RESUMO
A clustered countercurrent-flow micro-channel reactor (C-CFMCR) with adjustable magnification times was constructed for the preparation of KMnF3 perovskite fluoride by a co-precipitation process, in which the concentrations and feed rates of reactants were precisely controlled. Benefitting from the enhanced micromixing efficiency of the microreactor, the KMnF3 particles prepared in C-CFMCR were smaller and less aggregated than those produced with traditional stirred reactors (STR). The prepared KMnF3 was applied as the electrode material in supercapacitors, and the electrochemical measurements showed that the KMnF3 obtained under optimal conditions had a discharge specific capacitance of â¼442 F g-1 at a current density of 1 A g-1, with a decline of â¼5.4% after 5000 charge-discharge cycles in an aqueous electrolyte of 2 M KOH. It was also found that the morphologies and electrochemical performances of the prepared KMnF3 particles changed accordingly with the micromixing efficiencies of C-CFMCR, which can be adjusted by the reactor structure and operating conditions. An asymmetric supercapacitor assembled with the KMnF3 and activated carbon exhibited an energy density of 13.1 W h kg-1 at a power density of 386.3 W kg-1, with eminent capacitance retention of â¼81.2% after 5000 cycles. In addition, only a slight amplification effect of C-CFMCR on the co-precipitation process was noticed, indicating that the C-CFMCR is a promising technology for the massive and controllable production of KMnF3 particles as well as other ultrafine particles.
RESUMO
A clustered countercurrent-flow micro-channel reactor (C-CFMCR) has been assembled by the numbering-up of its single counterpart (S-CFMCR). Its micromixing performance was then studied experimentally using a competitive parallel reaction system, and the micromixing time was calculated as the micromixing performance index. It was found that the micromixing time of C-CFMCR was ranged from 0.34 to 10 ms according to its numbering-up times and the operating conditions of the reactor, and it was close to that of S-CFMCR under the same operating conditions, demonstrating a weak scaling-up effect from S-CFMCR to C-CFMCR. The C-CFMCR was then applied to prepare ultrafine manganese dioxide in a continuous manner at varying micromixing time. It showed that the micromixing time had a major effect on the particle structure. More uniform and smaller MnO2 particles were obtained with intensified micromixing. By building a typical three electrode system to characterize their performance as a supercapacitor material, the MnO2 particles prepared by both S-CFMCR and C-CFMCR under optimal conditions displayed a specific capacitance of ~175 F·g-1 at the current density of 1 A·g-1, with a decline of ~10% after 500 charge-discharge cycles. This work showed that C-CFMCR will have a great potential for the continuous and large-scale preparation of ultrafine particles.
RESUMO
Sansanmycins (SS), one of several known uridyl peptide antibiotics (UPAs) possessing a unique chemical scaffold, showed a good inhibitory effect on the highly refractory pathogens Pseudomonas aeruginosa and Mycobacterium tuberculosis, especially on the multi-drug resistant M. tuberculosis. This study employed high performance liquid chromatography-mass spectrometry detector (HPLC-MSD) ion trap and LTQ orbitrap tandem mass spectrometry (MS/MS) to explore sansanmycin analogues manually and automatically by re-analysis of the Streptomyces sp. SS fermentation broth. The structure-based manual screening method, based on analysis of the fragmentation pathway of known UPAs and on comparisons of the MS/MS spectra with that of sansanmycin A (SS-A), resulted in identifying twenty sansanmycin analogues, including twelve new structures (1-12). Furthermore, to deeply explore sansanmycin analogues, we utilized a GNPS based molecular networking workflow to re-analyze the HPLC-MS/MS data automatically. As a result, eight more new sansanmycins (13-20) were discovered. Compound 1 was discovered to lose two amino acids of residue 1 (AA1) and (2S, 3S)-N3-methyl-2,3-diamino butyric acid (DABA) from the N-terminus, and compounds 6, 11 and 12 were found to contain a 2',3'-dehydrated 4',5'-enamine-3'-deoxyuridyl moiety, which have not been reported before. Interestingly, three trace components with novel 5,6-dihydro-5'-aminouridyl group (16-18) were detected for the first time in the sansanmycin-producing strain. Their structures were primarily determined by detail analysis of the data from MS/MS. Compounds 8 and 10 were further confirmed by nuclear magnetic resonance (NMR) data, which proved the efficiency and accuracy of the method of HPLC-MS/MS for exploration of novel UPAs. Comparing to manual screening, the networking method can provide systematic visualization results. Manual screening and networking method may complement with each other to facilitate the mining of novel UPAs.