The current study presents a quick and simple method for synthesizing Ir nanoclusters decorated on an N-doped carbon (NC) matrix via pulsed laser ablation in liquid, followed by pyrolysis. The resulting Ir-NC material acts as a dual-functional electrocatalyst, efficiently facilitating hydrogen generation through the hydrazine oxidation reaction (HzOR) and the hydrogen evolution reaction (HER) in alkaline seawater. The optimized Ir-NC-2 catalyst exhibits a low operating potential of 23 mV versus the reversible hydrogen electrode for HzOR and a remarkably low overpotential of 24 mV for HER, achieving a current density of 10 mA cm in alkaline seawater, surpassing the performance of the Pt/C catalyst.
View Article and Find Full Text PDFHerein, a straightforward approach using pulsed laser technology to synthesize selective hexagonal-close-packed (hcp) Ru nanoparticles attached to Cu nanospheres (Ru/Cu) as bifunctional electrocatalyst for catalyzing the hydrogen evolution reaction (HER) and formaldehyde oxidation reaction (FOR) are reported. Initially, Ru-doped CuO flakes are synthesized using a coprecipitation method followed by transformation into Ru/Cu composites through a strategy involving pulsed laser irradiation in liquid. Specifically, the optimized Ru/Cu-4 composite not only demonstrates a low overpotential of 182 mV at 10 mA·cm for the HER but also an ultralow working potential of 0.
View Article and Find Full Text PDFThis study addresses the urgent need to focus on the nitrite reduction reaction (NORR) to ammonia (NH). A ternary-metal Prussian blue analogue (CoCuFe-PBA) was utilized as the template material, leveraging its tunable electronic properties to synthesize CoCuFe oxide (CoCuFe-O) through controlled calcination. Subsequently, a CoCuFe alloy (CoCuFe-A) was obtained via pulsed laser irradiation in liquids.
View Article and Find Full Text PDFEfficient and durable electrocatalysts for the hydrogen evolution reaction (HER) in alkaline seawater environments are essential for sustainable hydrogen production. Zeolitic imidazolate framework-8 (ZIF-8) is synthesized through pulsed laser ablation in liquid, followed by pyrolysis, producing N-doped porous carbon (NC). NC matrix serves as a self-template, enabling Pt nanocluster decoration (NC-Pt) via pulsed laser irradiation in liquid.
View Article and Find Full Text PDFDeveloping sustainable energy solutions is critical for addressing the dual challenges of energy demand and environmental impact. In this study, a zinc-nitrate (Zn-NO ) battery system was designed for the simultaneous production of ammonia (NH) via the electrocatalytic NO reduction reaction (NORR) and electricity generation. Continuous wave CO laser irradiation yielded precisely controlled CoFeO@nitrogen-doped carbon (CoFeO@NC) hollow nanocubes from CoFe Prussian blue analogs (CoFe-PBA) as the integral electrocatalyst for NORR in 1.
View Article and Find Full Text PDFSuperfluid helium nanodroplets are unique nanomatrices for the isolation and study of transient molecular species, such as radicals, carbenes, and ions. In this work, isomers of C3H4+ were produced upon electron ionization of propyne and allene molecules and interrogated via infrared spectroscopy inside He nanodroplet matrices. It was found that the spectrum of C3H4+ has at least three distinct groups of bands.
View Article and Find Full Text PDFThe present study details the strategic development of Co-doped CuO nanostructures via sophisticated and expedited pulsed laser ablation in liquids (PLAL) technique. Subsequently, these structures are employed as potent electrocatalysts for the anodic methanol oxidation reaction (MOR), offering an alternative to the sluggish oxygen evolution reaction (OER). Electrochemical assessments indicate that the Co-CuO catalyst exhibits exceptional MOR activity, requiring a reduced potential of 1.
View Article and Find Full Text PDFElectrochemical water splitting, driven by processed catalysts, is the most reasonable method for hydrogen production. This study demonstrates an activation phenomenon with ruthenium (Ru) nanoclusters on few-layered black phosphorus (BP), greatly enhancing the electrocatalytic hydrogen evolution reaction (HER). Efficient BP exfoliation was achieved using acoustic levitators and pulsed laser irradiation in liquids (PLIL), yielding charge-transfer Ru-nanoclusters on modulated surfaces.
View Article and Find Full Text PDFIn this work, we explored the in-situ reaction modeling of the molecular self-aggregation of methylene blue (MB), which is a cationic thiazine dye, in different solvents via a container-less acoustic levitator by floating of a single droplet. Our in-situ spectroscopic study revealed that the dimer essentially has a sandwich structural geometry with a deviation from parallel stacking and horizontal arrangements in the molecular planes. The real time conversion of the monomer in MB into a dimer and their dynamics in water and ethanol media were monitored using a free-standing acoustic levitator droplet system.
View Article and Find Full Text PDFInfrared (IR) spectroscopy using ultracold helium nanodroplet matrices has proven to be a powerful method to interrogate encapsulated ions, molecules, and clusters. Due to the helium droplets' high ionization potential, optical transparency, and ability to pick up dopant molecules, the droplets offer a unique modality to probe transient chemical species produced via photo- or electron impact ionization. In this work, helium droplets were doped with acetylene molecules and ionized via electron impact.
View Article and Find Full Text PDFHelium droplets are unique hosts for isolating diverse molecular ions for infrared spectroscopic experiments. Recently, it was found that electron impact ionization of ethylene clusters embedded in helium droplets produces diverse carbocations containing three and four carbon atoms, indicating effective ion-molecule reactions. In this work, similar experiments are reported but with the saturated hydrocarbon precursor of ethane.
View Article and Find Full Text PDFActa Crystallogr E Crystallogr Commun
February 2021
The title compound, [Pt(CHFNO)Cl], crystallizes with two crystallographically independent mol-ecules ( and ) in the asymmetric unit, which adopt similar conformations. The Pt atoms in both mol-ecules adopt distorted square-planar geometries, coordinated by one C and two N atoms from the tridentate 2',6'-di-fluoro-6-[3-(pyridin-2-yl-oxy)phen-yl]-2,3'-bi-pyridine ligand and a chloride anion: the C and Cl atoms are . In the crystal, C-H⋯Cl/F hydrogen bonds, F⋯π and weak π-π stacking inter-actions between adjacent and mol-ecules and between pairs of inversion-related B mol-ecules lead to the formation of a two-dimensional supra-molecular network lying parallel to the plane.
View Article and Find Full Text PDFThe induced circular dichroism (ICD) of phenol complexed with ()-(-)-2-butanol [PhOH-(-)BOH] in a supersonic jet is investigated using resonant two-photon ionization circular dichroism (R2PICD) spectroscopy. The R2PICD spectrum of PhOH-(-)BOH exhibits nonzero ICD bands near the absorption region of bare PhOH, where (-)BOH is transparent. Two different conformers containing a single hydrogen bond between PhOH and (-)BOH are identified using ultraviolet-ultraviolet hole-burning and infrared ion-dip spectroscopy combined with quantum theoretical calculations.
View Article and Find Full Text PDFActa Crystallogr E Crystallogr Commun
June 2019
The title compound, CHNOS, was synthesized by the reaction of 1,4,5,8-naphthalene-tetra-carb-oxy-lic dianhydride with 3-(methyl-sulfan-yl)propyl-amine. The whole mol-ecule is generated by an inversion operation of the asymmetric unit. This mol-ecule has an form with the terminal methyl-thio-propyl groups above and below the aromatic di-imide plane, where four intra-molecular C-H⋯O and C-H⋯S hydrogen bonds are present and the O⋯H⋯S angle is 100.
View Article and Find Full Text PDFWe demonstrated the morphology transformation of co-assemblies based on terpyridine-based ligands (1R and 1S) possessing R- or S-alanine analogues and their platinum(II) complex (2R-Pt and 2S-Pt). The right-handed helical ribbon of the co-assembly formed with 0.5 equivalents of 2R-Pt to 1R was converted into the left-handed helical ribbon with 0.
View Article and Find Full Text PDFInduced circular dichroism (ICD) is the CD observed in the absorption of an achiral molecule bound to a transparent chiral molecule through noncovalent interactions. ICD spectroscopy has been used to probe the binding between molecules, such as protein-ligand interactions. However, most ICD spectra have been measured in solution, which only exhibit the averaged CD values of all conformational isomers in solution.
View Article and Find Full Text PDFWe demonstrate the different origins of helical directions in polymeric gels derived from a hydrazone reaction in the absence and presence of Ni. The right-handed helicity of polymeric gels without Ni originates from the enantiomeric d-form alanine moiety embedded in the building block. However, the right-handed helicity is inverted to a left-handed helicity upon the addition of Ni, indicating that added Ni greatly affects the conformation of the polymeric gel by overcoming the influence of the enantiomer embedded in the building block on the helicity at the supramolecular level.
View Article and Find Full Text PDFActa Crystallogr E Crystallogr Commun
September 2017
The title compound, CHNOS {systematic name: 6-[2-(cyclo-hexyl-sulfan-yl)eth-yl]-5-pyrrolo-[3,4-]pyridine-5,7(6)-dione}, was obtained from the reaction of pyridine-2,3-di-carb-oxy-lic anhydride (synonym: quinolinic anhydride) with 2-(cyclo-hexyl-sulfan-yl)ethyl-amine. The dihedral angle between the mean plane of the cyclo-hexyl ring and the quinolinic acid imide ring is 25.43 (11)°.
View Article and Find Full Text PDFActa Crystallogr E Crystallogr Commun
June 2017
The title compound, CHNO [systematic name: 2,6-di-decyl-pyrrolo-[3,4-]iso-indole-1,3,5,7(2,6)-tetra-one], consists of a central pyromellitic di-imide moiety with terminal decyl groups at the N-atom positions. The centre of the mol-ecule lies on a crystallographic inversion centre so the asymmetric unit contains one half-mol-ecule. The mol-ecule exhibits a rod-shaped conformation, like other similar compounds of this type, the distance between the ends of terminal decyl groups being 32.
View Article and Find Full Text PDFJet-cooled acetaminophen (AAP)-water clusters, AAP-(HO), were investigated by mass-selected resonant two-photon ionization (R2PI), ultraviolet-ultraviolet hole-burning (UV-UV HB), infrared-dip (IR-dip), and infrared-ultraviolet hole-burning (IR-UV HB) spectroscopy. Each syn- and anti-AAP rotamer has three distinctive binding sites (-OH, >CO, and >NH) for a water molecule, thus 6 different AAP-(HO) conformers are expected to exist in the molecular beam. The origin bands of the AAP(OH)-(HO) and AAP(CO)-(HO) conformers (including their syn- and anti-conformers) in the R2PI spectrum are shifted to red and blue compared to those of the AAP monomer, respectively.
View Article and Find Full Text PDFTo more accurately assess the pathways of biological systems, a probe is needed that may respond selectively to adenosine triphosphate (ATP) for both in vitro and in vivo detection modes. We have developed a luminescence probe that can provide real-time information on the extent of ATP, ADP, and AMP by virtue of the luminescence and luminescence lifetime observed from a supramolecular polymer based on a C symmetrical terpyridine complex with Tb (S1-Tb). The probe shows remarkable selective luminescence enhancement in the presence of ATP compared to other phosphate-displaying nucleotides including adenosine diphosphate (ADP), adenosine monophosphate (AMP), guanosine triphosphate (GTP), thymidine triphosphate (TTP), HPO (Pi), and pyrophosphate (PPi).
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