With the increasing requirement for phosphorus resources and their shortage in nature, cyclic utilization of organophosphorus pollutants into phosphatic fertilizer might offer a sustainable approach to achieve the recycling of phosphorus. Herein, we first report the selective degradation of organophosphorus pollutants (such as HEDP and glyphosate), via the synergistic effect of peroxymonosulfate (PMS) and sodium percarbonate (SPC), into phosphates, which are continually converted into phosphatic fertilizer by struvite precipitation on the continuous-flow reactor. Quenching experiments, EPR result, electrochemical analysis, and DFT calculation suggest that the transfer of electrons from SPC to PMS results in the synthesis of catalytically active species (i.
View Article and Find Full Text PDFAdv Colloid Interface Sci
April 2025
Nanopore-based electrical detection technology holds single-molecule resolution and combines the advantages of high sensitivity, high throughput, rapid analysis, and label-free detection. It is widely applied in the determination of organic and biological macromolecules, small molecules, and nanomaterials, as well as in nucleic acid and protein sequencing. There are a wide variety of organic polymers and biopolymers, and their chemical structures, and conformation in solution directly affect their ensemble properties.
View Article and Find Full Text PDFPolymers and dendrimers are macromolecules, possessing unique and intriguing characteristics, that are widely applied in self-assembled functional materials, green catalysis, drug delivery and sensing devices. Traditional approaches for the structural characterization of polymers and dendrimers involve DLS, GPC, NMR, IR and TG, which provide their physiochemical features and ensemble information, whereas their unimolecular conformation and dispersion also are key features allowing to understand their transporting profile in confined ionic nanochannels. This work demonstrates the nanopore approach for the determination of charged homopolymers, neutral block copolymer and dendrimers under distinct bias potentials and pH conditions.
View Article and Find Full Text PDFElectrocatalytic carbon dioxide (CO) conversion into valuable chemicals paves the way for the realization of carbon recycling. Downsizing catalysts to single-atom catalysts (SACs), dual-atom catalysts (DACs), and sub-nanocluster catalysts (SNCCs) has generated highly active and selective CO transformation into highly reduced products. This is due to the introduction of numerous active sites, highly unsaturated coordination environments, efficient atom utilization, and confinement effect compared to their nanoparticle counterparts.
View Article and Find Full Text PDFDendrimers and supramolecular chemistry continue to fascinate researchers due to the endless unrevealed potential of their combination. This study investigates the self-assembly process of a series of hydrophobic triazolylferrocenyl dendrimers in aqueous medium. Deep investigation through NMR spectroscopy, absorption UV-vis spectroscopy along with theoretical simulations demonstrates that the ferrocenyl moieties interact intramolecularly and intermolecularly driving the self-assembly process.
View Article and Find Full Text PDFThis study explores the stabilization by niobic acid, of Pt, Ni, Pd, and Au nanoparticles (NPs) for the efficient microheterogeneous catalysis of NaBH hydrolysis for hydrogen production. Niobic acid is the most widely studied NbO polymorph, and it is employed here for the first time for this key reaction relevant to green energy. Structural insights from XRD, Raman, and FTIR spectroscopies, combined with hydrogen production data, reveal the role of niobic acid's Brønsted acidity in its catalytic activity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
The Cu-glutathione (GSH) redox system, essential in biology, is designed here as a supramacromolecular assembly in which the tetrahedral 18e Cu(I) center loses a thiol ligand upon adsorption onto ZIF-8, as shown by EXAFS and DFT calculation, to generate a very robust 16e planar trigonal single-atom Cu(I) catalyst. Synergy between Cu(I) and ZIF-8, revealed by catalytic experiments and DFT calculation, affords CO conversion into high-value-added chemicals with a wide scope of substrates by reaction with terminal alkynes or propargyl amines in excellent yields under mild conditions and reuse at least 10 times without significant decrease in catalytic efficiency.
View Article and Find Full Text PDFUnsaturated furanic aldehydes are derived from lignocellulosic biomass resources and subsequently used to produce valuable chemicals. However, the highly efficient, selective hydrogenation of the biomass-derived unsaturated furan CO bond remains challenging. Here we report that graphene-like nitrogen doped porous carbon (GNPC) nanosheets are synthesized from carbon-rich, sustainable, and renewable biomass precursors (glucose, fructose and 5-hydroxymethylfurfural, HMF) with high surface areas, large pore volumes and narrow mesopores.
View Article and Find Full Text PDFLignin, the most abundant natural material, is considered as a low-value commercial biomass waste from paper mills and wineries. In an effort to turn biomass waste into a highly valuable material, herein, a new-type of hollow carbon nanospheres (HCNs) is designed and synthesized by pyrolysis of biomass dealkali lignin, as an efficient nanocatalyst for the elimination of antibiotics in complex water matrices. Detailed characterization shows that HCNs possess a hollow nanosphere structure, with abundant graphitic C/N and surface N and O-containing functional groups favorable for peroxydisulfate (PDS) activation.
View Article and Find Full Text PDFElectrocatalytic transformation of CO to various syngas compositions is an exceedingly attractive approach to carbon-neutral recycling. Meanwhile, the achievement of selectivity, stability, and tunability of product ratios using single-component electrocatalysts is challenging. Herein, the theoretically-assisted design of the triple-component nanocomposite electrocatalyst CuSn-Cu-SnO that addresses this challenge is presented.
View Article and Find Full Text PDFFerrocene has been the most used organometallic moiety introduced in organic and bioinorganic drugs to cure cancers and various other diseases. Following several pioneering studies, two real breakthroughs occurred in 1996 and 1997. In 1996, Jaouen et al.
View Article and Find Full Text PDFThis review links various areas of inorganic chemistry around the themes developed by our research group during the last four decades. It is firstly based on the electronic structure of iron sandwich complexes, showing how the metal electron count dictates their reactivities, with various applications ( C-H activation, C-C bond formation) as reducing and oxidizing agents, redox and electrocatalysts and precursors of dendrimers and catalyst templates through bursting reactions. Various electron-transfer processes and consequences are explored, including the influence of the redox state on the acidity of robust ligands and the possibility to iterate C-H activation and C-C bond formation to build arene-cored dendrimers.
View Article and Find Full Text PDFHydrogen (H) generation and storage are actively investigated to provide a green source of energy, and formic acid (HCOOH), a major product obtained from the biomass, is regarded as a productive source of H. Therefore, improvements in heterogeneous catalysts are called for. Here, a novel type of catalyst support is proposed involving simple addition of the mixture of metal ion precursors to core-shell ZIF-8@ZIF-67, followed by reduction with NaBH, with performances surpassing those obtained using nanocatalysts in ZIF-8 or ZIF-67.
View Article and Find Full Text PDFObjectives: We aimed to evaluate (1) whether sedation analgesia (SA) used during therapeutic hypothermia (TH) was efficient to support the wellbeing of neonates with hypoxic-ischemic encephalopathy, (2) the SA level and its adjustment to clinical pain scores, and (3) the impact of inadequate SA on short-term neonatal outcomes evaluated at discharge.
Methods: This was an observational retrospective study performed between 2011 and 2018 in two level III centers in Alsace, France. We analyzed the wellbeing of infants by using the COMFORT-Behavior (COMFORT-B) clinical score and SA level during TH, according to which we classified infants into four groups: those with excess SA, adequate SA, lack of SA, and variability of SA.
Objective: To evaluate cytomegalovirus (CMV) viral load dynamics in blood and saliva during the first 2 years of life in symptomatic and asymptomatic infected infants and to identify whether these kinetics could have practical clinical implications.
Study Design: The Cymepedia cohort prospectively included 256 congenitally infected neonates followed for 2 years. Whole blood and saliva were collected at inclusion and months 4 and 12, and saliva at months 18 and 24.
Biomass valorization is essential, particularly in emerging countries. Here, hydrochar from arabica coffee straw was functionalized with a triazole group (HD-TRz) for use as a support of palladium nanoparticles (PdNPs-HD-TRz) applied in the Ullmann coupling reaction for the first time. It provided remarkably excellent selectivities, conversions at a temperature as low as 45 °C and catalyst recyclability, surpassing previous literature performances.
View Article and Find Full Text PDFAtom-precise nanoclusters-metal-organic framework (APNC/MOF) composites, as bifunctional material with well-defined structures, have attracted considerable attention in recent years. Despite the progress made to date, there is an urgent need to develop a generic and scalable approach for all APNCs. Herein, the authors present the Exploiting Fracture Strategy (EFS) and successfully construct a super-stable bifunctional APNC/ZIF-8(300 °C) composite overcoming the limitations of previous strategies in selecting APNCs.
View Article and Find Full Text PDFAlthough the chemistry of carbonyl-protected platinum nanoclusters is well established, their bonding mode remains poorly understood. In most of them, the average Pt oxidation state is zero or slightly negative, leading to the apparent average configuration 5d 6s ( = 0 or very small) and the apparent conclusion that metal-metal bonding cannot arise from the completely filled 5d shell nor from the empty (or almost empty) 6s orbitals. However, DFT calculations show in fact that in these species the actual average configuration is 5d 6s, which provides to the whole cluster a significant total number of 6s electrons that ensures metal-metal bonding.
View Article and Find Full Text PDFIn an effort to turn waste into wealth, Reactive Red 2 (RR2), a common and refractory organic pollutant in industrial wastewater, has been employed for the first time as a precursor to synthesize carbon nanodots (CNDs) by a facile, green and low-cost route, without utilization of any strong acids or other oxidizers. The detailed characterizations have confirmed that the synthesized CNDs exhibit good water dispersibility, with a mean particle size of 2.43 nm and thickness of 1-3 layers.
View Article and Find Full Text PDFMany studies have evaluated the Neonatal Individualized Developmental Care and Assessment Program (NIDCAP), but few studies have assessed changes in infant- and family-centered developmental care (IFCDC) practices during its implementation. The primary objective of this single center study was to investigate the impact of the implementation of the NIDCAP program on IFCDC practices used for management of extremely preterm infants (EPIs). The secondary objective was to determine during implementation the impact of this program on the short-term medical outcomes of all EPIs hospitalized at our center.
View Article and Find Full Text PDFAim: Very preterm infants are exposed to an atypical environment that could alter their developmental trajectory. We aimed to examine neonatal imitation, a foundation of social cognition, in very preterm and full-term infants.
Methods: In Strasbourg, France, between 2015 and 2018, we prospectively investigated the development of imitation skills.
Chemistry
November 2021
Electron transfer plays a major role in chemical reactions and processes, and this is particularly true of catalysis by nanomaterials. The advent of metal nanoparticle (NP) catalysts, recently including atomically precise nanoclusters (NCs) as parts of nanocatalyst devices has brought increased control of the relationship between NP and NC structures and their catalytic functions. Consequently, the molecular definition of these new nanocatalysts has allowed a better understanding and management of various kinds of electron transfer involved in the catalytic processes.
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