Mechanism of antimalarial action and mitigation of infection-mediated mitochondrial dysfunction by phyto-constituents of Andrographis paniculata ((Burm f.) Wall. ex Nees) in Plasmodium berghei-infected mice.

ETHNOPHARMACOLOGICAL RELEVANCE: Andrographis paniculata (AP) ((Burm f.) Wall. ex Nees) is a medicinal plant, documented for its folkloric use in the treatment of malaria. AIM: This study was designed to determine the potency of extract and fractions of A. paniculata (AP) as a curative, both for susceptible and resistant malaria and to also determine the plant's mechanism of action. This study was also designed to determine whether AP extract and its most potent fraction will mitigate infection-mediated mitochondrial dysfunction, and to assess the phytochemical constituents of the most potent fraction. MATERIALS AND METHODS: n-Hexane, dichloromethane, ethylacetate and methanol were used to partition the methanol extract of A. paniculata. Graded doses of these extract and fractions were used to treat mice infected with chloroquine-sensitive strain of P. berghei in a curative model. The most potent fraction was used to treat mice infected with resistant (ANKA strain) P. berghei. Inhibition of hemozoin formation, reversal of mitochondrial dysfunction and antiinflammatory potentials were determined. A combination of ultraperformance liquid chromatography-quadrupole time of flight-mass spectrometry and nuclear magnetic resonance spectroscopy were used for chemical analysis. RESULTS: Microscopy revealed that the dichloromethane fraction decreased the parasite burden the most, and inhibition of the hemozoin formation is one of its mechanisms of action. The dichloromethane fraction reversed parasite-induced mitochondrial pore opening in the host, enzyme-dependent ATP hydrolysis and peroxidation of host mitochondrial membrane phospholipids as well as its antiinflammatory potentials. The UPLC-qTOF-MS report and NMR fingerprints of the dichloromethane fraction of A. paniculata yielded fourteen compounds of which sibiricinone C was identified from the plant for the first time. CONCLUSION: Fractions of A. paniculata possess antiplasmodial effects with the dichloromethane fraction having the highest potency. The potent effect of this fraction may be attributed to the phytochemicals present because it contains terpenes implicated with antimalarial and antiinflammatory activities.

Metabolomics and in-vitro bioactivities studies of fermented Musa paradisiaca pulp: A potential alpha-amylase inhibitor.

The in-vitro synthesis of bio-compounds via fermentation is a promising route for bioactive molecules intended for disease control and management. Therefore, this study evaluated the effect of fermentation on the antioxidants, antihyperglycemic and anti-inflammatory properties and the resultant chemometric phytochemical profiles of unripe plantain fruits. The results revealed that Escherichia coli and Propionibacterium spp. are suspected as the key fermenters. The E coli showed negative results to the pathogenicity test; Propionibacterium appeared to be opportunistic. A significant increase in the total polyphenols and protein and decreased flavonoids was recorded in the phytochemical profile of the methanolic extract of the fermented unripe plantain pulp; however, the ascorbic acid content was not significantly altered. The 1H NMR fingerprint showed that there is a closely related chemical shift among the shorter fermentation time (days 2-6) and the unfermented, while the more extended fermentation periods (days 7-12) with enhanced bioactivities were closely related based on the chemometrics analyses. Furthermore, the UPLC-QTOF-MS analysis annotated the presence of bioactive compounds in the day-9 fermented sample: polyhydroxy glucose conjugates (3-Methoxy-4-hydroxyphenyl 6-O-(3,4,5-trihydroxybenzoyl)-beta-D-glucopyranoside), short chain peptide (leucyl-glycyl-glycine), amino acid derivatives (4-Aminophenylalanine, and N-Acetylhistidine), linear and cyclic fatty acid derivatives (palmitoyl putrescine, ricinoleic acid, phytosphingosine, gabalid, rubrenoic acid, 2-aminocyclopentanecarboxylic and cystodienioc acid). The synergistic effect of these newly formed compounds and the increase in the phenolic content of the day-9 fermented unripe plantain may account for its more potent antioxidant, anti-inflammatory and antihyperglycemic activity. Therefore, the products obtained from the day 9 fermentation of unripe plantain pulp may serve as potential nutraceutical agents against gastro-enteric sugar digestion and absorption and sugar-induced oxidative stress, inflammation and metabolic disease.

In vitro effects of 2-methyl-3-propylbutane-1,4-diol purified from Alstonia boonei on erythrocyte membrane stabilization and mitochondrial membrane permeabilization.

A recent review on the ethnomedicinal, chemical, pharmacological, and toxicological properties of Alstonia boonei revealed the plant's potential in the treatment and management of a range of diseases. However, most of these pharmacological effects are only traceable to the crude form of the plant extract and not specific natural products. Phytochemical investigation of the methanol fraction of the methanol extract of the stem-bark of Alstonia boonei led to the isolation and identification of 2-methyl-3-propylbutane-1,4-diol. The structures were elucidated by the application of 1D-, and 2D-NMR spectroscopic analyses and by comparison with literature data. In this study, the membrane stabilizing activity, mitochondrial membrane permeability transition pore opening, cytochrome c release, mitochondrial ATPase activity, and prevention of mitochondrial lipid peroxidation activity of 2-methyl-3-propylbutane-1,4-diol (MPBD) isolated from A. boonei were determined. The results showed that MPBD significantly (p < .05) prevented peroxidation of mitochondrial membrane lipids and hemolysis using both the heat-induced and hypotonic solution-induced membrane stabilization assays. On the contrary, the compound caused large amplitude swelling of rat liver mitochondria in the absence of calcium, significant (p < .05) cytochrome c release and enhancement of mitochondrial ATPase activity in vitro. Our findings suggest that MPBD showed characteristic biological properties useful in modulating cell death.

Effect of Different Climatic Regions and Seasonal Variation on the Antibacterial and Antifungal Activity, and Chemical Profile of Helichrysum aureonitens Sch. Bip.

Native South Africans make use of Helichrysum aureonitens Sch. Bip. extracts for the treatment of a variety of infections and they are important in traditional medicinal preparations. This study investigated the effect of seasonal variation and geographical location on the antibacterial and antifungal activities of H. aureonitens. Material was collected in two different seasons: early spring, with high rainfall and high temperatures (October), and late autumn, with low rainfall and lower temperatures (May). Further analysis was carried out using 1H-NMR based metabolomics to analyse and compare the chemical profiles of the plants in both seasons and locations. Plant materials were collected from two sites for each season, at Wakefield farm (KwaZulu-Natal), representing a colder, wetter environment, and Telperion (Mpumalanga), representing a drier and warmer environment. Leaves of H. aureonitens were tested against bacteria (Proteus vulgaris (P. vulgaris) and Bacillus subtilis (B. subtilis)) as well as fungi (Aspergillus flavus (A. flavus), Aspergillus nomius (A. nomius), Cladosporium cladosporioides (C. cladosporioides), Fusarium oxysporum (F. oxysporum) and Penicillum halotolerans (P. halotolerans)). Extracts from the October harvest showed significant activities against the Gram-negative bacterium P. vulgaris compared to the May harvest, with an MIC value of 62.5 µg/mL. Similar activity was observed between the extracts from the wet season across the two geographically different locations. There was generally very good antifungal activity observed for all the species, with the exception of A. nomius, which had MIC values ranging from 0.39-1.56 µg/mL. Extracts of plant materials harvested in the wetter region had a significantly higher activity against A. flavus and F. oxysporum in both seasons than those from plants harvested in the drier region. Telperion-harvested plants exhibited better activity against F. oxysporum in the autumn. Hydrogen-1 NMR metabolomic analysis confirmed the significant effects of the seasons and the peculiar climates of different localities on the secondary metabolite profile of H. aureonitens.

New Alk(en)ylhydroxycyclohexanes with Tyrosinase Inhibition Potential from Harpephyllum caffrum Bernh. Gum Exudate.

This work presents the first report on the phytochemical investigation of Harpephyllum caffrum Bernh. gum exudate. A known cardanol, 3-heptadec-12'-Z-enyl phenol (1) and three new alk(en)ylhydroxycyclohexanes, namely, (1R,3R)-1,3-dihydroxy-3-[heptadec-12'(Z)-enyl]cyclohexane (2) (1S,2S,3S,4S,5R)-1,2,3,4,5-pentahydroxy-5-[octadec-13'(Z)-enyl]cyclohexane (3) and (1R,2S,4R)-1,2,4-trihydroxy-4-[heptadec-12'(Z)-enyl]cyclohexane (4) were isolated from the gum. The structures of the compounds were determined by extensive 1D and 2D NMR spectroscopy and HR-ESI-MS data. The ethanolic extract of the gum was found to be the most potent tyrosinase inhibitor with IC50 of 11.32 µg/mL while compounds 2 and 3, with IC50 values of 24.90 and 26.99 µg/mL, respectively, were found to be potential anti-tyrosinase candidates from the gum. Gum exudate may be a potential source for non-destructive harvesting of selective pharmacologically active compounds from plants. The results also provide evidence that H. caffrum gum may find application in cosmetics as a potential anti-tyrosinase agent.

1H-NMR and LC-MS Based Metabolomics Analysis of Potato (Solanum tuberosum L.) Cultivars Irrigated with Fly Ash Treated Acid Mine Drainage.

1H NMR and LC-MS, commonly used metabolomics analytical platforms, were used to annotate the metabolites found in potato (Solanum tuberosum L.) irrigated with four different treatments based on FA to AMD ratios, namely: control (0% AMD; tap water), 1:1 (50% AMD), 3:1 (75% AMD is 75% FA: AMD), and 100% AMD (untreated). The effects of stress on plants were illustrated by the primary metabolite shifts in the region from δH 0.0 to δH 4.0 and secondary metabolites peaks were prominent in the region ranging from δH 4.5 to δH 8.0. The 1:3 irrigation treatment enabled, in two potato cultivars, the production of significantly high concentrations of secondary metabolites due to the 75% FA: AMD content in the irrigation mixture, which induced stress. The findings suggested that 1:1 irrigation treatment induced production of lower amounts of secondary metabolites in all crops compared to crops irrigated with untreated acid mine drainage treatment and with other FA-treated AMD solutions.

Anti-Pseudomonas aeruginosa activity of a C16-terpene dilactone isolated from the endophytic fungus Neofusicoccum luteum of Kigelia africana (Lam.).

Fungal endophytes have the capacity to biosynthesize secondary metabolites that are produced by their host plants. In this study, a dilactone terpenoid of C16 architecture was isolated from the fungal endophytes of Kigelia africana, in our attempt to identify anti-Pseudomonas aeruginosa metabolites. Thirty-eight fungal isolates were cultured for biomolecule production over a period of thirty days. Extracts from three (ZF 34, ZF 52 and ZF 91) of the fungi showed good anti-P. aeruginosa activity, with ZF 52 presenting the best MIC of 19.53 µg/mL and was accordingly subjected to chromatographic separation. Based on nuclear magnetic resonance (NMR) spectroscopy, high resolution mass spectrometry and single crystal X-ray diffraction (XRD) analyses, the isolated compound was identified as a C16-terpene dilactone, with a structure consistent with that of the known diterpene, CJ-14445. The isolated dilactone showed anti-P. aeruginosa activity with MIC of 0.61 µg/mL, signifying the antibacterial potential of the biomolecule. The bioactive fungal isolate (ZF 52) was identified as Neofusicoccum luteum based on genomic DNA sequencing. This is the first report of the endophyte N. luteum from K. africana and the first reported occurrence of CJ-14445 in the fungus.

Medicinal plants with anti-SARS-CoV activity repurposing for treatment of COVID-19 infection: A systematic review and meta-analysis.

The novel SARS-CoV-2 (severe acute respiratory syndrome coronavirus) has emerged as a significant threat to public health with startling drawbacks in all sectors globally. This study investigates the practicality of some medicinal plants for SARS-CoV-2 therapy using a systematic review and meta-analysis of their reported SARS-CoV-1 inhibitory potencies. Relevant data were systematically gathered from three databases, viz., Web of Science, PubMed and Scopus. The information obtained included botanical information, extraction method and extracts concentrations, as well as the proposed mechanisms. Fourteen articles describing 30 different plants met our eligibility criteria. Random effects model and subgroup analysis were applied to investigate heterogeneity. According to subgroup analysis, the substantial heterogeneity of the estimated mean based on the IC 50 values reporting the most potent anti-SARS-CoV 3C--like protease (3CLpro) inhibitors (10.07 %, p < 0.0001), was significantly higher compared to the most active anti-SARS-CoV papain-like protease (PLpro) inhibitors (6.12 %, p < 0.0001). More importantly, the literature analysis revealed that fruit extracts of Rheum palmatum L. and the compound cryptotanshinone isolated from the root of Salvia miltiorrhiza (IC 50 = 0.8 ± 0.2 µmol L-1) were excellent candidates for anti--SARS-CoV targeting PLpro. Meanwhile, iguesterin (IC 50 = 2.6 ± 0.6 µmol L-1) isolated from the bark of Tripterygium regelii emerged as the most excellent candidate for anti-SARS--CoV targeting 3CLpro. The present systematic review and meta-analysis provide valuable and comprehensive information about potential medicinal plants for SARS-CoV-2 inhibition. The chemotypes identified herein can be adopted as a starting point for developing new drugs to contain the novel virus.

Terpene-rich fractions of Ficus mucoso (Welw) modulate lipopolysaccharide-induced inflammatory mediators and aberrant permeability of the inner mitochondrial membrane in murine animal model.

Ficus mucoso is traditionally used to treat bronchial infections. This study compared the efficacy of terpene-rich fractions of F. mucoso root bark on lipopolysaccharide(LPS)-induced inflammation, liver mitochondrial permeability transition (mPT), an index of mitochondrial health, and associated pathological alterations. Terpene-Rich Fractions of Dichloromethane (TRDF) and Ethylacetate Fractions of F. mucoso (TREF) were obtained according to standard procedures. To induce systemic inflammation, a single intraperitoneal injection of 1mgLPS/kgbw was given to mice. Spectrophotometric techniques were used to evaluate the effects of the oral administration of TRDF and TREF (3 days) on levels of pro-inflammatory mediators (TNF-α, IL-1ß, IL-6) using ELSA techniques as well as antioxidant indices in normal and LPS-treated mice. The mPT pore opening, mitochondrial ATPase activity and lipid peroxidation were monitored spectrophotometrically. Our results revealed that treatment with LPS caused significant elevation in serum cytokine levels while administration of 50 and 100 mg/kg TRDF and TREF significantly reduced elevated serum levels of cytokines (TNF-α, IL-1ß, IL-6) in LPS-challenged mice. In addition, activitities of superoxide dismutase, catalase and liver marker enzymes (ALT and AST) as well as levels of mitochondrial lipid peroxides were significantly reduced in mice treated with TRDF and TREF relative to LPS-fed mice. Furthermore, LPS caused induction of opening of the liver mPT pore which was significantly inhibited by TRDF at 100 and 200 mg/kg bw by 71% and 88%, respectively, but only at 100 mg/kg TREF. Furthermore, mitochondrial ATPase activity was inhibited largely by TRDF. UPLC-ESI-MS analysis revealed the presence of terpenoid derivatives and a few aromatic metabolites in TRDF. The terpene dominance of TRDF metabolites was further justified on the 1H NMR fingerprint. Overall, TRDF is more effective as a cocktail of anti-inflammatory compounds than TREF against LPS-induced acute systemic inflammation.

Anti-Inflammatory Potentials of the n-Hexane Fraction of Alstonia boonei Stem Bark in Lipopolysaccharide-Induced Inflammation in Wistar Rats.

BACKGROUND: Inflammation is a protective response of the host to infections and tissue damage and medicinal plants have been used to regulate inflammatory response. The phytochemical contents of the n-hexane fraction of Alstonia boonei and their anti-inflammatory potentials in lipopolysaccharide-induced inflammation were investigated in rat liver. MATERIALS AND METHODS: A quantity of 5 mg/kg lipopolysaccharide (LPS) was used to induce inflammation in twenty-five male Wistar rats, grouped (n = 5) and treated as follows: negative control (10 mL/kg saline), positive control (1 mg/kg ibuprofen); 50, 100 and 20 mg/kg of the n-hexane fraction of Alstonia boonei were administered to test groups. In another experiment, twenty rats (n = 5, without LPS) were administered the same doses of the n-hexane fraction of A. boonei and ibuprofen for seven days. At the end of the experiment, animals were sacrificed, serum was obtained from blood and liver mitochondria isolated in a refrigerated centrifuge. Mitochondrial permeability transition (mPT) pore opening and mitochondrial F0F1 ATPase (mATPase) were determined spectrophotometrically. Serum interleukins 1ß, 6 (IL-1ß, IL-6), tumour necrosis factor alpha (TNF-α), C-reactive protein (CRP) and creatine kinase (CK), gamma glutamyl transferase (GGT), aspartate and alanine aminotransferases (AST and ALT,) of the animals in which inflammation was induced using LPS but treated with graded doses of n-hexane fraction of A. boonei were determined using the ELISA technique. The phytochemical contents of the n-hexane fraction of A. boonei were determined using ultra performance liquid chromatography-tandem mass spectrometer (UHPLC-MS). RESULTS: Calcium induced mPT in 8 fold and LPS induced mPT 14 fold in the negative control while the n-hexane fraction reversed mPT in the treated groups (50, 100 and 200 mg/kg) to 2, 4, 4 folds, respectively. LPS treatment of the negative group enhanced F0F1 mATPase activity, increased CRP, TNF-α, IL-1ß, IL-6 levels as well as CK, AST, ALT and GGT activities. These values were significantly reduced by 100 and 200 mg/kg of the n-hexane fraction. UHPLC-MS analysis of the fraction revealed the presence of terpenoids, phenolics and sphingolipids. CONCLUSION: These results showed that bioactive phytochemicals present in the n-hexane fraction of A. boonei were not toxic, have an anti-inflammatory effect and could be used for the treatment of inflammatory diseases.

Antimicrobial, Cytotoxic and Oxidative Stress Inhibitory Activities of Terpenoids and Flavonols from Senegalia nigrescens (Oliv.) P.J.H. Hurter.

Senegalia nigrescens (knob thorn) is a deciduous tree distributed in savannah regions from Tanzania to South Africa used for timber but also medicinally for the treatment of convulsions, wounds, and skin problems. In this study, the biological activities of six phytocompounds, namely: 3 ß -hydroxy-20(29)-en-lupan-30-al (1), 30-hydroxylup-20(29)-en-3 ß -ol (2), ent-kaur-15-en-18,20-diol (3), melanoxetin (4), quercetin (5) and quercetin-3-O-methyl ether (6), isolated from S. nigrescens were investigated. The compounds were screened against two bacterial (Escherichia coli and Staphylococcus aureus) and one fungal (Candida albicans) strain and were also tested for their cytotoxicity on breast cancer (MDA-MB-231) and normal murine macrophage (RAW 264.7) cell line. Effects of the compounds on attenuating the lipopolysaccharide (LPS)-induced intracellular reactive oxygen species (ROS) production in RAW 264.7 cells were quantified with the H2DCF-DA assay. This study revealed that flavonols (5 and 6) had the strongest antibacterial and antifungal effects, both having MIC values of 62.5, 31.25 and 31.25 µg/mL on E. coli, S. aureus and C. albicans, respectively. Compounds 2, 3 and 6 were the most cytotoxic against the breast cancer cells with IC50 values of 11.86, 12.62 and 14.03 µg/mL, respectively, while the least toxicity towards normal cells were observed in compounds 2, 5 and 6. All compounds (1-6) significantly lowered ROS production in RAW264.7 cells. In conclusion, tested compounds represent potential promising candidates as antimicrobial, anticancer and antidotes for LPS-induced oxidative stress. This is the first report on the antifungal, cytotoxicity and antioxidative activities of the ent-kaurene diterpenoid, ent-kaur-15-en-18,20-diol (3).

Comparative antimalarial, toxicity and mito-protective effects of Diospyros mespiliformis Hochst. ex A. DC. and Mondia whitei (Hook.f.) Skeels on Plasmodium berghei infection in mice.

ETHNOPHARMACOLOGICAL RELEVANCE: Diospyros mespiliformis Hochst. ex A. DC. and Mondia whitei (Hook.f.) Skeels are traditionally used in Africa for the treatment of malaria. However, scientific evidence to substantiate this folkloric claim and their effects on liver mitochondria during malaria treatment have not been reported. AIM OF THE STUDY: This study investigated the efficacy of D. mespiliformis and M. whitei against chloroquine-sensitive and resistant strains of malarial parasites in mice. It also investigated the toxicity and protection against cellular organelles like mitochondria. MATERIALS AND METHODS: Male Swiss mice were infected with a chloroquine resistant (ANKA) strain of Plasmodium berghei and were treated via oral gavage with methanol extracts of D. mespiliformis and M. whitei reconstituted in diluted dimethylsulfoxide as vehicle (DMSO, 5% v/v) for five consecutive days. Percentage parasite load and clearance were assessed by microscopy. The infected control was treated with the vehicle. Hematological indices were assessed using standard procedures. Alanine aminotransferase (ALT), aspartate aminotransferase (AST) and alkaline phosphatase (ALP) were determined using assay kits. Hepatic mitochondria were isolated via centrifugation, and their permeability transition (mPT), ATPase (mATPase) activity and lipid peroxidation (mLPO) were determined spectroscopically. Liver tissue histology was carried out by standard laboratory procedures. Phytochemical analysis of both extracts were performed using LC-MS to identify the most prominent compounds from each of the extracts. RESULTS: After treatment on day 5, D. mespiliformis and M. whitei at 400 mg/kg decreased mean values for: percentage parasitemia (5.0 ± 1.0, 2.0 ± 0.2), increased Packed Cell Volume (PCV) (36.0 ± 1.4, 36.0 ± 0.0%) and platelets (2.0 ± 1.4, 2.0 ± 2.8 × 105mm3) relative to the untreated control (20.0 ± 5.2; 30.0 ± 0.0%; 1.4 ± 1.4 × 105 mm3, respectively). At the same dose, D. mespiliformis and M. whitei decreased ALT (8.0 ± 3.8, 24.2 ± 4.0U/L), AST (6.2 ± 0.8, 8.0 ± 0.9U/L) and ALP (56.0 ± 0.7, 51.0 ± 1.0U/L) activities compared to the infected control (77.0 ± 10.9U/L, 14.0 ± 0.7U/L and 76.0 ± 6.0U/L, respectively). Both D. mespiliformis and M. whitei reversed mPT opening, decreased mATPase enhancement and mLPO, relative to the control. Histopathology of the liver showed extensive hemorrhagic lesions and severe disseminated congestion in the infected control while both D. mespiliformis and M. whitei were well tolerated at the highest dose. The LC-MS analysis of D. mespiliformis showed the presence of betulinic acid, tocopherol and kaempferol with antimalarial and antioxidant properties while the M. whitei sample contained coumarin and chlorogenic acid that have antimalarial and hepato-protective properties. CONCLUSIONS: D.mespiliformis and M. whitei show antimalarial effects against resistant Plasmodium berghei infection, enhanced cell viability, mito-protection and are not toxic in mice.

Ethnobotany, phytochemistry and pharmacological significance of the genus Bulbine (Asphodelaceae).

ETHNOPHARMACOLOGICAL RELEVANCE: The genus Bulbine (Asphodelaceae) is spread across Southern Africa and Australia and has been traditionally used for various medicinal applications such as treating skin diseases, burns, diarrhoea, and sexually transmitted diseases. AIM OF THIS REVIEW: The aim is to present a critical review of the ethnomedicinally important species of the genus Bulbine with a comprehensive overview of their chemical constituents and biological activities. MATERIALS AND METHODS: This paper is an overview of literature published on the genus Bulbine in the last six decades with regards to phytochemical composition and their respective pharmacological potentials with the aid of data obtained from the search engine Google Scholar with string searches performed using keywords to obtain relevant publications from scientific databases including ACS Journals, PubMed, Science Direct, SciELO, Sci Finder, Springer, Tailor & Francis, The Plant List Database, Web of Science and Wiley. RESULTS: The literature survey reveals that only 12 species in the genus Bulbine have been reported to be used traditionally with scientific records of ethnomedicinal usage Anthraquinones appeared as the most abundant phytochemicals in the genus. Other isolated/detected metabolites include isofuranonaphthoquinones, flavonoids, and triterpenoids. Promising pharmacological activities have been reported by members of the genus with antiplasmodial, antitrypanosomal, antiviral, antioxidant, anticancer, anti-inflammatory and anti-microbial activity, potent wound healing properties as well as improved reproduction. CONCLUSIONS: This review showed the traditional uses of this genus and its preventative and curative properties in the management of the listed diseases providing support from bioassays of the tested compounds and extracts. State-of-the-art analytical techniques are required for the characterisation and quantification of the compounds within the genus. The efficacy of the therapeutic potential of the Bulbine species need to be further confirmed with pre-clinical and clinical studies.

Clean technology for synchronous sequestration of charged organic micro-pollutant onto microwave-assisted hybrid clay materials.

The Sustainable Development Goal 6 (SDG #6) of the United Nations (UN) is hinged on the provision, availability, and sustainability of water for the global populace by 2030. In a bid to achieve this goal, the quest to seek for ubiquitous and low-cost adsorbents to treat effluents laden with industrial dyes, such as methylene blue (MB), is on the increase in recent years. Acute exposure of humans to (MB) dye causes cyanosis, necrosis, and jaundice and even leads to death. In this research, zinc-modified hybrid clay composite adsorbent (materials from kaolinite and biomass (crushed Carica papaya seeds and/or plantain peel)) was developed via microwave route. This adsorbent was characterized using field emission scanning electron microscopy (FE-SEM), Fourier transform infrared (FTIR) spectroscopy, energy-dispersive X-ray (EDX), and high-resolution transmission electron microscopy (HR-TEM). These characterization techniques confirmed the success achieved in doping hybrid clay with Zn. These adsorbents were used to sequester cationic dye (MB) from aqueous solutions and textile effluent under various experimental conditions. The adsorption and desorption data obtained were analyzed using various kinetic models, which are two-step kinetics, pseudo-first order, pseudo-second order, fractal kinetics, first-order desorption, second-order desorption, and modified statistical rate theory (MSRT) desorption models. Results showed that the adsorption of the dye occurred via several chemical interactions, while the latter models (for desorption) indicated that desorption occurred in two different desorption sites on the adsorbent surfaces, which showed that the adsorption of MB dye onto the adsorbents was stable without the emergence of any secondary pollution. Adsorption of MB was achieved within 15 min for aqueous solutions and 900 min for textile effluent, which is an improvement on previous results from other studies. The three adsorption-desorption cycles for MB uptake by the adsorbents showed that it is pragmatically applicable to treat textile effluents. Hence, low-cost composite adsorbents have a potential for the effective remediation of MB dye from textile effluents as this study confirmed.

Visible-Light-Mediated Photodynamic Water Disinfection @ Bimetallic-Doped Hybrid Clay Nanocomposites.

This study reports a new class of photocatalytic hybrid clay nanocomposites prepared from low-cost sources (kaolinite clay and Carica papaya seeds) doped with Zn and Cu salts via a solvothermal process. X-ray diffraction analysis suggests that Cu-doping and Cu/Zn-doping introduce new phases into the crystalline structure of Kaolinite clay, which is linked to the reduced band gap of kaolinite from typically between 4.9 and 8.2 eV to 2.69 eV for Cu-doped and 1.5 eV for Cu/Zn hybrid clay nanocomposites (Nisar, J.; Århammar, C.; Jämstorp, E.; Ahuja, R. Phys. Rev. B 2011, 84, 075120). In the presence of solar light irradiation, Cu- and Cu/Zn-doped nanocomposites facilitate the electron-hole pair separation. This promotes the generation of singlet oxygen which in turn improves the water disinfection efficiencies of these novel nanocomposite materials. The nanocomposite materials were further characterized using high-resolution scanning electron microscopy, fluorimetry, thermogravimetric analysis, and Raman spectroscopy. The breakthrough times of the nanocomposites for a fixed bed mode of disinfection of water contaminated with 2.32 × 107 cfu/mL E. coli ATCC 25922 under solar light irradiation are 25 h for Zn-doped, 30 h for Cu-doped, and 35 h for Cu/Zn-doped nanocomposites. In the presence of multidrug and multimetal resistant strains of E. coli, the breakthrough time decreases significantly. Zn-only doped nanocomposites are not photocatalytically active. In the absence of light, the nanocomposites are still effective in decontaminating water, although less efficient than under solar light irradiation. Electrostatic interaction, metal toxicity, and release of singlet oxygen (only in the Cu-doped and Cu/Zn-doped nanocomposites) are the three disinfection mechanisms by which these nanocomposites disinfect water. A regrowth study indicates the absence of any living E. coli cells in treated water even after 4 days. These data and the long hydraulic times (under gravity) exhibited by these nanocomposites during photodisinfection of water indicate an unusually high potential of these nanocomposites as efficient, affordable, and sustainable point-of-use systems for the disinfection of water in developing countries.

Quorum sensing inhibitory potential and in silico molecular docking of flavonoids and novel terpenoids from Senegalia nigrescens.

ETHNOPHARMACOLOGICAL RELEVANCE: Senegalia nigrescens is used in traditional medicine for the treatment of dysentery and convulsions. AIMS OF THE STUDY: This study was aimed at identifying bioactive compounds from S. nigrescens and carrying out in vitro and in silico anti-quorum sensing studies on the compounds. MATERIALS AND METHODS: Extracts of S. nigrescens were chromatographed repeatedly. The isolated compounds were characterised using NMR spectroscopy and mass spectrometry. The anti-quorum sensing potential of S. nigrescens crude extracts and selected phytochemicals was quantified using Chromobacterium violaceum quorum sensing-controlled violacein inhibition assays. Qualitative modulation of quorum sensing activity and signal synthesis was investigated using agar diffusion double ring assays and C. violaceum. Molecular docking was conducted to explore the binding conformations of ent-kaurene diterpenes and flavonoids into the binding sites of quorum sensing regulator proteins, CviR and CviR'. RESULTS: Phytochemical investigation of S. nigrescens resulted in the isolation of a new ent-kaurene diterpenoid (ent-kaur-15-en-18,20-diol) alongside ent-kaur-15-en-18-ol, being isolated for the first time from a plant species. Other compounds isolated included 30-hydroxylup-20(29)-en-3ß-ol, 3ß-hydroxy-20(29)-en-lupan-30-al, lupeol, stigmasterol, a long chain alcohol (tetracosan-1-ol) and three flavonoids (melanoxetin, quercetin and quercetin-3-O-methyl ether). Structures of isolated compounds were elucidated using different spectroscopic techniques including 1D and 2D NMR. Inhibition of violacein production was concentration-dependent, with 56.52% inhibition being obtained with 200 µg of quercetin-3-O-methyl ether, while 53.38% inhibition was obtained with 600 µg of quercetin. Agar diffusion double ring assays indicated CviI synthase/CviR receptor modulation by S. nigrescens phytochemicals, suggesting that quorum signal synthesis was down-regulated and/or targeting binding of signal to the receptor. The computed binding energy data suggested that the flavonoids had a stronger tendency to inhibit both CviR and CviR' with varying binding affinities. CONCLUSION: S. nigrescens crude extracts together with the novel ent-kaurenoids and flavonoids demonstrated potential anti-quorum sensing activity. S. nigrescens may thus represent a source of anti-quorum sensing therapeutic candidates for the control of existing and emerging infectious diseases.

Phytochemical Analysis with Antioxidant and Cytotoxicity Studies of the Bioactive Principles from Zanthoxylum capense (Small Knobwood).

BACKGROUND: Zanthoxylum capense (small knobwood) is a South African species known for a wide range of anecdotal uses. However, there is a dearth of information on its phytoconstitutional make-up, specifically its knobs, with only a few reports on the bioactive compounds that could justify its ethnomedicinal use. OBJECTIVES: This work aimed to identify the active principles in Z. capense and evaluate their cytotoxicity against breast cancer tumor cells. METHOD: Extracts from the stem bark, knobs and leaves were purified using chromatographic methods and characterized using spectroscopic techniques. Cytotoxicity of isolated compounds was evaluated on mammalian MCF-7, Caco-2 tumor cell lines and HEK295, a normal kidney cell line. RESULTS: The following compounds were isolated from the plant: a quaternary benzophenanthridine-type alkaloid (chelerythrine) along with its alkanoamine derivative (6-hydroxydihydrochelerythrine), an indolopyridoquinazoline alkaloid (rutaecarpine), an alkyl p-coumaric acid ester (dodecyl-trans-p-coumarate), a lignan (sesamin), a flavanol (catechin), two triterpenoids (lupeol and sitosterol) and two pigments (pheophytin a and lutein). In the cytotoxicity study, all tested samples decreased the viability of the MCF-7 tumor cells by at least 23% at concentration 1 µg mL-1 and Caco-2 tumor cells by at least 15% at concentration 5 µg mL-1 but a mild toxic effect on HEK295 across the tested samples. RESULTS: The following compounds were isolated from the plant: a quaternary benzophenanthridine-type alkaloid (chelerythrine) along with its alkanoamine derivative (6-hydroxydihydrochelerythrine), an indolopyridoquinazoline alkaloid (rutaecarpine), an alkyl p-coumaric acid ester (dodecyl-trans-p-coumarate), a lignan (sesamin), a flavanol (catechin), two triterpenoids (lupeol and sitosterol) and two pigments (pheophytin a and lutein). In the cytotoxicity study, all tested samples decreased the viability of the MCF-7 tumor cells by at least 23% at concentration 1 µg mL-1 and Caco-2 tumor cells by at least 15% at concentration 5 µg mL-1 but a mild toxic effect on HEK295 across the tested samples.

A dual-purpose silver nanoparticles biosynthesized using aqueous leaf extract of Detarium microcarpum: An under-utilized species.

The need for green synthesis of emerging industrial materials has led to the biosynthesis of nanoparticles from plants to circumvent the adverse by-products of chemical synthesis. In this study, the leaf extract of Detarium mirocarpum Guill & Perr, a small tree belonging to the family Fabaceae (Legume), was used to synthesize silver nanoparticles (DAgNPs). DAgNPs were characterized using spectroscopic techniques (Ultraviolet-Visible spectroscopy and Fourier Transform Infrared spectroscopy) which showed hydroxyl and carbonyl functional groups to be responsible for their synthesis. DAgNPs were observed to be crystalline and spherical. The average size, determined by transmission electron microscopy (TEM) was 17.05nm. The antioxidant activity of DAgNPs ranked from moderate to good. The ability of DAgNPs to sense Hg(2+) and Fe(3+) ions in aqueous medium was also investigated. The quenching of the SPR peak at 430nm was used to monitor the toxic and heavy metal ions with linear ranges of 20-70µgmL(-1) and 10-40µgmL(-1) for Hg(2+) and Fe(3+), respectively. The limit of detection (LOD) and limit of quantification (LOQ) obtained for Hg(2+) was 2.05µgmL(-1) and 6.21µgmL(-1), respectively and for Fe(3+) was 5.01µgmL(-1) and 15.21µgmL(-1), respectively. The intra- and inter-day assessments of accuracy and repeatability gave relative errors less than 1% in all instances. DAgNPs can therefore provide a convenient method of sensing the toxic metals easily.