Photochemical
behaviors of pyruvic acid in multiple phases
have
been extensively studied, while those of its conjugate base, the pyruvate
anion (CH3COCOO–, PA–) are less understood and remain contradictory in gaseous versus
aqueous phases. Here in this article, we report a joint experimental
and theoretical study combining cryogenic, wavelength-resolved negative
ion photoelectron spectroscopy (NIPES) and high-level quantum chemical
computations to investigate PA– actinic photochemistry
and its dependence on microsolvation in the gas phase. PA–·nH2O (n = 0–5)
clusters were generated and characterized, with their low-lying isomers
identified. NIPES conducted at multiple wavelengths across the PA– actinic regime revealed the PA– photochemistry
extremely sensitive to its hydration extent. While bare PA– anions exhibit active photoinduced dissociations that generate the
acetyl (CH3CO–), methide (CH3
–) anions, their corresponding radicals, and slow
electrons, one single attached water molecule results in significant
suppression with a subsequent second water being able to completely
block all dissociation pathways, effectively annihilating all PA– photochemical reactivities. The underlying dissociation
mechanisms of PA–·nH2O (n = 0–2) clusters are proposed involving nπ* excitation, dehydration, decarboxylation, and
further CO loss. Since the photoexcited dihydrate does not have sufficient
energy to overcome the full dehydration barrier before PA– could fragmentate, the PA– dissociation pathway
is completely blocked, with the energy most likely released via loss
of one water and internal electronic and vibrational relaxations.
The insight unraveled in this work provides a much-needed critical
link to connect the seemingly conflicting PA– actinic
chemistry between the gas and condensed phases.
In the current study, Cu 2 ZnSnS 4 (CZTS) thin film was successfully fabricated by the facile nanocrystals (NCs)-printing approach combined with rapid thermal annealing (RTA) process. Firstly, the CZTS NCs were synthesized by a thermal solution method and the possible formation mechanism was analyzed briefly. Then the influences of RTA toleration temperature and duration time on the various properties of as-printed thin films were examined via XRD, Raman, FE-SEM, UV-vis-IR spectroscopy, EDS and XPS treatments in detail. As observed, the RTA factors of temperature and time had significant impacts on the structure and morphology of as-prepared thin films, while there were no obvious effects on the band gap energy in studied conditions. The results showed that the obtained thin film at optimal RTA conditions of (600 • C, 20 min) featured a kesterite structure in pure phase and an irregular morphology consisting of large grains. Moreover, the satisfactory composition of a Cu-poor, Zn-rich state and an ideal band gap energy of 1.4 eV suggests that as-fabricated CZTS thin film is a suitable light-absorbing layer candidate for the application in thin film solar cells.
Staphylococcus aureus (S. aureus) is one of the most common pathogens for nosocomial and community infections, which is closely related to the occurrence of pyogenic and toxic diseases in human beings. In the current study, a lab-built microchip capillary electrophoresis (microchip CE) system was employed for the rapid determination of S. aureus, while a simple-to-use space domain internal standard (SDIS) method was carried out for the reliable quantitative analysis. The precision, accuracy, and reliability of SDIS were investigated in detail. Noted that these properties could be elevated in SDIS compared with traditional IS method. Remarkably, the PCR products of S. aureusnuc gene could be identified and quantitated within 80 s. The theoretical detection limit could achieve a value of 0.066 ng/μL, determined by the using SDIS method. The current work may provide a promising detection strategy for the high-speed and highly efficient analysis of pathogens in the fields of food safety and clinical diagnosis.
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