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1.
Spectrochim Acta A Mol Biomol Spectrosc ; 324: 124942, 2025 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-39128386

RESUMO

Long-term and excessive use of tetracycline hydrochloride (TC) can lead to its accumulation in the environment, which can cause water contamination, bacterial resistance, and food safety problems. 2,6-Pyridine dicarboxylic acid (DPA) is a major biomarker of Bacillus anthracis spores, and its rapid and sensitive detection is of great significance for disease prevention and counter-terrorism. A bifunctional ratiometric fluorescent nanoprobe has been fabricated to detect DPA and TC. 3,5-dicarboxyphenylboronic acid (BOP) was intercalated into layered europium hydroxide (LEuH) by the ion-exchange method and exfoliated into nanosheets as a fluorescent nanoprobe (PNP). DPA and TC could significantly enhance the red fluorescence of Eu3+ through the antenna effect under different excitation wavelengths, while the fluorescence of BOP can be used as a reference based on the constant emission intensity, realizing ratiometric detection. A low limit of detection (LOD) for the target (DPA: 9.7 nM, TC: 21.9 nM) can be achieved. In addition, visual detection of DPA and TC was realized using color recognition software based on the obvious color changes. This is the first ratiometric fluorescent nanoprobe based on layered rare-earth hydroxide (LRH) for the detection of DPA and TC simultaneously, which opens new ideas in the design of multifunctional probes.


Assuntos
Bacillus anthracis , Biomarcadores , Corantes Fluorescentes , Espectrometria de Fluorescência , Esporos Bacterianos , Tetraciclina , Corantes Fluorescentes/química , Espectrometria de Fluorescência/métodos , Bacillus anthracis/isolamento & purificação , Biomarcadores/análise , Tetraciclina/análise , Limite de Detecção , Ácidos Picolínicos/análise , Antraz/diagnóstico
2.
Artigo em Inglês | MEDLINE | ID: mdl-39312398

RESUMO

The integration of the hydrogen evolution reaction (HER) with the methanol oxidation reaction (MOR) has been demonstrated to be a viable strategy for the energy-saving generation of H2 and value-added formate, which relies primarily on highly active and cost-effective bifunctional electrocatalysts. Herein, an efficient electrocatalyst consisting of controllable Ni nanoparticles (NPs) coated with ultrathin graphitic carbon shells was obtained by the pyrolysis of a Ni-Zn metal-organic framework. Intriguingly, we found that zinc vaporization not only resulted in the relatively small Ni NPs but also ultrathin carbon shells (≤3 layers). The density functional theory simulations confirmed that these ultrathin carbon shells significantly influenced electrocatalytic activity by facilitating electron transfer from the Ni core to the carbon shell. The optimized Ni1(Zn)@C demonstrated high catalytic activity for both HER and MOR, and only a low potential of 97 mV at 10 mA cm-2 was required for HER and 1.48 V at 30 mA cm-2 for MOR. In a two-electrode electrocatalytic cell measurement, a cell voltage of 1.63 V was observed at 10 mA cm-2 in the presence of methanol, 240 mV lower than that without methanol.

3.
ChemSusChem ; : e202401930, 2024 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-39315907

RESUMO

Currently one-pot conversion of sugars to 2,5-furandicarboxylic acid (FDCA) is of significant interest due to the attainability of sugars as a feedstock and the enormous potential of FDCA as a bioplastic monomer. However, it remains challenging to construct efficient catalysts for this process. In this study, Co3O4 species were anchored to a sulfonated covalent organic framework thus affording a bifunctional catalyst (Co3O4@COF-SO3H). The sulfonic acid sites dehydrate sugars to 5-hydroxymethylfurfural (HMF), which is next oxidized to FDCA as catalyzed by the Co3O4 species. Such a process was applied in the conversion of various binary and ternary deep eutectic mixtures involving choline chloride and sugars without additional solvent. The maximum FDCA yield of 84% was obtained using glucose-fructose eutectic mixture as the substrates. Moreover, the catalyst was recyclable and stable under the applied reaction conditions. Our process eliminates the employment of organic solvents and expensive noble metal catalysts, resulting in green and economic biomass conversions.

4.
Eur J Med Chem ; 279: 116919, 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39342682

RESUMO

Fibroblast activation protein-α (FAPα) is highly expressed in tumor-associated cells and has become one of the most attractive targeting sites in cancer diagnosis and therapy. To ameliorate the rapid metabolism of FAPα inhibitor (FAPI), here, a multifunctional binding agent was introduced to simultaneously achieve 211At radiolabeling and tumor retention prolongation of corresponding radiolabeled drug. 211At-APBA-FAPI was successfully synthesized by conjugating 211At with the designed FAPI carrier in satisfactory radiochemical yield (>60 %). 211At-APBA-FAPI exhibited excellent in vitro stability, significant tumor affinity and specific killing effect on FAPα-positive U87MG cells. Molecular docking reveals that FAPI decorated with albumin binder can bind with FAPα protein via multiple intermolecular interactions with a considerable binding energy of -9.66 kcal/mol 211At-APBA-FAPI exhibits good targeting in murine xenograft models, showing obviously longer tumor retention than previously-reported radioastatinated compound. As a result, 211At-APBA-FAPI presents pronounced therapeutic effect with ignorable normal organs/tissues biotoxicity. All these indicate that introducing a multifunctional binding agent can effectively enhance the availability of FAPI for 211At conjugation and tumoricidal effect, providing vital hints for the translation of targeted-alpha therapy based on radiolabeled FAPI derivatives.

5.
Drug Discov Today ; : 104194, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39343161

RESUMO

Post-translational modifications (PTMs) of proteins are crucial for regulating biological processes and their dysregulation is linked to various diseases, highlighting PTM regulation as a significant target for drug development. Traditional drug targets often interact with multiple proteins, resulting in lower selectivity and inevitable adverse effects, which limits their clinical applicability. Recent advancements in bifunctional molecules, such as proteolysis-targeting chimeras (PROTACs), have shown promise in targeting PTMs precisely. However, regulatory mechanisms for many of the >600 known PTMs remain underexplored. This review examines current progress and challenges in designing bifunctional molecules for PTM regulation, focusing on effector selection and ligand design strategies, aiming to propel the utilization and advancement of bifunctional molecules to the forefront of PTM research.

6.
Drug Dev Res ; 85(6): e22258, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39253992

RESUMO

The 2-nitroimidazole based 99mTc-radiopharmaceuticals are widely explored for imaging tumor hypoxia. Radiopharmaceuticals for targeting hypoxia are often lipophilic and therefore, show significant uptake in liver and other vital organs. In this context, lipophilic radiopharmaceuticals with design features enabling faster clearance from liver may be more desirable. A dipicolylamine-NCS bifunctional chelator that could generate a thiourea-bridge up on conjugation to primary amine bearing molecule was used to synthesize a 2-nitroimidazole-dipicolyl amine ligand for radiolabeling with 99mTc(CO)3 core. Corresponding Re(CO)3-analogue was prepared to establish the structure of 2-nitroimidazole-99mTc(CO)3 complex prepared in trace level. The 2-nitroimidazole-99mTc(CO)3 complex showed a hypoxic to normoxic ratio of ~2.5 in CHO cells at 3 h. In vivo, the complex showed accumulation and retention in tumor with high tumor to blood and tumor to muscle ratio. The study demonstrated the utility of metabolizable thiourea-bridge in 2-nitroimidazole-99mTc(CO)3 complex in inducing faster clearance of the radiotracer from liver. The dipicolylamine-NCS bifunctional chelator reported herein can also be used for radiolabeling other class of target specific molecules with 99mTc(CO)3 core.


Assuntos
Compostos Radiofarmacêuticos , Tioureia , Hipóxia Tumoral , Animais , Compostos Radiofarmacêuticos/farmacocinética , Células CHO , Tioureia/análogos & derivados , Tioureia/farmacocinética , Tioureia/química , Cricetulus , Camundongos , Nitroimidazóis/farmacocinética , Nitroimidazóis/química , Compostos de Organotecnécio/farmacocinética , Compostos de Organotecnécio/química , Compostos de Organotecnécio/administração & dosagem , Distribuição Tecidual , Ácidos Picolínicos/farmacocinética , Ácidos Picolínicos/química , Humanos , Tecnécio
7.
Chemistry ; : e202402341, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-39278832

RESUMO

D-Glucose-to-L-sorbose isomerization on Lewis acidic zeolite is a highly attractive avenue for sorbose production. But the L-sorbose yield is limited by the competing D-glucose-to-D-fructose isomerization and reaction equilibrium. In this work, it is suggested that ethanol directs the glucose conformation for selective D-glucose-to-L-sorbose isomerization. It also reacts with the produced L-sorbose to form ethyl-sorboside, which allows the D-glucose-to-L-sorbose isomerization to proceed beyond the thermodynamic equilibrium limit.  It is shown that a bifunctional zeolite Beta containing framework titanium (Ti) and boron (B) is a selective catalyst for this tandem reaction: Lewis acidic framework Ti catalyzes the D-glucose-to-L-sorbose isomerization via an intramolecular 5,1-hydride shift process as confirmed by isotopic tracing experiments followed by 13C-NMR, while weak Brønsted acid framework B selectively promotes the sorbose ketalization with ethanol. A remarkably high yield of L-sorbose with a high fraction of sugar (>95%: 27% unreacted glucose, 11.4% fructose, 57% sorbose) was obtained after the mixture produced in ethanol was hydrolyzed.

8.
Membranes (Basel) ; 14(9)2024 Aug 23.
Artigo em Inglês | MEDLINE | ID: mdl-39330523

RESUMO

In this study, an ionic liquid-based polymer inclusion membrane (IL-PIM) made of (50% polymer-50% CyphosIL104) was used to extract and separate the rare earth elements (REEs) Y, La, Nd, and Sm in chloride solutions. The effect of extraction time and pH was studied to optimize the extraction and separation conditions. The four REEs were effectively extracted at pH 4-5 from both single and mixed metals solutions. However, at pH 2, only Y was extracted. The recovery of the extracted REEs from the loaded PIM was achieved using HNO3 and H2SO4. In the case of La, it was quantitatively back-extracted with H2SO4 after a contact time of 1 h, while up to 4 h was necessary to recover 70% of the extracted Y, Sm, and Nd. Extraction isotherms were studied, and the Freundlich isotherm model was the most adequate to describe the interaction between the PIM and the REEs. Finally, the developed PIM was investigated for the extraction of REEs from mixtures containing other metals, which showed great selectivity for the REEs.

9.
ACS Chem Biol ; 2024 Sep 26.
Artigo em Inglês | MEDLINE | ID: mdl-39325690

RESUMO

Recent advances in the field of translational chemical biology use diverse "proximity-inducing" synthetic modalities to elicit new modes of "event driven" pharmacology. These include mechanisms of targeted protein degradation and immune clearance of pathogenic cells. Heterobifunctional "chimeric" compounds like Proteolysis TArgeting Chimeras (PROTACs) and Antibody Recruiting Molecules (ARMs) leverage these mechanisms, respectively. Both systems function through the formation of reversible "ternary" or higher-order biomolecular complexes. Critical to function are key parameters, such as bifunctional molecule affinity for endogenous proteins, target residence time, and turnover. To probe the mechanism and enhance function, covalent chemical approaches have been developed to kinetically stabilize ternary complexes. These include electrophilic PROTACs and Covalent Immune Recruiters (CIRs), the latter designed to uniquely enforce cell-cell induced proximity. Inducing cell-cell proximity is associated with key challenges arising from a combination of steric and/or mechanical based destabilizing forces on the ternary complex. These factors can attenuate the formation of ternary complexes driven by high affinity bifunctional/proximity inducing molecules. This Account describes initial efforts in our lab to address these challenges using the CIR strategy in antibody recruitment or receptor engineered T cell model systems of cell-cell induced proximity. ARMs form ternary complexes with serum antibodies and surface protein antigens on tumor cells that subsequently engage immune cells via Fc receptors. Binding and clustering of Fc receptors trigger immune cell killing of the tumor cell. We applied the CIR strategy to convert ARMs to covalent chimeras, which "irreversibly" recruit serum antibodies to tumor cells. These covalent chimeras leverage electrophile preorganization and kinetic effective molarity to achieve fast and selective covalent engagement of the target ternary complex protein, e.g., serum antibody. Importantly, covalent engagement can proceed via diverse binding site amino acids beyond cysteine. Covalent chimeras demonstrated striking functional enhancements compared to noncovalent ARM analogs in functional immune assays. We revealed this enhancement was in fact due to the increased kinetic stability and not concentration, of ternary complexes. This finding was recapitulated using analogous CIR modalities that integrate peptidic or carbohydrate binding ligands with Sulfur(VI) Fluoride Exchange (SuFEx) electrophiles to induce cell-cell proximity. Mechanistic studies in a distinct model system that uses T cells engineered with receptors that recognize covalent chimeras or ARMs, revealed covalent receptor engagement uniquely enforces downstream activation signaling. Finally, this Account discusses potential challenges and future directions for adapting and optimizing covalent chimeric/bifunctional molecules for diverse applications in cell-cell induced proximity.

10.
J Colloid Interface Sci ; 678(Pt C): 968-976, 2024 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-39326168

RESUMO

The development of sustainable energy technologies relies on the exploitation of efficient and durable electrocatalysts for water splitting at high current densities. Our work presents a novel bifunctional catalyst, denoted as NM@NC/CC, which combines the benefits of NiSe2-MoSe2 heterojunctions with nitrogen-enriched porous carbon derived from metal-organic frameworks (MOFs). The integration of these components is designed to harness their combined advantages, which include enhanced electron transfer, improved mass and gas evolution dynamics, and an increased number of catalytically active sites. These features collectively optimize the energetics for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). As a result, the catalyst facilitates rapid kinetics for the overall water-splitting process. The NM@NC/CC demonstrates low overpotentials, requiring only 91 mV for the HER and 280 mV for the OER to reach a current density of 10 mA cm-2. Even at higher current densities of 100 mA cm-2 for HER and 50 mA cm-2 for OER, the overpotentials are only 159 mV and 350 mV, respectively. Additionally, a two-electrode setup using this catalyst achieves a current density of 10 mA cm-2 with a minimal cell voltage of 1.56 V. The insights gained from this study will contribute to the advancement of electrocatalysts for energy conversion technologies.

11.
Mikrochim Acta ; 191(10): 628, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39327334

RESUMO

Stainless steel sheets were coated with carbon ink to obtain disposable carbon electrodes, which were used as supports for moleculary imprinted polymer (MIP) electrochemical sensors by electropolymerizing o-phenylenediamine and o-aminophenol along with indole-3-acetic acid (IAA) as the template. After optimization, the MIP biosensors could be used for sensitive and selective detection of IAA with the limit of quantification of 0.1 µM. Our experimental results showed that stable and reproducible electrochemical responses could be achieved for the disposable MIP biosensors. This approach was successfully used for detection of IAA in different tissues of pea sprouts. This study reveals the potential of MIP electrochemical sensors in practical applications and shrinks the trench between the research and the real world.

12.
Chemosphere ; 364: 143309, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39265733

RESUMO

Herein, coupling of noble metal-free plasmonic copper nanoparticles with tungsten suboxide and supporting on zeolite nanoclay (Cu/WO3-x@ZNC) composite will be introduced for bi-functional photocatalytic ciprofloxacin (CIP) degradation and water photothermal evaporation under visible/infrared (Vis/IR) exposure. Reduced band-gap of WO3-x via oxygen vacancies creation and localized surface plasmon resonance (LSPR) formation by Cu nanoparticles contributed significantly the extension and intensification of composite's photo-absorption range. Furthermore, small mesoporous structure of ZNC enhanced CIP adsorption and charge carriers separation where the reported photocatalytic efficiencies were 88.3 and 81.7% upon IR and Vis light exposure respectively. It was evidenced that plasmonic hot electrons (e-.s) and hydroxyl radicals (OH•-) performed the basic functions of the photocatalytic process. At the other side, oxygen vacancies existence, plasmonic effect, and confining thermal characteristics of WO3-x, Cu, and ZNC correspondingly induced water photothermal evaporation with efficiencies up to 97.5 and 72.8% under IR and Vis illumination respectively. This work introduces synthesis of a novel bi-functional photocatalytic-photothermal composite by metal sub-oxide and non-noble metal plasmonic coupling and supporting on naturally-derived carrier for water restoration under broad spectral exposure.


Assuntos
Ciprofloxacina , Cobre , Tungstênio , Ciprofloxacina/química , Cobre/química , Tungstênio/química , Catálise , Poluentes Químicos da Água/química , Óxidos/química , Nanopartículas Metálicas/química , Água/química , Zeolitas/química , Raios Infravermelhos , Fotólise , Processos Fotoquímicos , Ressonância de Plasmônio de Superfície , Adsorção
13.
Mol Genet Metab Rep ; 41: 101137, 2024 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-39282052

RESUMO

D-bifunctional protein (DBP) deficiency, a fatal peroxisomal enzyme disorder, typically manifests with life-threatening symptoms in the first two years of childhood. We present the case of an infant with elevated lysophosphatidylcholine C26:0 (C26:0-LPC) levels identified during X-linked adrenoleukodystrophy (ALD) screening, leading to a diagnosis of DBP deficiency due to a homozygous HSD17B4 c.1041T>A, p.(Tyr347Ter) variant. Starting at two months of age, the infant experienced seizures, hypotonia, and developmental delays, prompting the initiation of experimental treatment with the readthrough agent PTC124 (ataluren) at six months. The treatment led to a decrease in C26:0-LPC levels from 0.65 µM to 0.53 µM; concomitant fish oil supplementation transiently increased C26:0-LPC to 0.74 µM before returning to 0.53 µM after cessation of supplementation. The patient demonstrated improved swallowing and progressive motor and speech development during a two-year treatment period, with no further seizures. This case report highlights the potential of nonsense readthrough therapy for peroxisomal disorders, a group of metabolic diseases that currently lack targeted treatments.

14.
Heliyon ; 10(17): e37134, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-39286105

RESUMO

Radioactive Cs+ and I- ions are major components of nuclear wastewater, typically existing as counter ions. Due to their high water solubility and mobility, these ions can spread through contaminated water and soil into ecosystems, necessitating continuous removal and management. In this study, we synthesized a reusable bifunctional Ni@Pt/K2NiFe(CN)6 composite that can simultaneously remove radioactive Cs+ and I- ions and, for the first time, enable their separate recovery in aqueous solutions. In this material, K2NiFe(CN)6 acted as an electrochemically switched ion exchanger, controlling the adsorption/desorption of Cs+, while Pt enabled the spontaneous adsorption and electrochemical desorption of I-, and the magnetic Ni core allowed for efficient adsorbent recovery. The adsorption isotherms of both Cs+ and I- were best fitted using the Langmuir model, and the corresponding adsorption capacities were comparable to those of conventional adsorbents used for the separate removal of Cs+ and I-. Furthermore, the composite demonstrated stability over 100 sorption cycles, maintaining high recovery efficiencies of 97.9 % for Cs+ and 99.7 % for I-, thereby proving its reusability. Thus, the developed composite holds great promise for radioactive wastewater treatment and environmental restoration.

15.
Small ; : e2403336, 2024 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-39221547

RESUMO

In the quest for efficient and stable oxygen evolution catalysts (OECs) for photoelectrochemical water splitting, the surface modification of BiVO4 is a crucial step. In this study, a novel and robust OEC, based on 3-(bis(pyridin-2-ylmethyl) amino) propanoic acid bifunctional linker known as dipicolyl alanine acid (DPAA) and cobalt ions, is prepared and fully characterized. The DPAA is anchored to the surface of BiVO4 and utilized to tether cobalt ions. The Co-DPAA/BiVO4 photoanode exhibits remarkable stability and efficiency toward photoelectrochemical water oxidation. Specifically, it showed anodic photocurrent increase of 7.1, 5.0, 3.0, and 1.3-fold at 1.23 VRHE as compared to pristine BiVO4, DPAA/BiVO4, Co-BiVO4, and Co-Pi/BiVO4 photoanodes, respectively. The photoelectrochemical and IMPS studies revealed that the Co-DPAA/BiVO4 photoanode exhibits a longer transient decay time for surface-trapped holes, higher charge transfer kinetics, and charge separation efficiency compared to Co-Pi/BiVO4 and pristine BiVO4 photoelectrodes. This indicates that the Co-DPAA effectively reduces surface recombination and facilitates charge transfer. Moreover, at 1.23 VRHE, the Co-DPAA/BiVO4 photoanode achieved a faradic efficiency of 92% for oxygen evolution reaction and could retain a turnover frequency of 3.65 s-1. The- exhibited effeciency is  higher than most of the efficient molecular oxygen evolution catalyst based on Ru.

16.
J Colloid Interface Sci ; 678(Pt A): 970-978, 2024 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-39226837

RESUMO

Designing highly effective, low-cost bifunctional electrocatalysts without noble metals for overall water splitting remains a significant challenge. In this work, interfacial coupling of Ce-doped CoSe2 nanoneedle arrays with MXene (Ce-CoSe2/MXene) is developed via the facile hydrothermal and selenization methods. The extensive specific surface area and favorable hydrophilicity of Ti3AlC2, combined with the optimized electronic structure and abundant active sites from Ce-doping and selenization, contribute to the exceptional bifunctional electrocatalytic performance of the Ce-CoSe2/MXene electrode. Specifically, this heterostructure achieves a low hydrogen evolution reaction (HER) overpotential of 34 mV at 10 mA cm-2, an oxygen evolution reaction (OER) overpotential of 279 mV at 100 mA cm-2, and an overall water splitting (OWS) potential as low as 1.45 V at 10 mA cm-2. In-situ Raman spectroscopy reveals that surface reconstruction would improve catalytic activity and stability. Theoretical calculations indicate that the Ce-CoSe2/MXene can improve the adsorption of intermediates and facilitate HER/OER process by lowering the kinetic barrier, thereby enhancing electrocatalytic activity. This research marks a substantial advancement in the development of low-cost, efficient electrocatalysts for overall water splitting.

17.
Small Methods ; : e2401139, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39235422

RESUMO

The development of bifunctional, non-noble metal-based electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) through morphology and electronic engineering is highly attractive for efficient water splitting. Herein, hierarchical nanoarrays consisting of crystalline cobalt phosphide nanorods covered by amorphous Fe-doped cobalt phosphide nanocuboids (CoP/FeCoPx) are constructed as bifunctional catalysts for both HER and OER. Experimental results and theoretical calculations reveal that the catalysts exhibit balanced dual-catalytic properties due to simultaneous introduction of Fe doping and phosphorus vacancies, leading to an optimized electronic structure of the CoP/FeCoPx. Furthermore, the hierarchical nanoarrays made of crystalline/amorphous heterostructures significantly enhance the performance of the electrocatalysts. As a result, the CoP/FeCoPx catalyst demonstrates remarkable performance in both HER and OER, with overpotentials of 74 and 237 mV at 10 mA cm-2 in 1 m KOH, respectively, as well as a low cell voltage of 1.53 V at 10 mA cm-2 for alkaline overall water splitting. This work integrates the morphology engineering involving design of hierarchical crystalline/amorphous nanoarrays and the electronic engineering through Fe doping and phosphorus vacancies for efficient water electrolysis. It may open a new route toward rational design and feasible fabrication of high-performance, multifunctional, non-noble metal-based electrocatalysts for energy conversion.

18.
Chem Asian J ; : e202400969, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39295253

RESUMO

The impact of surface area, pore volume, and heteroatom type on the performance of porous organic polymers (POPs) in various applications remains unclear. To investigate this, three isoreticular POPs were employed having one common building block, resulting in varying surface areas, pore volumes, and heteroatom compositions. This study aimed to establish a correlation between the structural features of POPs (surface area, pore volume, and heteroatom type) with their adsorption capacity, and catalytic efficiency. To explore this relationship, the Knoevenagel condensation reaction was used as a model system, testing various substituted aldehydes to further validate our findings. Additionally, the capture of radioactive iodine vapor at 75°C was simulated to examine the correlation with adsorption capacity, comparing the gravimetric iodine uptake capacity of each POP to gain insights into this relationship.

19.
ACS Appl Mater Interfaces ; 16(37): 49349-49361, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39230248

RESUMO

With the intensification of global environmental pollution and resource scarcity, hydrogen has garnered significant attention as an ideal alternative to fossil fuels due to its high energy density and nonpolluting nature. Consequently, the urgent development of electrocatalytic water-splitting electrodes for hydrogen production is imperative. In this study, a superwetting selenide catalytic electrode with a peony-flower-shaped micronano array (MoS2/Co0.8Fe0.2Se2/NixSey/nickel foam (NF)) was synthesized on NF via a two-step hydrothermal method. The optimal catalytic activity of cobalt-iron selenide was achieved by adjusting the Co/Fe ratio. The intrinsic catalytic activity of the electrodes was enhanced by incorporating transition metal selenides, which then served as a precursor for the subsequent loading of MoS2 nanoflowers on the surface to fully expose the active sites. Furthermore, the superwetting properties of the electrode accelerated electrolyte penetration and electron/mass transfer, while also facilitating bubble detachment from the electrode surface, thereby preventing "bubble shielding effect". This resulted in superior oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance, as well as overall water splitting capabilities. In a 1.0 M KOH solution, the electrode required only 166 and 195 mV overpotential to achieve a current density of 10 mA cm-2 for OER and HER, respectively. When functioning as a bifunctional catalytic electrode, only 1.60 V of voltage was necessary to drive the electrolyzer to reach a current density of 10 mA cm-2. Moreover, laboratory simulations of wind and solar energy-driven water splitting validated the feasibility of establishing a sustainable energy-to-hydrogen production chain. This work provides new insights into the preparation of low-overpotential, high-catalytic-activity superhydrophilic and underwater superaerophobic catalytic electrodes by rationally adjusting elemental ratios and exploring changes in electrode surface wettability.

20.
J Colloid Interface Sci ; 678(Pt B): 828-841, 2024 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-39270384

RESUMO

The production of hydrogen gas as an environmentally friendly and emission-free fuel source, has emerged as the preeminent substitute for traditional fossil fuels. The demand for a viable and low-cost substitute of the anodic Oxygen Evolution Reaction (OER) in hydrogen gas production has led researchers to explore the Hydrazine Oxidation Reaction (HzOR), aiming to reduce overpotential. In this study, we present the synthesis of a NiSeP@NiCo/Cu electrocatalyst via electrodeposition method, offering precise control over parameter adjustments and an affordable price. The binder-free nanosheet structure of this electrocatalyst demonstrates improved performance in water electrolysis, resulting in potentials of -40 and -134 mV vs. Reversible Hydrogen Electrode (RHE) for Hydrogen Evolution Reaction (HER) and 0.041 and 0.194 V (vs. RHE) for HzOR (i = 10 and 100 mA.cm-2). The electrode has excellent features, including active electrochemical surface, synergistic effects among the elements, high stability, super-hydrophilicity and super-aerophobicity. The Bi-functional performance of electrode was tested in a two-electrode set for HER/HzOR, the cell voltage required to reach current densities of 10 and 100 mA.cm-2 were determined as 0.071 and 0.298 V respectively. On the whole, this work presents the excellent capabilities of the synthesized electrode (NiSeP@NiCo/Cu) for hydrogen gas production.

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