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1.
Angew Chem Int Ed Engl ; 62(28): e202303557, 2023 Jul 10.
Article in English | MEDLINE | ID: mdl-37191972

ABSTRACT

In aqueous zinc (Zn) batteries, the Zn anode suffers from severe corrosion reactions and consequent dendrite growth troubles that cause fast performance decay. Herein, we uncover the corrosion mechanism and confirm that the dissolved oxygen (DO) other than the reputed proton is a principal origin of Zn corrosion and by-product precipitates, especially during the initial battery resting period. In a break from common physical deoxygenation methods, we propose a chemical self-deoxygenation strategy to tackle the DO-induced hazards. As a proof of concept, sodium anthraquinone-2-sulfonate (AQS) is introduced to aqueous electrolytes as a self-deoxidizing additive. As a result, the Zn anode sustains a long-term cycling of 2500 h at 0.5 mA cm-2 and over 1100 h at 5 mA cm-2 together with a high Coulombic efficiency up to 99.6 %. The full cells also show a high capacity retention of 92 % after 500 cycles. Our findings provide a renewed understanding of Zn corrosion in aqueous electrolytes and also a practical solution towards industrializing aqueous Zn batteries.

2.
ACS Nano ; 17(1): 668-677, 2023 Jan 10.
Article in English | MEDLINE | ID: mdl-36534047

ABSTRACT

The aqueous zinc (Zn) battery is a safe and eco-friendly energy-storage system. However, the use of Zn metal anodes is impeded by uncontrolled Zn deposition behavior. Herein, we regulate the Zn-ion deposition process for dendrite-free Zn metal anodes using an aminosilane molecular layer with high zincophilic sites and narrow molecule channels. The aminosilane molecular layer causes Zn ions to undergo consecutive processes including being captured by the amine functional groups of aminosilane and diffusing through narrow intermolecular channels before electroplating, which induces partial dehydration of hydrated Zn ions and uniform Zn ion flux, promoting reversible Zn stripping/plating. Through this molecule-induced capture-diffusion-deposition procedure of Zn ions, smooth and compact Zn electrodeposited layers are obtained. Hence, the aminosilane-modified Zn anode has high Coulombic efficiency (∼99.5%), long lifespan (∼3000 h), and high capacity retention in full cells (88.4% for 600 cycles). This strategy not only has great potential for achieving dendrite-free Zn anodes in practical Zn batteries but also suggests an interface-modification principle at the molecular level for other alternative metallic anodes.

3.
Small ; 16(29): e2001736, 2020 Jul.
Article in English | MEDLINE | ID: mdl-32567230

ABSTRACT

Rechargeable aqueous zinc (Zn) ion-based energy storage systems have been reviving recently because of their low cost and high safety merits; however, they still suffer from the problems of corrosion and dendrite growth on Zn metal anodes that cause gas generation and early battery failure. Unfortunately, the corrosion problem has not received sufficient attention until now. Here, it is pioneeringly demonstrated that decorating the Zn surface with a dual-functional metallic indium (In) layer, acting as both a corrosion inhibitor and a nucleating agent, is a facile but effective strategy to suppress both drastic corrosion and dendrite growth. Symmetric cells assembled with the treated Zn electrodes can sustain up to 1500 h of plating/stripping cycles with an ultralow voltage hysteresis (54 mV), and a 5000 cycle-life is achieved for a prototype full cell. This work will instigate the further development of aqueous metal-based energy storage systems.

4.
Eur J Med Chem ; 94: 298-305, 2015 Apr 13.
Article in English | MEDLINE | ID: mdl-25771108

ABSTRACT

Acetohydroxyacid synthase (AHAS) catalyzes the first essential biosynthetic step of branched-chain amino acids and is a biologically safe target against Mycobacterium tuberculosis (MTB). In our previous research, we used virtual screening to identify some novel AHAS inhibitors as potent antituberculosis agents. In this study, we synthesized twenty-four additional quinazolinone benzoates and explored their antitubercular activity. Five of these compounds displayed significant MTB-AHAS inhibition and their IC50 values were determined to be in the range of 6.50 µM-12.08 µM. Importantly, these compounds also exhibited strong in vitro activity (MICs in the range of 2.5-10 mg/L) and intracellular activity against clinically isolated extensively drug-resistant strains of M. tuberculosis. Taken together, these results indicated that the quinazolinone benzoate compounds should be regarded as promising lead compounds for the development of potent antituberculosis drugs with a novel mode of action.


Subject(s)
Acetolactate Synthase/antagonists & inhibitors , Antitubercular Agents/pharmacology , Benzoates/pharmacology , Enzyme Inhibitors/pharmacology , Mycobacterium tuberculosis/drug effects , Quinazolinones/pharmacology , Acetolactate Synthase/metabolism , Antitubercular Agents/chemical synthesis , Antitubercular Agents/chemistry , Benzoates/chemical synthesis , Benzoates/chemistry , Crystallography, X-Ray , Dose-Response Relationship, Drug , Enzyme Inhibitors/chemical synthesis , Enzyme Inhibitors/chemistry , Microbial Sensitivity Tests , Models, Molecular , Molecular Structure , Quinazolinones/chemical synthesis , Quinazolinones/chemistry , Structure-Activity Relationship
5.
J Chem Inf Model ; 53(2): 343-53, 2013 Feb 25.
Article in English | MEDLINE | ID: mdl-23316686

ABSTRACT

Acetohydroxyacid synthase (AHAS) has been regarded as a promising drug target against Mycobacterium tuberculosis (MTB) as it catalyzes the biosynthesis of branched-chain amino acids. In this study, 23 novel AHAS inhibitors were identified through molecular docking followed by similarity search. The determined IC(50) values range from 0.385 ± 0.026 µM to >200 µM against bacterium AHAS. Five of the identified compounds show significant in vitro activity against H37Rv strains (MICs in the range of 2.5-80 mg/L) and clinical MTB strains, including MDR and XDR isolates. More impressively, compounds 5 and 7 can enhance the killing ability against macrophages infected pathogen remarkably. This study suggests our discovered inhibitors can be further developed as novel anti-MTB therapeutics targeting AHAS.


Subject(s)
Acetolactate Synthase/antagonists & inhibitors , Antitubercular Agents/chemistry , Antitubercular Agents/pharmacology , Mycobacterium tuberculosis/drug effects , Mycobacterium tuberculosis/enzymology , Tuberculosis/drug therapy , Acetolactate Synthase/metabolism , Cell Line , Humans , Macrophages/microbiology , Microbial Sensitivity Tests , Molecular Docking Simulation , Tuberculosis/microbiology
6.
J Med Chem ; 56(1): 210-9, 2013 Jan 10.
Article in English | MEDLINE | ID: mdl-23237384

ABSTRACT

The sulfonylurea herbicides exert their activity by inhibiting plant acetohydroxyacid synthase (AHAS), the first enzyme in the branched-chain amino acid biosynthesis pathway. It has previously been shown that if the gene for AHAS is deleted in Candida albicans , attenuation of virulence is achieved, suggesting AHAS as an antifungal drug target. Herein, we have cloned, expressed, and purified C. albicans AHAS and shown that several sulfonylureas are inhibitors of this enzyme and possess antifungal activity. The most potent of these compounds is ethyl 2-(N-((4-iodo-6-methoxypyrimidin-2-yl)carbamoyl)sulfamoyl)benzoate (10c), which has a K(i) value of 3.8 nM for C. albicans AHAS and an MIC90 of 0.7 µg/mL for this fungus in cell-based assays. For the sulfonylureas tested there was a strong correlation between inhibitory activity toward C. albicans AHAS and fungicidal activity, supporting the hypothesis that AHAS is the target for their inhibitory activity within the cell.


Subject(s)
Acetolactate Synthase/antagonists & inhibitors , Antifungal Agents/chemical synthesis , Benzoates/chemical synthesis , Candida albicans/drug effects , Sulfonylurea Compounds/chemical synthesis , Acetolactate Synthase/chemistry , Amino Acid Sequence , Antifungal Agents/chemistry , Antifungal Agents/pharmacology , Benzoates/chemistry , Benzoates/pharmacology , Candida albicans/enzymology , Catalytic Domain , Disk Diffusion Antimicrobial Tests , Herbicides/pharmacology , Microbial Sensitivity Tests , Models, Molecular , Molecular Sequence Data , Recombinant Proteins/antagonists & inhibitors , Recombinant Proteins/chemistry , Structure-Activity Relationship , Sulfonylurea Compounds/chemistry , Sulfonylurea Compounds/pharmacology
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