JOURNAL OF ORGANIC CHEMISTRY
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2024
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IF 3.3
Hui Xu,Zhi-Jiang Jiang,Yun Jia,Yuhang Su,Jian-Fei Bai,Zhanghua Gao,Jia Chen,Kun Gao
Aromatic sulfones are the prevailing scaffolds in pharmaceutical and material sciences. However, compared to their widespread application, the selective deuterium labeling of these structures is restricted due to their electron-deficient properties. This study presents two comprehensive strategies for the deuteration of aromatic sulfones. The base-promoted deuteration uses DMSO-d6 as the deuterium source, resulting in a rapid H/D exchange within 2 h. Meanwhile, a silver-catalyzed protocol offers a much milder option by using economical D2O to furnish the labeled sulfones.
研究领域:
药物化学
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材料科学
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有机合成
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ACS Nano
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2026
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IF 17.3
Lin Liu,Xiuxiu Wang,Xinran Song,Hui Huang,Xiaoyu Geng,Xue Wang,Wei Yan,Tianming Xu,Meiqi Chang,Yu Chen,Jishun Yang
Jellyfish envenomation poses a significant clinical challenge, with Nemopilema nomurai (N. nomurai) venom capable of inducing life-threatening hepatotoxicity through mechanisms that remain poorly understood. Here, we demonstrate that its tentacle extract (TE) simultaneously triggers a reactive oxygen species (ROS) burst, activates the canonical NLRP3/Caspase-1/Gasdermin D (GSDMD) pyroptosis pathway, and induces ZDHHC9-dependent GSDMD palmitoylation, collectively contributing to hepatic injury. To counteract this dual-pathway activation, we engineered ultrasmall iridium nanoantidotes (Ir NAs) with multienzyme mimetic activities, which effectively scavenge ROS, thereby suppressing both NLRP3 inflammasome activation and GSDMD palmitoylation while preserving mitochondrial function. These nanoantidotes significantly attenuated hepatocyte pyroptosis and histopathological damage, reduced mortality in vivo, and exhibited favorable biocompatibility with rapid clearance. Our work not only identifies GSDMD palmitoylation as a critical event in jellyfish venom-induced hepatotoxicity but also presents a translatable nanotherapeutic strategy for marine envenomation and related inflammatory disorders.
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Frontiers in Microbiology
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2023
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IF 5.2
Zhai Fanfan,Hao Li,Chen Xiaomin,Jiang Ting,Guo Qianhong,Xie Liping,Ma Ying,Du Xiaobo,Zheng Zhiqin,Chen Kun,Fan Jun
Autoblinking is a widespread phenomenon and exhibits high level of intensity in some bacteria. In Deinococcus radiodurans (D. radiodurans), strong autoblinking was found to be indistinguishable from PAmCherry and greatly prevented single-molecule tracking of proteins of interest. Here we employed the bright photoswitchable fluorescent protein mMaple3 to label PprI, one essential DNA repair factor, and characterized systematically the fluorescence intensity and bleaching kinetics of both autoblinking and PprI-mMaple3 molecules within cells grown under three different conditions. Under minimal media, we can largely separate autoblinking from mMaple3 molecules and perform reliably single-molecule tracking of PprI in D. radiodurans, by means of applying signal-to-noise ratio and constraining the minimal length for linking the trajectories. We observed three states of PprI molecules, which bear different subcellular localizations and distinct functionalities. Our strategy provides a useful means to study the dynamics and distributions of proteins of interest in bacterial cells with high level of autoblinking.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2023
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IF 3.1
Yibo Guo,Ke Shen,Xinshuai Zhang,Hua Huang
l -threonate is the metabolite of vitamin C, while d -erythronate is the metabolite of N -acetyl- d -glucosamine, the nutritional supplement for joint health. They are widely distributed in the environment and human biofluids. Nevertheless, the catabolisms of l -threonate and d -erythronate are sparsely reported. Here we explored the functional diversity of an acid sugar kinase family (Pfam families PF07005-PF17042), and discovered a novel 2-oxo-tetronate kinase. The conserved genome neighborhood of the 2-oxo-tetronate kinase encodes members of class-II fructose-bisphosphate aldolase family (F_bP_aldolase, PF01116) and a dehydrogenase family (PF03446-PF14833). Instructed by this analysis, we experimentally verified that these enzymes are capable of degrading l -threonate into dihydroxyacetone phosphate (DHAP) in Arthrobacter sp. ZBG10, Clostridium scindens ATCC 35704, and Pseudonocardia dioxanivorans ATCC 55486. Meanwhile, a convergent catabolic pathway for d -erythronate was characterized in P . dioxanivorans ATCC 55486. Moreover, the phylogenetic distribution analysis indicates that the biological range of the identified l -threonate and d -erythronate catabolic pathways appears to extend mostly to members of the Actinomycetota , Cyanobacteriota , Bacillota , Pseudomonadota , and Bacteroidota phyla.
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Natural Products and Bioprospecting
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2018
·Vol. 8
·期 6
·413-418
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IF 0
Wang Xia,Peng Xing-Rong,Lu Jing,Hu Gui-Lin,Qiu Ming-Hua
Abstract In present study, four new dammarane-type triterpenoids, namely caffruones A–D ( 1 – 4 ), were isolated from the cherries of Coffea arabica . Their structures were elucidated by extensive spectroscopic analysis including 1D, 2D NMR (HSQC, HMBC, 1 H– 1 H COSY, and ROESY), HRMS and IR spectra. This is the first time that tetracyclic triterpenes have been reported in genus Coffea . Graphical Abstract
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BIOMEDICINE & PHARMACOTHERAPY
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2018
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IF 3.457
Yuhui Wang,Jinyang Shen,Xiaolin Yang,Ye Jin,Zhonglin Yang,Rufeng Wang,Fuming Zhang,Robert J. Linhardt
Background Glucocorticoid hormones are implicated in the pathogenesis of Alzheimer’s disease (AD) and other diseases including diabetes, hyperlipidemia , and osteoporosis . Akebia saponin D (ASD) possesses numerous pharmacological activities , including as an anti-AD, anti-hyperlipidemia, anti-diabetes, and anti-osteoporosis agent. The anti-AD effect of ASD is possibly through its regulation of glucocorticoid levels. Purpose The present study was undertaken to investigate the neuroprotective effects of ASD on Aβ 25-35 -induced cognitive deficits and to elucidate its underlying mechanism of action. Methods The AD rat model was established by an intracerebroventricular injection of Aβ 25-35 into the lateral ventricles. Spatial learning and anxiety state were assessed by Morris water maze task and elevated plus-maze assay, respectively. The degree of hypertrophy of adrenal gland was analyzed using the viscera coefficient. Corticosterone and ACTH concentrations in the plasm were measured using biochemical assay kits. The activity of 11β-hydroxysteroid dehydrogenase type-1 (11β-HSD1) in liver and groin fat pad was assessed by measuring cortisol production. Results Compared with the control group, AD rats displayed significant spatial learning and reference memory impairments, serious anxiety disorders, obvious hypertrophy of adrenal gland, elevated corticosterone and ACTH levels in the plasma, and increased 11β-HSD1 activity in liver and groin fat pad. ASD could significantly ameliorate the memory deficits and anxiety symptoms, markedly reduce the viscera coefficient of adrenal gland, observably decrease corticosterone and ACTH concentrations, and showed no effect on the activity of 11β-HSD1. Conclusions These results indicate that ASD might exert a significant neuroprotective effect on cognitive impairment, driven in part by reducing systemic corticosterone level by down-regulation of the hypothalamic-pituitary-adrenal (HPA) axis.
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AMINO ACIDS
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2018
·Vol. 50
·期 9
·1269-1278
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IF 2.906
Wu Pinping,Hu Fan,Wang Ruya,Gao Lingxuan,Huang Tao,Xin Yufu,He Hua
A new colorimetric analysis approach for chiral recognition of d - and l -forms of phenylalanine (phe) was developed based on triangular silver nanoplates (TAg-NPs). The TAg-NPs could be used as chiral colorimetric probes for d - and l -forms of phe. Upon addition of d -phe to TAg-NPs solution, a color change from blue to purple to pink could be observed, while no obvious color change was found on addition of l -phe. l -phe could prevent the TAg-NPs from being etched to small size particles while the protective effect of d -phe was weak. Moreover, the enantiomeric excess of d -phe could be determined using the proposed chiral assay in the percentage of l -phe from 0 to 100% with a correlation coefficient of 0.9855. The phenomenon could be monitored by bare eyes and quantified analysis by UV–Vis spectrophotometry. The developed approach had several advantages, such as simplicity, visualization, short analysis time and low cost. This study presented a fast visualization analysis method of chiral d / l -phenylalanine and may lay the foundation for the development of visualization chiral recognition of other target analytes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yu-Xuan Xiao,Jie Ying,Ge Tian,Yong Tao,Hao Wei,Si-Yu Fan,Ze-Hao Sun,Wan-Juan Zou,Jie Hu,Gang-Gang Chang,Weihua Li,Xiao-Yu Yang,Christoph Janiak
The strong Pt-carbon interaction is a very promising way to high-performance design of electrocatalysts. However, the heavy d-π overlap, a high strength of Pt-C bonding, in sp 2 bonded graphitic carbons with low level of defects is rarely reported. Herein, PtPd nanoparticles and graphitic carbon nanofibers (PtPd/CNF) have been integrated via heavy d-π overlap by an interfacial wettability approach and their formation mechanism has also been fully elucidated. The features of strong d-π overlap and high dispersion of metals offer PtPd/CNF with enhanced ORR activity (5.8 folds of specific activity than commercial Pt/C), and excellent structural stability and electrocatalytic durability. A new “heavy d-π overlap” concept, characteristics, and mechanism are proposed at an atomic-/nanoscale to clarify the generation of the predictive interaction as well as the interface charge transfer. It is believed that the study on heavy d-π overlap sheds new light on the fundamental aspects of the nature of Pt-C interaction.
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JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 44
·20641-20653
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IF 4.682
Ren Meiqi,Dong Xiaoli,Wang Yu,Zheng Nan,Ma Hongchao,Zhang Xiufang
Conjugated microporous polymers have attracted significant attention in recent years due to their high porosity, broad functionality and excellent chemical stability. In this work, the small-sized layered structure of poly(phenylenethiazolo[5,4-d]thiazole) (p-PhTT) copolymer was achieved by a facile solvothermal-assisted exfoliation process in a polar organic solvent. Owing to the shorter diffusion length, the layered structure could enhance carrier diffusion from the interior to the surface, as well as provide more active sites in photocatalytic reaction. The obtained exfoliated p-PhTT copolymers show good dispersion and stability in aqueous solution and exhibit efficiently photocatalytic activity for degrading rhodamine B dye under visible-light irradiation. This effective method offers a promising strategy for exfoliating other organic porous polymers. Graphical Abstract
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY
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2022
·Vol. 88
·期 9
·
IF 5.005
Dong-Xu Jia,Fan Wang,Rui Zhao,Bo-Di Gu,Chen Peng,Li-Qun Jin,Zhi-Qiang Liu,Yu-Guo Zheng
d-Alanine belongs to nonessential amino acids that have diverse applications in the fields of food and health care. (R)-transaminase [(R)-TA]-catalyzed asymmetric amination of pyruvate is a feasible alternative for the synthesis of d-alanine, but low catalytic efficiency and thermostability limit enzymatic utilization. In this work, several potential (R)-TAs were discovered using NCBI database mining synchronously with enzymatic structure-function analysis, among which Capronia epimyces TA (CeTA) showed the highest activity for amination of pyruvate using (R)-α-methylbenzylamine as the donor. Furthermore, enzymatic residues surrounding a large catalysis pocket were subjected to saturation and combinatorial mutagenesis, and positive mutant F113T showed dramatic improvement in activity and thermostability. Molecular modeling indicated that the substitution of phenylalanine with threonine afforded alleviation of steric hindrance in the pocket and induced formation of additional hydrogen bonds with neighboring residues. Finally, using recombinant cells containing F113T as a biocatalyst, the conversion yield of amination of 100 mM pyruvate to d-alanine achieved up to 95.2%, which seemed to be the highest level in the literature regarding synthesis of d-alanine using TAs. The inherent characteristics rendered CeTA F113T a promising platform for efficient preparation of d-alanine operating with high productivity.IMPORTANCE d-Alanine is an important compound with many valuable applications. Its asymmetric synthesis employing (R)-ω-TA is considered an attractive choice. According to the stereoselectivity, ω-TAs have either (R)- or (S)-enantiopreference. There has been a variety of literature regarding screening, characterizing, and molecular modification of (S)-ω-TAs; in contrast, the research about (R)-ω-TA has lagged behind. In this work, we identify several (R)-ω-TAs and succeeded in creating mutant F113T, which showed not only better efficiency toward pyruvate but also higher thermostability compared with the original enzyme. The obtained original enzymes and positive mutants displayed important application value for pushing symmetric synthesis of d-alanine to a higher level.
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ACS Applied Electronic Materials
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2022
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IF 4.494
Zhang Chen,Xiaotian Sun,Zizheng Wang,Yong Zhu,Chuanxiang Cao,Jiadong Zhou,Yanfeng Gao
Porous carbon was fabricated for broadband microwave absorption application, which was obtained from facile KOH activated carbon microspheres prepared from hydrothermal d-fructose. It is found that micropores (diameter < 2 nm) in the porous carbon played an important role in broadband and high microwave absorption properties. The prepared samples can achieve a wide bandwidth (the widest is 7.9 GHz, from 10.1 to 18 GHz), high dielectric loss (−60.0 dB as the best), and low thickness sensitivity (the bandwidth maintains 70% of the maximum within a film thickness fluctuation of up to 1.02 mm). Our findings offered an invaluable insight into designing and synthesizing highly microwave-absorbing materials through the micro/nanostructure.
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2021
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IF 3.575
Yongxin Li,Hua Huang,Xinshuai Zhang
1-Deoxy-D-sorbitol, the 1-deoxy analogue of D-sorbitol, has been detected in human urine as well as in natural herbs and spices. Although there are sporadic reports about 1-deoxy-D-sorbitol dehydrogenase, the complete catabolic pathway of 1-deoxy-D-sorbitol remains unsolved. Informed by the promiscuous activities of fructose-6-phosphate aldolase (FSA) which is involved in the sorbitol (glucitol) utilization ( gut ) operon and guided by the large scale bioinformatics analysis, we predicted and then experimentally verified the gut operon encoded by Bacillus licheniformis ATCC14580 is responsible for the catabolism of both D-sorbitol and 1-deoxy-D-sorbitol by in vitro activity assays of pathway enzymes , in vivo growth phenotypes, and transcriptomic studies. Moreover, the phylogenetic distribution analysis suggests that the D-sorbitol and 1-deoxy-D-sorbitol catabolic gene cluster is mostly conserved in members of Firmicutes phylum.
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