To evaluate the efficacy and safety of atropine 0.01% eye drops for myopia control in a multicentric pediatric Spanish cohort. An interventional, prospective, multicenter study was designed. Children ...aged between 6 and 14 years, with myopia between - 2.00 D to - 6.00 D, astigmatism < 1.50 D and documented previous annual progression greater than - 0.5 D (cycloplegic spherical equivalent, SE) were included. Once nightly atropine 0.01% eye drops in each eye were prescribed to all participants for 12 months. Age, gender, ethnicity and iris color were registered. All patients underwent the same follow-up protocol in every center: baseline visit, telephone consultation 2 weeks later and office controls at 4, 8 and 12 months. At each visit, best-corrected visual acuity, and cycloplegic autorefraction were assessed. Axial length (AL), anterior chamber depth and pupil diameter were measured on an IOL Master (Carl Zeiss Meditec, Inc, Dublin, CA). Adverse effects were registered in a specific questionnaire. Mean changes in cycloplegic SE and AL in the 12 months follow-up were analyzed. SE progression during treatment was compared with the SE progression in the year before enrollment for each patient. Correlation between SE and AL, and annual progression distribution were evaluated. Progression risk factors were analyzed by multivariate logistic regression analyses. Of the 105 recruited children, 92 completed the treatment. Mean SE and AL changes were - 0.44 ± 0.41 D and 0.27 ± 0.20 mm respectively. Mean SE progression was lower than the year before treatment (- 0.44 ± 0.41 D versus - 1.01 ± 0.38 D; p < 0.0001). An inverse correlation between SE progression and AL progression (r: - 0.42; p < 0.0001) was found. Fifty-seven patients (62%) had a SE progression less than - 0.50 D. No risk factors associated with progression could be identified in multivariate analyses. Mean pupil diameter increment at 12-months visit was 0.74 ± 1.76 mm. The adverse effects were mild and infrequent, and decreased over the time. Atropine 0.01% is effective and safe for myopia progression control in a multicentric Spanish children cohort. We believe this efficacy might be extensible to the myopic pediatric population from Western countries with similar social and demographic features. More studies about myopia progression risk factors among atropine treated patients are needed.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
The control over the chemical and electronic properties of carbon nitride‐based materials is highly challenging due to limitations of the traditionally used solid‐state reaction. Tailoring ...parameters, such as morphology, surface area, or energy band positions, in this kind of materials is essential for the improvement of the overall performance in a given application, namely photo‐ or electrocatalysis, sensing, or water treatment, amongst others. The supramolecular preorganization of carbon‐nitrogen based monomers via non‐covalent interactions prior to the thermal condensation has made it possible to design graphitic carbon nitride‐like (CN) materials and target specific properties. In this review, we discuss the latest developments in the synthesis of CN and other carbon‐based materials from the supramolecular preorganization of monomers and the consequences on the photocatalytic performance. The monomer sequence, solvent, and reaction conditions which determine the final structure of the supramolecular assembly, and therefore the final CN properties after calcination, are thoroughly discussed.
This Review describes the synthesis of carbon nitride materials by using ordered supramolecular assemblies as reactants. The tailored design of the chemical, photophysical and catalytic properties of carbon nitride materials after calcination by smart supramolecular assemblies design are thoroughly discussed.
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FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UL, UM, UPUK
Graphitic carbon nitride materials (CNs) have emerged as suitable photocatalysts and heterogeneous catalysts for various reactions thanks to their tunable band gap, suitable energy‐band position, ...high stability under harsh chemical conditions, and low cost. However, the utilization of CN in photoelectrochemical (PEC) and photoelectronic devices is still at an early stage owing to the difficulties in depositing high‐quality and homogenous CN layer on substrates, its wide band gap, poor charge‐separation efficiency, and low electronic conductivity. In this Minireview, we discuss the synthetic pathways for the preparation of various structures of CN on substrates and their underlying photophysical properties and current photoelectrochemical performance. The main challenges for CN incorporation into PEC cell are described, together with possible routes to overcome the standing limitations toward the integration of CN materials in PEC and other photoelectronic devices.
At the coalface: The advantages, drawbacks, and prospects of using polymeric graphitic carbon‐nitride based materials as the active components in water‐splitting photoelectrochemical cells is reviewed and discussed.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Biomass is recognized as an ideal CO2 neutral, abundant, and renewable resource substitute to fossil fuels. The rich proton content in most biomass derived materials, such as ethanol, ...5‐hydroxymethylfurfural (HMF) and glycerol allows it to be an effective hydrogen carrier. The oxidation derivatives, such as 2,5‐difurandicarboxylic acid from HMF, glyceric acid from glycerol are valuable products to be used in biodegradable polymers and pharmaceuticals. Therefore, combining biomass‐derived compound oxidation at the anode and hydrogen evolution reaction at the cathode in a biomass electrolysis or photo‐reforming reactor would present a promising strategy for coproducing high value chemicals and hydrogen with low energy consumption and CO2 emissions. This review aims to combine fundamental knowledge on photo and electro‐assisted catalysis to provide a comprehensive understanding of the general reaction mechanisms of different biomass‐derived molecule oxidation. At the same time, catalyst requirements and recent advances for various feedstock compounds are also reviewed in detail. Technoeconomic assessment and life cycle analysis are performed on various feedstocks to assess the relative benefits of various processes, and finally critical prospects are given on the challenges and opportunities for technology development to meet the sustainability requirement of the future global energy economy.
This review summarizes recent research progress in photo‐ and electrochemical oxidation of biomass feedstocks for the production of chemicals and hydrogen. High‐level technoeconomic assessment and life cycle analysis are performed to evaluate the economic value and environmental impact of biomass electrolysis. Based on the outcomes, perspectives on current technical challenges and future opportunities are provided.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Abstract
To evaluate the age-related efficacy and safety of atropine 0.01% eye drops over 2 years for myopia control in a multicentric pediatric Spanish cohort. A non-controlled, interventional, ...prospective multicenter study was conducted as an extension of the Spanish Group of Atropine Treatment for Myopia Control Study (GTAM 1). Children aged 6–14 years with myopia from − 2.00 to − 6.00 D, astigmatism < 1.50 D and documented annual myopic progression of at least − 0.50 D under cycloplegic examination were recruited. From the original cohort of 105 participants, 92 children who had been receiving atropine 0.01% eye drops once nightly in each eye for 1 year continued their participation in this extended study (GTAM 2). All the patients underwent a standardized quarterly follow-up protocol, which included measurements of best-corrected visual acuity (BCVA), cycloplegic autorefraction, axial length (AL), anterior chamber depth (ACD), and pupil diameter. The study sample was divided into three age groups: 6–8, 9–11, and 12–14 years old. The mean change in cycloplegic spherical equivalent (SE) and axial length (AL) during the 24 months of follow-up was analyzed. Correlations between SE and AL, as well as the distribution of annual progression, were evaluated. Adverse effects were recorded using a specific questionnaire. Finally, 81 children completed the follow-up and were included in the analysis. Over the 2-year period, the mean changes in SE and AL were − 0.88 ± 0.60 D and 0.49 ± 0.25 mm, respectively. Additionally, 51 patients (63%) experienced SE annual progression lower than − 0.50 D. The correlation between the progression of SE and AL during the total period of treatment was mild (r = − 0.36; p < 0.001). There were no differences between the first and the second year of treatment in the progression of SE (− 0.42 ± 0.41 D versus − 0.45 ± 0.39 D; p = 0.69) or AL (0.25 ± 0.16 mm versus 0.23 ± 0.14 mm; p = 0.43). Older patients (12–14 years old) showed less AL progression than younger children (6–8 years old): 0.36 ± 0.18 mm versus 0.59 ± 0.30 mm; p = 0.01. Adverse effects were mild, infrequent, and decreased over time. On average, the myopia progression in control groups from other published biannual studies exceeded that observed in our study. Over 2 years, atropine 0.01% demonstrated a safe treatment for controlling myopia progression in a multicentric cohort of Spanish children. The effect remained stable during this period. Older patients exhibited a more favorable response in terms of AL enlargement. However, further studies are needed to investigate the age-related effect of low-dose atropine in the Caucasian population.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Abstract
A general synthesis of carbon nitride (CN) films with extended optical absorption, excellent charge separation under illumination, and outstanding performance as a photoanode in ...water-splitting photoelectrochemical cells is reported. To this end, we introduced a universal method to rapidly grow CN monomers directly from a hot saturated solution on various substrates. Upon calcination, a highly uniform carbon nitride layer with tuned structural and photophysical properties and in intimate contact with the substrate is obtained. Detailed photoelectrochemical and structural studies reveal good photoresponse up to 600 nm, excellent hole extraction efficiency (up to 62%) and strong adhesion of the CN layer to the substrate. The best CN photoanode demonstrates a benchmark-setting photocurrent density of 353 µA cm
−2
(51% faradaic efficiency for oxygen), and external quantum yield value above 12% at 450 nm at 1.23 V versus RHE in an alkaline solution, as well as low onset potential and good stability.
We report the facile and environmental-friendly synthesis of an efficient carbon nitride photocatalyst for hydrogen production and dyes degradation by using a unique supramolecular assembly with an ...element gradient as the reactant. The element gradient is acquired through the selective removal of barbituric acid from the surface of a supramolecular assembly that comprises barbituric acid, melamine, and cyanucric acid, using hydrochloric acid as a surface modifier. The tailored design of the supramolecular aggregate results in inner and outer parts, which have carbon-rich and carbon-poor domains, respectively. Structural and optical investigations of the new assemblies reveal that the hydrogen–chlorine interaction generates a carbon gradient through the starting supramolecular assembly and to a better packing and structural alignment of the supramolecular units. Detailed X-ray photoelectron spectroscopy and photophysical studies of the final carbon nitride-like materials after calcination at 550 °C indicate that the element gradient across the starting precursor directly projects on the final carbon nitride chemical and element composition, as well as on its optical and photocatalytic properties. The spatial arrangement of the starting monomers leads to the formation of a unique energy-level structure in the final material, which is intended to improve the efficiency of charge separation under illumination and, thereby, result in a strong enhancement of photocatalytic activity toward a high hydrogen production and fast dyes degradation. This work provides new opportunities for the rational design of carbon nitride and other metal-free materials with unique and controllable chemical, optical, and catalytic properties for sustainable energy-related applications.
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IJS, KILJ, NUK, PNG, UL, UM
Herein we report the photocontrol of cucurbit8uril (CB8)-mediated supramolecular polymerization of azobenzene-containing monomers. The CB8 polymers were characterized both in solution and in the ...solid state. These host–guest complexes can be reversibly switched between highly thermostable photostationary states. Moreover, a remarkable stabilization of Z-azobenzene was achieved by CB8 complexation, allowing for structural characterization in the solid state.
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Thermoresponsive materials are generating significant interest on account of the sharp and tunable temperature deswelling transition of the polymer chain. Such materials have shown promise in drug ...delivery devices, sensing systems, and self-assembly. Incorporation of nanoparticles (NPs), typically through covalent attachment of the polymer chains to the NP surface, can add additional functionality and tunability to such hybrid materials. The versatility of these thermoresponsive polymer/nanoparticle materials has been shown previously; however, significant and important differences exist in the published literature between virtually identical materials. Here we use poly(N-isopropylacrylamide) (PNIPAm)-AuNPs as a model system to understand the aggregation behavior of thermoresponsive polymer-coated nanoparticles in pure water, made by either grafting-to or grafting-from methods. We show that, contrary to popular belief, the aggregation of PNIPAm-coated AuNPs, and likely other such materials, relies on the size and concentration of unbound “free” PNIPAm in solution. It is this unbound polymer that also leads to an increase in solution turbidity, a characteristic that is typically used to prove nanoparticle aggregation. The size of PNIPAm used to coat the AuNPs, as well as the concentration of the resultant polymer–AuNP composites, is shown to have little effect on aggregation. Without free PNIPAm, contraction of the polymer corona in response to increasing temperature is observed, instead of nanoparticle aggregation, and is accompanied by no change in solution turbidity or color. We develop an alternative method for removing all traces of excess free polymer and develop an approach for analyzing the aggregation behavior of such materials, which truly allows for heat-triggered aggregation to be studied.
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The rational design of ultralong carbon nitride nanostructures is highly attractive due to their high aspect ratio alongside their high surface-to-bulk ratio, which make them suitable candidates for ...various applications such as photocatalysts, water treatment, and sensors. However, the synthesis of ultralong, continuous carbon nitride wires is highly challenging. Here we report the synthesis of 4 cm long and large lateral size carbon nitride wires by utilizing unique supramolecular spheres composed of graphitic carbon nitride (g-CN) monomers as the reactants. In situ scanning electron microscopy studies reveal that upon calcination the g-CN wires spontaneously start to grow from the spheres, while the remaining assembly which acts as a substrate creates self-standing carbon-rich g-CN porous films. The different morphology, chemical composition, and electronic properties of the wires and carbon-rich g-CN allow their utilization as both photocatalyst and water cleaning materials. The g-CN wires exhibit excellent photoactivity for hydrogen production whereas the porous carbon-rich g-CN porous film can be efficiently used for water cleaning applications. The reported work opens opportunities for tailored design of g-CN nanostructures and their use as multifunctional materials for photocatalysis, sensing, and other energy-related applications.
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