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SOLID STATE SCIENCES · 2025 · IF 3.3

Synthesis and pressure-induced structural phase transition of energetic molecular perovskite DAI-1

Tingting Yan,Han Li,Dongyang Xi,Linan Liu,Dinghan Jin,Lei Sun

We synthesized the energetic molecular perovskite DAI-1 (C 48 H 112 I 24 N 16 Na 8 O 96 ) and investigated its behavior under high pressure using high-pressure Raman spectroscopy. DAI-1 exhibits an ABX 3 cubic perovskite structure, with significant changes in its Raman spectrum occurring between 4.3 and 7.1 GPa, signaling a phase transition. Releasing the pressure after applying it up to 12.3 GPa showed that the Raman spectrum did not return to its original state, indicating an irreversible phase transition. Furthermore, we conducted simulations to analyze the trend of changes in the crystal structure under pressure. This study serves as a reference for in-depth research on the high-pressure behavior of DAI-1 and other related substances.

CAS / MDL: 10450-60-9 7790-28-5
研究领域: 材料科学 · 物理学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2024 · IF 3.8

Improved Catalytic Performance on Post-Treated Zeolites SAPO-18 for 1-Butene Cracking

Tingting Lu,Yufei Sun,Zhiwei Wang,Shuo Zhang,Yongsheng Yang,Hongdan Zhang,Peng Cheng,Zhen Zhao

A facile and effective post-treatment route has been systematically applied for the preparation of hierarchical zeolites SAPO-18 using oxalic acid or sodium citrate etching solution. The influence of acidic or alkaline post-treatment on the relative crystallinity, morphology, chemical composition, pore characteristics, and acidity of a series of zeolites SAPO-18 was investigated by X-ray diffraction, scanning and transmission electron microscopy, X-ray fluorescence spectroscopy, nitrogen adsorption–desorption, temperature-programmed desorption of ammonia, and solid-state magic angle spinning nuclear magnetic resonance spectroscopy experiments. Post-treatment led to an increase in mesoporosity by widening the micropores, but a decrease in the acid strength of zeolite SAPO-18 samples. The effects of mesoporosity and acidity on the catalytic cracking performance of zeolite SAPO-18 samples were studied. The hierarchical zeolite SAPO-18 sample post-treated by alkaline sodium citrate solution with suitable concentration exhibited better catalytic conversion and improved light olefin selectivity in cracking of 1-butene.

CAS / MDL: 7087-68-5
研究领域: 材料科学 · 催化化学
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PHYSICS LETTERS A · 2024 · IF 2.3

High-pressure behavior of hydrogen-bonded polymorphic material 1-methylhydantoin Form-I

Ting-ting Yan,Ran Jiang,Dong-yang Xi,Long Ma,Dan-dan Zhang,Yi-fei Xu

This study investigated the structural stability of 1-methylhydantoin (1-MH, C 4 H 6 N 2 O 2 ) Form-I at room temperature using Raman spectroscopy and a diamond anvil cell (DAC) for high-pressure experiments. Two phase transitions were identified at pressures of 0.6–1.7 GPa and 3.4–6.7 GPa. After complete release of pressure, the spectrum aligned with the Raman spectrum at ambient pressure, indicating reversibility of the phase transition. Analysis of Hirshfeld surface energy and fingerprints was conducted to assess changes in intermolecular interactions, revealing that the phase transitions are associated with rearrangements in the hydrogen-bonded network.

研究领域: 物理化学 · 材料科学
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BIOSCIENCE REPORTS · 2018 ·Vol. 38 ·期 2 · IF 2.899

Thermokinetic profile of NDM-1 and its inhibition by small carboxylic acids

Wang Qian,He Yuan,Lu Rui,Wang Wen-Ming,Yang Ke-Wu,Fan Hai Ming,Jin Yi,Blackburn G. Michael

The New Delhi metallo-β-lactamase (NDM-1) is an important clinical target for antimicrobial research, but there are insufficient clinically useful inhibitors and the details of NDM-1 enzyme catalysis remain unclear. The aim of this work is to provide a thermodynamic profile of NDM-1 catalysed hydrolysis of β-lactams using an isothermal titration calorimetry (ITC) approach and to apply this new method to the identification of new low-molecular-weight dicarboxylic acid inhibitors. The results reveal that hydrolysis of penicillin G and imipenem by NDM-1 share the same thermodynamic features with a significant intrinsic enthalpy change and the release of one proton into solution, while NDM-1 hydrolysis of cefazolin exhibits a different mechanism with a smaller enthalpy change and the release of two protons. The inhibitory constants of four carboxylic acids are found to be in the micromolar range. The compounds pyridine-2,6-dicarboxylic acid and thiazolidine-2,4-dicarboxylic acid show the best inhibitory potency and are confirmed to inhibit NDM-1 using a clinical strain of Escherichia coli. The pyridine compound is further shown to restore the susceptibility of this E. coli strain to imipenem, at an inhibitor concentration of 400 μM, while the thiazoline compound also shows a synergistic effect with imipenem. These results provide valuable information to enrich current understanding on the catalytic mechanism of NDM-1 and to aid the future optimisation of β-lactamase inhibitors based on these scaffolds to tackle the problem of antibiotic resistance.

CAS / MDL: 30675-13-9
研究领域: 微生物学 · 药理学 · 生物化学
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Cell Metabolism · 2025 · IF 30.9

Macrophage PD-1 regulates energy expenditure and metabolic dysfunction under immune checkpoint blockade

Ming-Ming Wu,Yan-Chao Yang,Zhi-Qiang Hu,Jie-Yu Chang,Han Xiao,Chang Miao,Bo-Wen Zhang,Zhi-Xi He,Di Zhu,Yu-Ran Duan,Shuo Wang,Jian-Yu Liu,Zhan-Peng Guo,Yu Sun,Dan-Yang Liu,Miao Yu,Yue Zhang,Jian-Jun Mao,Shuai Jiang,Bing-Kun Zhang,Zhu Mei,Jun Gao,Chen Liang,Qiu-Shi Wang,Chang-Jiang Yu,Dan Zhao,Cheng-Hui Yan,Yue Li,Zhen-Wei Pan,Zheng Chen,Da-Qian Xu,Tong Liu,Yong Ji,Zhi-Ren Zhang

Immune checkpoint inhibitor (ICI) therapies increase the risk of metabolic syndrome; the underlying mechanisms remain elusive. We show that an anti-PD-1 antibody targets macrophage PD-1 to reduce energy expenditure without affecting food intake, augmenting the susceptibility of mice to high-fat diet (HFD)-induced obesity and systemic metabolic disorders. Mechanistically, lipopolysaccharide (LPS) activates Unc-51-like autophagy activating kinase 1 (ULK1) in a mammalian target of rapamycin (mTOR)-dependent manner. Activated ULK1 phosphorylates PD-1 at Thr250 to inhibit FBXO38-mediated PD-1 ubiquitination and degradation by disrupting FBXO38-PD-1 binding. Phosphorylated PD-1 interacts with inositol-requiring enzyme 1α (IRE1α) and attenuates IRE1α autophosphorylation to suppress endoplasmic reticulum (ER) stress-mediated inflammatory responses. Suppressing IRE1α alleviates HFD-induced metabolic disorders in macrophage-specific PD-1 knockout mice by rescuing the reduced energy expenditure. Our findings highlight the critical role of macrophage PD-1 at the intersection of immune checkpoint blockade, energy expenditure, and metabolic dysfunction. The underscored moonlighting function of macrophage PD-1 may provide a new rationale for combating ICI therapy- and HFD-induced metabolic diseases.

CAS / MDL: 30525-89-4
研究领域: 免疫学 · 代谢学 · 细胞生物学 · 分子生物学 · 肥胖研究
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JOURNAL OF CONTROLLED RELEASE · 2024 · IF 10.5

Functionalized aluminum hydroxide-based self-adjuvanted nanovaccine orchestrates antitumor immune responses via Dectin-1 signaling

Xiaoli Ling,Zhipeng Tian,Dong Chen,Yujia Zhang,Ziyan Dong,Dan He,Jiayu Li,Zhidi He,Jiaxin Li,Fang Chen,Qin He,Man Li

Self-adjuvanted vaccine delivery platforms possess potential for targeted delivery of antigens and initiation of potent immune responses. Although aluminum-containing adjuvants have been approved and widely used in human vaccines, their effectiveness in inducing Th1-type immune responses is far from satisfactory. To facilitate antigen delivery and activate potent antitumor immune responses, a self-adjuvanted nanovaccine (CPBG-Al@OVA) is constructed by functionalizing aluminum hydroxide with β-1,3-glucan, which recognizes pattern recognition receptors via Dectin-1. Carboxymethyl-phosphorylated β-1,3-glucan (CPBG) has been synthesized and optimized to achieve superior adjuvanticity while maintaining water solubility. CPBG then self-assembles with aluminum hydroxide and the targeted antigen, leading to the formation of a nanovaccine CPBG-Al@OVA. Owing to the favorable nanoscale size distribution, CPBG-Al@OVA effectively drains to the lymph nodes and is internalized by antigen-presenting cells (APCs) through Dectin-1-mediated endocytosis, activating the Syk and Raf1 signaling pathways and leading to upregulated TNFSF15 and OX40L expression to activate APCs. Following immunization, CPBG-Al@OVA activates potent CD8 + T cell and humoral responses to inhibit tumor growth. Notably, mice vaccinated with CPBG-Al@OVA showed extended survival, with more than 70 % of the mice surviving for over 50 days post-tumor challenge. Moreover, the CPBG-Al nanoparticle also possesses personalized immune-activating capacity by encapsulating tumor lysate as an antigen, specifically suppressing tumor growth. This strategy synergizes the adjuvant effects of aluminum and β-1,3-glucan, offering a platform for self-adjuvanted nanovaccine design with significant clinical translational potential.

CAS / MDL: 220904-83-6
研究领域: 免疫学 · 癌症研究 · 疫苗学 · 分子生物学
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS · 2020 · IF 3.209

(S)-1-(5-(4-Methylpiperazin-1-yl)-2,4-dinitrophenyl)pyrrolidine-2-carboxylic acid as a derivatization reagent for ultrasensitive detection of amine enantiomers by HPLC-MS/MS and its application to the chiral metabolite analysis of (R)-1-aminoindan in saliva

Youxi Jin,Yu Pan,Biao Jin,Dongri Jin,Chunbo Zhang

(S)-1-(5-(4-Methylpiperazin-1-yl)-2,4-dinitrophenyl)pyrrolidine-2-carboxylic acid (Pro-PPZ) was employed as a chiral derivatization reagent (CDR) for the efficient enantioseparation and ultrasensitive mass spectrometric detection of chiral amines. Pro-PPZ was prepared from the one-step reaction of 1-(5-fluoro-2,4-dinitrophenyl)-4-methylpiperazine (PPZ) and l -proline. Two amines and two amino acid methyl esters were selected as model chiral amines, which were easily labeled with Pro-PPZ under mild reaction conditions (35 °C for 10 min) generating Pro-PPZ-amine derivatives. The resulting diastereomers were completely separated by reversed-phase liquid chromatography (RP-LC) using an ODS column ( R s = 3.4–17.0 for amines). Ultrasensitive detection limits on femtomolar level were obtained for the tested amines using multiple reaction monitoring (MRM) chromatograms at a single monitoring ion, m/z 289 (0.1–5.0 fmol for amines). The practical metabolite analysis of (R)-1-aminoindan (R-AI) in saliva samples was performed by LC–MS/MS using the Pro-PPZ derivatization method. The method was validated in terms of precision, accuracy, and linearity. Using this method, R-AI concentrations in saliva were determined after a single oral administration of the drug rasagiline to healthy male and female subjects, but no (S)-1-aminoindan (S-AI) was detected, which suggesting that R-AI was not converted into S-enantiomer in the metabolic process. R-AI concentrations in four healthy volunteers ranged from 32.85 nM to 49.45 nM, with an average value of 43.76 nM. To date, there is no LC–MS (or MS/MS) method reported for the enantioselective determination of R-AI in human saliva samples.

研究领域: 分析化学 · 药物代谢 · 临床医学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Tunable Chemiluminescence Kinetics with Hierarchically Structured HKUST-1 and Its Sensing Application for Concanavalin A Analysis

Sijie Yuan,Ying Tu,Ru Yu,Fei Nie

Introducing novel catalysts is essential for developing chemiluminescence (CL) systems that exhibit sustained and robust emission. Traditional Luminol-H2O2 systems typically feature flash-type CL emission. In this study, we discovered that the porous material HKUST-1 can induce a long-lasting and intense CL emission when combined with Luminol-H2O2. This long-term emission signal can be directly detected by the smartphone. By changing the calcination temperature, a series of microporous and hierarchically porous HKUST-1 materials were prepared as catalysts to adjust the kinetic characteristics of the CL signal of Luminol-H2O2 system from flash-type to glow-type. A systematic investigation into the influence of the central metal and ligand, aperture, and particle size of HKUST-1 on the CL kinetic properties revealed that the pore structure has the most pronounced impact on the dynamics of the Luminol-H2O2 CL reaction. Capitalizing on the intense emission of the HKUST-1-catalyzed Luminol-H2O2 system, we established a CL sandwich immunoassay strategy for concanavalin A (ConA), demonstrating good linearity and low detection limit. This research presents a significant endeavor in modulating the dynamics of CL signal emissions.

研究领域: 分析化学 · 生物传感 · 材料科学
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JOURNAL OF MOLECULAR LIQUIDS · 2024 · IF 5.3

Experimental and simulation study on the solubility of 1-naphthylamine in twelve neat solvents

Bolun Mei,Yueru Wang,Jianhua Zhou,Xingchuan Yang,Yi Yu,Li Xu,Guoji Liu

To meet the demand of separating and purifying 1-naphthylamine from the reaction production and filling the solubility data gap, the solubility of 1-naphthylamine in twelve pure solvents (acetone, acetonitrile, ethyl acetate, n-butyl acetate, cyclohexane, n-heptane, methanol, ethanol, n-propanol, iso-propanol, n-butanol, and iso-butanol) was experimentally investigated in the range from 273.15 K to 308.15 K. It was found that the solubility of 1-naphthylamine increases markedly with increasing temperature in all solvent systems. The maximum solubility was 0.8978 (in the solvent of acetone, T  = 308.15 K) and the minimum solubility was 0.005485 (in the solvent of n-heptane, T  = 273.15 K). Then the experimental solubility data was correlated by the modified Apelblat model, Van't Hoff model, NRTL model, Wilson model, and Margules model. ARD% was calculated to assess the accuracy of the five equations and the results indicated that the modified Apelblat model fits optimally with an average ARD% value of 1.62 %. The effects of various physicochemical properties such as solvent polarity, hydrogen bond donor, hydrogen bond acceptor, and cohesive energy density on solute dissolution behavior were explored. In addition, the apparent thermodynamic properties of 1-naphthylamine in different solvents were analyzed based on modified Van’t Hoff model, which indicated the dissolution process of 1-naphthylamine in selected solvents is endothermic and entropy-driving. Finally, the effect of intermolecular interactions on the dissolution behavior was investigated at the molecular scale through molecular dynamics simulation studies, including molecular electrostatic potential surface, solvation free energy and radial distribution function analysis. This work will provide a fundamental guidance for the crystallization, separation, and purification of 1-naphthylamine.

CAS / MDL: 134-32-7
研究领域: 化学工程 · 物理化学
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JOURNAL OF CHEMICAL THERMODYNAMICS · 2015 · IF 2.679

(Liquid + liquid) equilibria for (water + 1-propanol or acetone + β-citronellol) at different temperatures

Hengde Li,Yongtao Han,Cheng Huang,Chufen Yang

On this paper, experimental (liquid   +   liquid) equilibrium (LLE) results are presented for systems composed of β-citronellol and aqueous 1-propanol or acetone. To evaluate the phase separation properties of β-citronellol in aqueous mixtures, LLE values for the ternary systems (water   +   1-propanol   +   β-citronellol) and (water   +   acetone   +   β-citronellol) were determined with a tie-line method at T   =   (283.15, 298.15, and 313.15   ±   0.02)   K and atmospheric pressure. The reliability of the experimental tie-lines was verified by the Hand and Bachman equations. Ternary phase diagrams, distribution ratios of 1-propanol and acetone in the mixtures are shown. The effect of the temperature on the ternary (liquid   +   liquid) equilibria was examined and discussed. The experimental LLE values were satisfactorily correlated by extended UNIQUAC and modified UNIQUAC models.

研究领域: 化学工程 · 热力学
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Sensing and Bio-Sensing Research · 2024 · IF 5.4

Electrochemiluminescence ratio sensor for detecting MCP-1 based on s-PdNS

Weiran Mao,Xiaoyan Zhang,Yuanyuan Yin,Xiaohua Tang,Qingqing Jiang,Xia Chen,Xiaoliang Chen

This study proposes a novel sandwich-based ratio electrochemiluminescence (ECL) immunosensor for detecting monocyte chemotactic protein-1 (MCP-1), a marker of cardiovascular disease. We synthesized sulfur-doped palladium nanosheets (S-PdNS), which possess a stable structure and uniform morphology, and can quench signals generated by the S 2 O 8 2− /O 2 ECL system. Using glutaraldehyde (GA), we conjugated luminol to these nanosheets and combined them with a secondary antibody. This modification enabled the nanomaterial to produce a new luminol signal as an internal reference for detection while quenching the S 2 O 8 2− /O 2 ECL signal. To date, no studies have utilized both mechanisms for detection. Furthermore, the deposition of gold nanoparticles (AuNPs) on the surface of the glassy carbon electrode (GCE) allowed for increased antibody binding and improved electron transmission in the ECL system. When trace analytes are present, the S 2 O 8 2− /O 2 ECL signal decreases, and the luminol ECL signal increases. This setup allowed us to obtain two signals from one measurement and use the ratio to construct a standard curve, significantly reducing the possibility of misjudgment. Under optimal conditions, the linear detection range for MCP-1 is 10 –2.5 pg mL −1 to 10 3  pg mL −1 , with a detection limit of 1.6 fg mL −1 (S / N  = 3). The immunosensor also exhibited excellent selectivity, repeatability, and stability, expanding the application of the dual luminescence mechanism and providing an effective method for early monitoring of cardiovascular disease.

CAS / MDL: 9048-46-8 521-31-3
研究领域: 生物医学工程 · 分析化学
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RSC Advances · 2017 ·Vol. 7 ·期 65 ·41070-41076 · IF 3.108

A novel cellulose–silicalite-1 membrane with excellent gas separation property

Xin-ling Fu,Ming Zeng,Jian-bo Zhou,Chao Xu

A novel strategy for synthesizing silicalite-1 membrane by hydrothermal synthesis without organic template after coating the support with a mixture of modified cellulose and seeds was successfully proposed. The membrane possesses high ideal separation factors of H2 over various gases which is larger than the corresponding Knudsen diffusion coefficients. The selectivity of AcOH from AcOH/H2O mixtures can reach to 65 and stable for 180 h. The characterization results by XRD and SEM showed that the excellent performance can be attributed to both modified cellulose and the synthesis without organic template. Modified cellulose attracted more silicalite-1 nutrients to the support and assisted the synthesis of more compact silicalite-1 zeolite membrane. Calcination after synthesis was avoided, thus avoiding macrostructure defects appearing during the process of calcination.

CAS / MDL: 9004-34-6 4499-86-9
研究领域: 材料科学 · 化学工程
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