Light-responsive and ultrapermeable two-dimensional metal-organic framework membrane for efficient ionic energy harvesting.

Nanofluidic membranes offer exceptional promise for osmotic energy conversion, but the challenge of balancing ionic selectivity and permeability persists. Here, we present a bionic nanofluidic system based on two-dimensional (2D) copper tetra-(4-carboxyphenyl) porphyrin framework (Cu-TCPP). The inherent nanoporous structure and horizontal interlayer channels endow the Cu-TCPP membrane with ultrahigh ion permeability and allow for a power density of 16.64 W m-2, surpassing state of-the-art nanochannel membranes. Moreover, leveraging the photo-thermal property of Cu-TCPP, light-controlled ion active transport is realized even under natural sunlight. By combining solar energy with salinity gradient, the driving force for ion transport is reinforced, leading to further improvements in energy conversion performance. Notably, light could even eliminate the need for salinity gradient, achieving a power density of 0.82 W m-2 in a symmetric solution system. Our work introduces a new perspective on developing advanced membranes for solar/ionic energy conversion and extends the concept of salinity energy to a notion of ionic energy.

Unlocking osmotic energy harvesting potential in challenging real-world hypersaline environments through vermiculite-based hetero-nanochannels.

Nanochannel membranes have demonstrated remarkable potential for osmotic energy harvesting; however, their efficiency in practical high-salinity systems is hindered by reduced ion selectivity. Here, we propose a dual-separation transport strategy by constructing a two-dimensional (2D) vermiculite (VMT)-based heterogeneous nanofluidic system via an eco-friendly and scalable method. The cations are initially separated and enriched in micropores of substrates during the transmembrane diffusion, followed by secondary precise sieving in ultra-thin VMT laminates with high ion flux. Resultantly, our nanofluidic system demonstrates efficient osmotic energy harvesting performance, especially in hypersaline environment. Notably, we achieve a maximum power density of 33.76 W m-2, a 6.2-fold improvement with a ten-fold increase in salinity gradient, surpassing state-of-the-art nanochannel membranes under challenging conditions. Additionally, we confirm practical hypersaline osmotic power generation using various natural salt-lake brines, achieving a power density of 25.9 W m-2. This work triggers the hopes for practical blue energy conversion using advanced nanoarchitecture.

Nobiletin Ameliorates Nonalcoholic Fatty Liver Disease by Regulating Gut Microbiota and Myristoleic Acid Metabolism.

Disturbance of the gut microbiota plays a critical role in the development of nonalcoholic fatty liver disease (NAFLD). Increasing evidence supports that natural products may serve as prebiotics to regulate the gut microbiota in the treatment of NAFLD. In the present study, the effect of nobiletin, a naturally occurring polymethoxyflavone, on NAFLD was evaluated, and metabolomics, 16S rRNA gene sequencing, and transcriptomics analysis were performed to determine the underlying mechanism of nobiletin, and the key bacteria and metabolites screened were confirmed by in vivo experiment. Nobiletin treatment could significantly reduce lipid accumulation in high-fat/high-sucrose diet-fed mice. 16S rRNA analysis demonstrated that nobiletin could reverse the dysbiosis of gut microbiota in NAFLD mice and nobiletin could regulate myristoleic acid metabolism, as revealed by untargeted metabolomics analysis. Treatment with the bacteria Allobaculum stercoricanis, Lactobacillus casei, or the metabolite myristoleic acid displayed a protective effect on liver lipid accumulation under metabolic stress. These results indicated that nobiletin might target gut microbiota and myristoleic acid metabolism to ameliorate NAFLD.

Evolving interplay between natural products and gut microbiota.

Growing evidence suggests gut microbiota status affects human health, and microbiota imbalance will induce multiple disorders. Natural products are gaining increasing attention for their therapeutical effects and less side effects. The emerging studies support that the activities of many natural products are dependent on gut microbiota, meanwhile gut microbiota is modulated by natural products. In this review, we summarized the interplay between the gut microbiota and host disease, and the emerging molecular mechanisms of the interaction between natural products and gut microbiota. Focusing on gut microbiota metabolite of various natural products, and the effects of natural products on gut microbiota, we summarized the biotransformation pathways of natural products, and discussed the effect of natural products on the composition modulation of gut microbiota, protection of gut mucosal barrier and modulation of the gut microbiota metabolites. Dissecting the interplay between gut microbiota and natural products will help elucidate the therapeutic mechanisms of natural products.

Selective Ion Transport in Two-Dimensional Lamellar Nanochannel Membranes.

Precise and ultrafast ion sieving is highly desirable for many applications in environment-, energy-, and resource-related fields. The development of a permselective lamellar membrane constructed from parallel stacked two-dimensional (2D) nanosheets opened a new avenue for the development of next-generation separation technology because of the unprecedented diversity of the designable interior nanochannels. In this Review, we first discuss the construction of homo- and heterolaminar nanoarchitectures from the starting materials to the emerging preparation strategies. We then explore the property-performance relationships, with a particular emphasis on the effects of physical structural features, chemical properties, and external environment stimuli on ion transport behavior under nanoconfinement. We also present existing and potential applications of 2D membranes in desalination, ion recovery, and energy conversion. Finally, we discuss the challenges and outline research directions in this promising field.

Novel hydrophilic straw biochar for the adsorption of neonicotinoids: kinetics, thermodynamics, influencing factors, and reuse performance.

Nitenpyram (NIT) is the most water-soluble neonicotinoid (NEO). It has been shown to pose a serious threat to human health and the environment but was always ignored due to its limited market share. There were few experts who studied NIT's transport behavior on biochar. In this study, two types of biochar were co-activated separately using zinc chloride combined with phosphoric acid and potassium hydroxide combined with acetic acid, marked as ZBC and KBC. Characterizations suggested that hydrophilic ZBC and KBC had more surface functional groups than unmodified biochar (BC), and specific surface areas of ZBC (456.406 m2·g-1) and KBC (750.588 m2·g-1) were significantly higher than of BC (67.181 m2·g-1). The pore structures of KBC and ZBC were hierarchical porous structures with different pore sizes and typical microporous structure, respectively. The adsorption performance of either NIT or IMI on KBC was better than that on ZBC. Only 0.4 g·L-1 of KBC can absorb 89.62% of NIT in just 5 min. The equilibrium adsorption amounts of NIT on ZBC and KBC were 17.995 mg·g-1 and 82.910 mg·g-1. Elovich and Langmuir models were used to evaluate the whole adsorption process, which was attributed to the chemisorption mechanism. In addition, removal rates of NIT were negatively correlated to NIT's initial concentration and positively correlated to the dose of biochar. pH had almost no effect on adsorption, but the presence of salt ions can inhibit the removal of NIT. Long-term stabilities of biochars were also acceptable. These findings will promote the development in the preparation of biochar fields and provide a positive reference value for NEO removal.

Anti-obesity natural products and gut microbiota.

The link between gut microbiota and obesity or other metabolic syndromes is growing increasingly clear. Natural products are appreciated for their beneficial health effects in humans. Increasing investigations demonstrated that the anti-obesity bioactivities of many natural products are gut microbiota dependent. In this review, we summarized the current knowledge on anti-obesity natural products acting through gut microbiota according to their chemical structures and signaling metabolites. Manipulation of the gut microbiota by natural products may serve as a potential therapeutic strategy to prevent obesity.

In vitro human intestinal microbiota biotransformation of nobiletin using liquid chromatography-mass spectrometry analysis and background subtraction strategy.

In this study, the in vitro biotransformation of nobiletin by human intestinal microbiota, which is a bioactive polymethoxyflavone widely presented in Citrus plants, has been investigated via utilizing an anaerobic incubation protocol. The incubation samples were detected using high-performance liquid chromatography/quadrupole time-of-flight mass spectrometry. A background subtraction strategy incorporated in Microsoft Office was employed to eliminate the interferences in medium and feces. The parent and three metabolites sinensetin, 5-hydroxy-6,7,3',4'-tetramethoxyflavone, and 5-demethylnobiletin were detected and identified based on the characteristics of their protonated molecules. The proposed metabolic pathway revealed that nobiletin went through phase I metabolism including demethylation and demethoxylation in human intestinal microbiota. The characterization of nobiletin metabolic profile transformed by human intestinal bacteria would be helpful for understanding its efficacy and action mechanism.

Intestinal α1-2-Fucosylation Contributes to Obesity and Steatohepatitis in Mice.

BACKGROUND & AIMS: Fucosyltransferase 2 (Fut2)-mediated intestinal α1- 2-fucosylation is important for host-microbe interactions and has been associated with several diseases, but its role in obesity and hepatic steatohepatitis is not known. The aim of this study was to investigate the role of Fut2 in a Western-style diet-induced mouse model of obesity and steatohepatitis. METHODS: Wild-type (WT) and Fut2-deficient littermate mice were used and features of the metabolic syndrome and steatohepatitis were assessed after 20 weeks of Western diet feeding. RESULTS: Intestinal α1-2-fucosylation was suppressed in WT mice after Western diet feeding, and supplementation of α1-2-fucosylated glycans exacerbated obesity and steatohepatitis in these mice. Fut2-deficient mice were protected from Western diet-induced features of obesity and steatohepatitis despite an increased caloric intake. These mice have increased energy expenditure and thermogenesis, as evidenced by a higher core body temperature. Protection from obesity and steatohepatitis associated with Fut2 deficiency is transmissible to WT mice via microbiota exchange; phenotypic differences between Western diet-fed WT and Fut2-deficient mice were reduced with antibiotic treatment. Fut2 deficiency attenuated diet-induced bile acid accumulation by altered relative abundance of bacterial enzyme 7-α-hydroxysteroid dehydrogenases metabolizing bile acids and by increased fecal excretion of secondary bile acids. This also was associated with increased intestinal farnesoid X receptor/fibroblast growth factor 15 signaling, which inhibits hepatic synthesis of bile acids. Dietary supplementation of α1-2-fucosylated glycans abrogates the protective effects of Fut2 deficiency. CONCLUSIONS: α1-2-fucosylation is an important host-derived regulator of intestinal microbiota and plays an important role for the pathogenesis of obesity and steatohepatitis in mice.

Citrus polymethoxyflavones attenuate metabolic syndrome by regulating gut microbiome and amino acid metabolism.

Metabolic syndrome (MetS) is intricately linked to dysregulation of gut microbiota and host metabolomes. Here, we first find that a purified citrus polymethoxyflavone-rich extract (PMFE) potently ameliorates high-fat diet (HFD)-induced MetS, alleviates gut dysbiosis, and regulates branched-chain amino acid (BCAA) metabolism using 16S rDNA amplicon sequencing and metabolomic profiling. The metabolic protective effects of PMFE are gut microbiota dependent, as demonstrated by antibiotic treatment and fecal microbiome transplantation (FMT). The modulation of gut microbiota altered BCAA levels in the host serum and feces, which were significantly associated with metabolic features and actively responsive to therapeutic interventions with PMFE. Notably, PMFE greatly enriched the commensal bacterium Bacteroides ovatus, and gavage with B. ovatus reduced BCAA concentrations and alleviated MetS in HFD mice. PMFE may be used as a prebiotic agent to attenuate MetS, and target-specific microbial species may have unique therapeutic promise for metabolic diseases.

A simple method to discriminate Guangchenpi and Chenpi by high-performance thin-layer chromatography and high-performance liquid chromatography based on analysis of dimethyl anthranilate.

Citri Reticulatae Pericarpium (CRP), the dried pericarp of Citrus reticulata Blanco, can be divided into "Guangchenpi" (GCP, the dried pericarps derived from Citrus reticulata 'Chachi') and "Chenpi" (CP, the dried pericarps derived from other cultivars of Citrus reticulata Blanco). To discriminate between GCP and CP, a simple and reliable high-performance thin-layer chromatography (HPTLC) method was firstly developed to analyze the volatile compound dimethyl anthranilate, and a high-performance liquid chromatography (HPLC) method was established to simultaneously quantify dimethyl anthranilate and three predominant flavonoids (hesperidin, nobiletin and tangeretin) in CRP samples. Both the HPTLC analysis and HPLC-orthogonal partial least squares discrimination analysis (OPLS-DA) indicated that GCP can be effectively distinguished from CP based on analysis of dimethyl anthranilate. Our results indicated that dimethyl anthranilate can be used as a marker compound for discrimination of GCP and CP. This work provided a convenient approach which might be applied for quality evaluation of CRP.

Cultivar differentiation of Citri Reticulatae Pericarpium by a combination of hierarchical three-step filtering metabolomics analysis, DNA barcoding and electronic nose.

The traditional Chinese medicine Citri Reticulatae Pericarpium (CRP) was mainly originated from the dried pericarp of Citrus reticulata 'Chachi' (Crc), Citrus reticulata 'Dahongpao' (Crd), Citrus reticulata 'Unshiu' (Cru) and Citrus reticulata 'Tangerina' (Crt) in China. Since these four cultivars have great similarities in morphology, reliable methods to differentiate CRP cultivars have rarely been reported. To discriminate the differences of these CRP cultivars, herein an efficient and reliable method by combining metabolomics, DNA barcoding and electronic nose was first established. The hierarchical three-step filtering metabolomics analysis based on liquid chromatography-quadrupole time-of-flight mass spectrometry (LC-QTOF-MS) indicated that 9 species-specific chemical markers including 6 flavanone glycosides and 3 polymethoxyflavones could be considered as marker metabolites for discrimination of the geoherb Crc from other cultivars. A total of 19 single nucleotide polymorphism (SNP) sites were found in nuclear internal transcribed spacer 2 (ITS2) of CRP, and three stable SNP sites (33, 128 and 174) in the ITS2 region can distinguish the four CRP cultivars. The electronic nose coupled with chemometrics could also be used to effectively distinguish Crc from other CRP cultivars. Therefore, our results indicated that the integrated method will be an effective strategy for discrimination of similar herbal medicines.

Evaluation of anti-lipase activity and bioactive flavonoids in the Citri Reticulatae Pericarpium from different harvest time.

BACKGROUND: Inhibition of pancreatic lipase is an attractive approach to the treatment of obesity and other metabolic disorders. Naturally occurring phytochemicals are promising sources of lipase inhibitors. PURPOSE: In the present study, the anti-lipase activity of Citri Reticulatae Pericarpium (CRP) extracts was firstly evaluated in vitro. Moreover, the dynamic alteration of bioactive flavonoids in CRP collected at different time and its correlation with anti-lipase activities was investigated. STUDY DESIGN/METHODS: Quantitative analysis of multi-components by a single-marker (QAMS) method was developed and validated for simultaneous determination of six flavonoids including narirutin, hesperidin, didymin, nobiletin, 3,5,6,7,8,3',4'-heptamethoxyflavone and tangeretin. Anti-lipase activity evaluation and docking studies of the flavonoids was also carried out to screen out the candidate lipase inhibitors. RESULTS: The QAMS method validation results exhibited that the developed method had desirable specificity, linearity, precision and accuracy. CRP collected in early months contained higher concentrations of bioactive flavonoids, and exhibited more potent anti-lipase activity. CONCLUSION: Harvest timing had a significant impact on the amounts of bioactive flavonoids and the anti-lipase activities of CRP extracts. The contents of total flavonoids were positively correlated with the anti-lipase activities of CRP, and polymethoxyflavones played a significant role in the hypolipidemic effect of CRP. Nobiletin might be the most potential lipase inhibitor in CRP.

Qualitative and quantitative analysis of chemical constituents in Ardisiae Japonicae Herba.

Ardisiae Japonicae Herba is a well-known traditional Chinese medicine for the treatment of bronchitis conjunctivitis, pneumonia, and trauma. In this work, a high-performance liquid chromatography coupled with quadrupole time-of-flight mass spectrometry method was first established for the separation and structural identification of the chemical constituents in Ardisiae Japonicae Herba. A total of 15 compounds including coumarins, flavonoid glycosides, and catechins were identified or tentatively characterized based on their chromatographic behaviors and mass spectral fragmentation and by comparisons with the reference standards. Furthermore, a simple high-performance liquid chromatography with diode array detection method was developed for the simultaneous determination of five major constituents. Results obtained from method validation, including linearity, precision, repeatability, stability, and recovery, showed that the established method was reliable and accurate. Bergenin and quercitrin were found to be the most abundant constituents and could be served as chemical markers for quality control of Ardisiae Japonicae Herba.

A new compound, methylbergenin along with eight known compounds with cytotoxicity and anti-inflammatory activity from Ardisia japonica.

A new compound, methylbergenin (1), was isolated from the whole plants of Ardisia japonica (Thunb.) Bl. (Myrsinaceae), along with eight known compounds: demethoxybergenin (2), bergenin (3), afzelin (4), quercitrin (5), bauerenol (6), bauerenone (7), α-spinasterol (8) and chondrillasterone (9). Compounds 1, 7 and 9 were isolated from A. japonica for the first time. The structure of compound 1 was determined on the basis of NMR (1D and 2D) and mass spectroscopic analysis. The absolute configuration of 1 was assessed by single-crystal X-ray diffraction. Compounds 1, 4, 5, 7 and 9 showed potential inhibitory effects against nitric oxide production in LPS stimulated RAW 264.7 murine macrophages. In addition, Compounds 7 and 9 exhibited cytotoxicity against A549 and HepG-2 cells.

Novel naphtho[2,1-d]oxazole-4,5-diones as NQO1 substrates with improved aqueous solubility: Design, synthesis, and in vivo antitumor evaluation.

A new series of ortho-naphthoquinone analogs of ß-lapachone were designed, synthesized and evaluated. The biological results indicated that most of our compounds were efficient substrates for NQO1. The new scaffold with water-soluble side chain resulted in greater solubility under acidic condition compared to ß-lapachone. Thus avoiding the use of hydroxylpropyl ß-cyclodextrin which would finally cause the rapid drug clearance from the blood and dose-limiting toxicity in the form of hemolytic anemia. The most soluble and promising compound in this series was 2-((4-benzylpiperazin-1-yl)methyl)naphtho[2,1-d]oxazole-4,5-dione (3k), which inhibited cancer cell (NQO1-rich A549 cell line) growth at IC50 values of 4.6±1.0µmol·L(-1). Furthermore, compound 3k had in vivo antitumor activity in an A549 tumor xenografts mouse model comparable to the activity obtained with ß-lapachone. The results indicated that these ortho-naphthoquinones could serve as promising leads for further optimization as novel substrates for NQO1.

Two new triterpenoid glycosides from the leaves of Anthocephalus chinensis.

Nine compounds were isolated from the leaves of Anthocephalus chinensis by column chromatography on silica gel and Sephadex LH-20, and their structures were elucidated by spectroscopic techniques as clethric acid-28-O-ß-d-glucopyranosyl ester (1), mussaendoside T (2), ß-stigmasterol (3), hederagenin (4), ursolic acid (5), clethric acid (6), 3ß,6ß,19α,24-tetrahydroxyurs-12-en-28-oic acid (7), mussaendoside I (8), and cadambine (9). Compounds 1 and 2, and 7 and 8 were isolated from the plants of this genus for the first time, and compounds 1 and 2 were new triterpenoid glycosides.