uptake in a folate receptor overexpressing MCF-7 cell line, validating bimodal imaging chemical design and a magnetic HPLC system. This novel approach, combining folic acid-capped Fe3O4 nanocarriers as a targeting vector with 18F labeling, is promising to apply this probe for bimodal PET/MR-studies.

The economic burden of malaria on the household in south-central Vietnam.

BACKGROUND: Each year, several thousand cases of malaria occur in south-central Vietnam. Evidence from elsewhere suggests that malaria can have an economic impact on the household as the illness prevents households from completing their normal, physically demanding, productive duties such as tending crops and animals. The economic impact of malaria on households was explored within the Raglay ethnic minority living in the montainous and forested area of south-central Vietnam (Ninh Thuan Province). METHODS: Two-hundred fifty-one malaria patients were identified and interviewed in an exit survey at Community Health Centres. The same patient sample was then re-interviewed in a household survey two to four weeks later. Survey data were complemented by approximately 40 informal discussions with health workers, vendors, patients, and community leaders. RESULTS: Each episode of malaria was estimated to cost the patient's household an average of 11.79 USD (2005 prices), direct costs for travel and treatment representing 6% of the total while the remainder was loss in annual income. CONCLUSION: Whilst government provision of malaria treatment keeps the direct costs relatively low, the overall loss in income due to illness can still be significant given the poverty amongst this population, especially when multiple cases of malaria occur annually within the same household.

Cost-effectiveness of long-lasting insecticide-treated hammocks in preventing malaria in South-central Vietnam.

BACKGROUND: Despite much success in reducing the burden of malaria in Vietnam, pockets of malaria persist and eliminating them remains an important development goal. In central Vietnam, insecticide-treated hammocks have recently been introduced to help counter the disease in the highly forested, mountainous areas, where other measures have so far been unsuccessful. This study assesses the cost-effectiveness of using long-lasting insecticide-treated hammocks in this area. METHODS AND FINDINGS: This cost-effectiveness study was run alongside a randomized control trial testing the efficacy of the long-lasting insecticide-treated hammocks. Data were collected through an exit survey, a household survey, expenditure records and key informant interviews. The study estimates that under normal (non-trial) conditions the total net societal cost per malaria episode averted in using long-lasting insecticide-treated hammocks in this area was 126 USD. Cost per hammock, including insecticidal netting, sewing, transport, and distribution was found to be approximately 11.76 USD per hammock. Average savings per episode averted were estimated to be $14.60 USD for the health system and 14.37 USD for households (including both direct and indirect cost savings). The study estimates that the annual financial outlay required of government to implement this type of programme to be 3.40 USD per person covered per year. CONCLUSION: The study finds that the use of a hammock intervention could represent good value for money to help prevent malaria in more remote areas, where traditional control measures such as insecticide-treated bednets and indoor residual spraying are insufficient or inappropriate to control malaria. However, the life span of the hammock-the number of years over which it effectively deters mosquitoes-has a significant impact on the cost-effectiveness of the intervention and study results should be interpreted in light of the evidence on effectiveness gathered in the years to come.