ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaoyu Hu,Fengyun Ding,Renjin Xiong,Yongtao An,Xingwen Feng,Jiangfeng Song,Linsen Zhou,Peilong Li,Changlun Chen
Realizing ideal deuterium separation from isotopic mixtures remains a daunting challenge because of their almost identical sizes, shapes, and physicochemical properties. Using the quantum sieving effect in porous materials with suitable pore size and open metal sites (OMSs) enables efficient hydrogen isotope separation. Herein, synthetic HKUST-1-derived microporous mixed-valence Cu(I)Cu(II)-BTC (BTC = benzene-1,3,5-tricarboxylate), featuring a unique network of distinct Cu(I) and Cu(II) coordination sites, can remarkably boost the D2/H2 isotope separation, which has a high selectivity (SD2/H2) of 37.9 at 30 K, in comparison with HKUST-1 and other porous materials. Density functional theory (DFT) calculations indicate that the introduction of Cu(I) macrocycles in the framework decreases the pore size and further leads to relatively enhanced interaction of H2/D2 molecules on Cu(II) sites. The significantly enhanced selectivity of Cu(I)Cu(II)-BTC at 30 K can be mainly attributed to the synergistic effect of kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS). The results reveal that Cu(I) OMSs exhibit counterintuitive behaviors and play a crucial role in tuning quantum sieving without a complex structural design, which provides a deeper insight into quantum sieving mechanisms and a new strategy for the intelligent design of highly efficient isotope systems.
研究领域:
材料科学
·
物理化学
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DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2015
·
IF 12.113
Xiao-Li Pei,Yang Yang,Zhen Lei,Shan-Shan Chang,Zong-Jie Guan,Xian-Kai Wan,Ting-Bin Wen,Quan-Ming Wang
The activation of C(sp3)–H bonds is challenging, due to their high bond dissociation energy, low proton acidity, and highly nonpolar character. Herein we report a unique gold(I)–silver(I) oxo cluster protected by hemilabile phosphine ligands [OAu3Ag3(PPhpy2)3](BF4)4 (1), which can activate C(sp3)–H bonds under mild conditions for a broad scope of methyl ketones (RCOCH3, R = methyl, phenyl, 2-methylphenyl, 2-aminophenyl, 2-hydroxylphenyl, 2-pyridyl, 2-thiazolyl, tert-butyl, ethyl, isopropyl). Activation happens via triple deprotonation of the methyl group, leading to formation of heterometallic Au(I)–Ag(I) clusters with formula RCOCAu4Ag4(PPhpy2)4(BF4)5 (PPhpy2 = bis(2-pyridyl)phenylphosphine). Cluster 1 can be generated in situ via the reaction of [OAu3Ag(PPhpy2)3](BF4)2 with 2 equiv of AgBF4. The oxo ion and the metal centers are found to be essential in the cleavage of sp3 C–H bonds of methyl ketones. Interestingly, cluster 1 selectively activates the C–H bonds in −CH3 rather than the N–H bonds in −NH2 or the O–H bond in −OH which is traditionally thought to be more reactive than C–H bonds. Control experiments with butanone, 3-methylbutanone, and cyclopentanone as substrates show that the auration of the C–H bond of the terminal methyl group is preferred over secondary or tertiary sp3 C–H bonds; in other words, the C–H bond activation is influenced by steric effect. This work highlights the powerful reactivity of metal clusters toward C–H activation and sheds new light on gold(I)-mediated catalysis.
研究领域:
无机化学
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有机金属化学
·
催化
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DOI
PubMed
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2016
·
IF 2.653
Yong Hu,Hai-Long Wu,Xiao-Li Yin,Hui-Wen Gu,Rong Xiao,Li Wang,Huan Fang,Ru-Qin Yu
A rapid interference-free spectrofluorometric method combined with the excitation-emission matrix fluorescence and the second-order calibration methods based on the alternating penalty trilinear decomposition (APTLD) and the self-weighted alternating trilinear decomposition (SWATLD) algorithms, was proposed for the simultaneous determination of nephrotoxic aristolochic acid I (AA-I) and aristololactam I (AL-I) in five Chinese herbal medicines. The method was based on a chemical derivatization that converts the non-fluorescent AA-I to high-fluorescent AL-I, achieving a high sensitive and simultaneous quantification of the analytes. The variables of the derivatization reaction that conducted by using zinc powder in acetose methanol aqueous solution, were studied and optimized for best quantification results of AA-I and AL-I. The satisfactory results of AA-I and AL-I for the spiked recovery assay were achieved with average recoveries in the range of 100.4–103.8% and RMSEPs < 0.78 ng mL − 1 , which validate the accuracy and reliability of the proposed method. The contents of AA-I and AL-I in five herbal medicines obtained from the proposed method were also in good accordance with those of the validated LC-MS/MS method. In light of high sensitive fluorescence detection, the limits of detection (LODs) of AA-I and AL-I for the proposed method compare favorably with that of the LC-MS/MS method, with the LODs < 0.35 and 0.29 ng mL − 1 , respectively. The proposed strategy based on the APTLD and SWATLD algorithms by virtue of the “second-order advantage”, can be considered as an attractive and green alternative for the quantification of AA-I and AL-I in complex herbal medicine matrices without any prior separations and clear-up processes.
研究领域:
中药学
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分析化学
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毒理学
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DOI
PubMed
高影响因子
NATURE CELL BIOLOGY
·
2025
·
IF 19.1
Wang Bin,Wang Yongqiang,Pan Ting,Zhou Lili,Ran Yu,Zou Jing,Yan Xiaohua,Wen Zhenke,Lin Shixian,Ren Aiming,Wang Fangwei,Liu Zhuang,Liu Ting,Lu Huasong,Yang Bing,Zhou Fangfang,Zhang Long
Maintaining innate immune homeostasis is critical for preventing infections and autoimmune diseases but effective interventions are lacking. Here we identified C864–C869-mediated intermolecular disulfide-linkage formation as a critical step for human RIG-I activation that can be bidirectionally regulated to control innate immune homeostasis. The viral-stimulated C864–C869 disulfide linkage mediates conjugation of an SDS-resistant RIG-I oligomer, which prevents RIG-I degradation by E3 ubiquitin-ligase MIB2 and is necessary for RIG-I to perform liquid–liquid phase separation to compartmentalize downstream signalsome, thereby stimulating type I interferon signalling. The corresponding C865S ‘knock-in’ caused an oligomerization defect and liquid–liquid phase separation in mouse RIG-I, which inhibited innate immunity, resulting in increased viral load and mortality in mice. Using unnatural amino acids to generate covalent C864–C869 linkage and the development of an interfering peptide to block C864–C869 residues, we bidirectionally regulated RIG-I activities in human diseases. These findings provide in-depth insights on mechanism of RIG-I activation, allowing for the development of methodologies that hold promising implications in clinics.
研究领域:
免疫学
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分子生物学
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病毒学
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产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 8
·1721
·
IF 4.2
Shoudong Wang,Lei Zhou,Hongyun Qin,Zixu Dong,Haoyuan Li,Bo Liu,Zhilu Wang,Lina Zhang,Qiang Fu,Xia Chen
Hydrofluorocarbons (HFCs) have important applications in different industries; however, they are environmentally unfriendly due to their high global warming potential (GWP). Hence, reclamation of used hydrofluorocarbons via energy-efficient adsorption-based separation will greatly contribute to reducing their impact on the environment. In particular, the separation of azeotropic refrigerants remains challenging, such as typical mixtures of CH2F2(HFC-23) and CHF3(HFC-32), due to a lack of adsorptive mechanisms. Metal–organic frameworks (MOFs) can provide a promising solution for the separation of CHF3–CH2F2mixtures. In this study, the adsorption mechanism of CHF3–CH2F2mixtures in TIFSIX-2-Cu-i was revealed at the microscopic level by combining static pure-component adsorption experiments, molecular simulations, and density-functional theory (DFT) calculations. The adsorption separation selectivity of CH2F2/CHF3in TIFSIX-2-Cu-i is 3.17 at 3 bar under 308 K. The existence of similar TiF62−binding sites for CH2F2or CHF3was revealed in TIFSIX-2-Cu-i. Interactions between the fluorine atom of the framework and the hydrogen atom of the guest molecule were found to be responsible for determining the high adsorption separation selectivity of CH2F2/CHF3. This exploration is important for the design of highly selective adsorbents for the separation of azeotropic refrigerants.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
TALANTA
·
2025
·
IF 6.1
Yafang Shen,Xingyue Tang,Jiangqi Wang,Huang Dai,Yanna Cui,Qiuyue Hu,Yuxin Wu,Fei Jia,Guijie Hao
Recent years have witnessed the flourishing of CRISPR/Cas-based biosensors in various fields. However, most of them were developed for nucleic acid detection because non-nucleic acid targets are unable to unleash the cleavage activity of the CRISPR/Cas system directly. To circumvent this problem, activator DNA and deoxyribonuclease I (DNase I) were introduced in this research to render the CRISPR/Cas12a system as a new powerful tool for the detection of enrofloxacin (ENR), a common veterinary drug. In this biosensor, target ENR competed with DNase I- and bovine serum albumin-ENR composite-modified gold nanoparticles (DNase I-AuNPs-BSA-ENR) for the binding sites on the surface of antibody-modified magnetic nanoparticles (immuno-MNPs). Then, the captured DNase I-AuNPs-BSA-ENR degraded the activator DNA in the solution, which inhibited the activation of the CRISPR/Cas12a system. Finally, the fluorescence released by the activated CRISPR/Cas12a system was measured for the quantitative detection of ENR. The ingenious use of activator DNA and DNase I helped transduce the target recognition event into the cleavage activity of the CRISPR/Cas12a system. Moreover, the dual enzymatic amplification from DNase I and the CRISPR/Cas12a system guaranteed the sensitivity of this method with a low detection limit of 0.04 ng/mL. The developed biosensor extended the application of the CRISPR/Cas12a system for the sensitive detection of non-nucleic acid targets, providing a powerful tool in various fields such as environmental monitoring, food safety and clinical diagnosis.
研究领域:
生物技术
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食品安全
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环境监测
·
临床诊断
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产品关联
DOI
PubMed
高影响因子
PHYTOMEDICINE
·
2021
·
IF 5.34
Yajie Cai,Bing Xu,Fei Zhou,Jianzhi Wu,Shuo Li,Qi Zheng,Yajing Li,Xiaojiaoyang Li,Feng Gao,Shifen Dong,Runping Liu
Background Ulcerative colitis (UC) is a chronic relapsing inflammatory disease that markedly elevates the risk of colon cancers and results in disability. The disrupted immune homeostasis has been recognized as a predominant player in the pathogenesis of UC. However, the overall remission rate of current therapies based on immunoregulation is still unsatisfactory. Si-Ni-San (SNS) has been found effective in relieving UC through thousands of years of clinical practice, yet the specific mechanisms of the protective effect of SNS were not fully elucidated. Purpose We aim to investigate the therapeutic effects of SNS against the development of chronic colitis and the underlying mechanisms. Methods We established a DSS-induced chronic experimental colitis mouse model to evaluate the effect of SNS. RNA-sequencing, bioinformatic analysis, and in vitro studies were performed to investigate the underlying mechanisms. Results Our data demonstrated that SNS significantly ameliorated chronic experimental colitis via inhibiting the expression of genes associated with inflammatory responses. Interestingly, SNS significantly suppressed DSS-induced type I interferon (IFN) responses instead of directly downregulating the production of pro-inflammatory cytokines, such as Il-6. In vitro study further found that SNS selectively inhibited STING and RIG-I pathway-induced type I IFN responses by modulating TBK1- and IRF3-dependent signaling transduction. SNS also suppressed the expression of IFN-stimulated genes by directly inhibiting STAT1 and STAT2 activation. Conclusion Our study not only provides novel insights into the pathogenic role of type I IFN responses in colitis but also suggested that SNS or bioactive compounds derived from SNS may serve as novel therapeutic strategies for the treatment of UC via interfering type I IFN-mediated inflammation.
研究领域:
药理学
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免疫学
·
胃肠病学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Meng-yuan Zhang,Jun Cai
Red dragon fruit peel is a pectin-rich fruit waste that is a potential source of prebiotics and whose different sources and structures will influence its prebiotic function. Thus, we compared the effects of three extraction methods on the structure and prebiotic function of red dragon fruit pectin, the results showed that the citric acid extracted pectin produced a high Rhamnogalacturonan-I (RG-I) region (66.59 mol%) and more side-chains of Rhamnogalacturonan-I ((Ara + Gal)/Rha = 1.25), which can promote bacterial proliferation significantly. The side-chains of Rhamnogalacturonan-I may be an important factor in that pectin can promote the proliferation of B. animalis. Our results provide a theoretical basis for the prebiotic application of red dragon fruit peel.
研究领域:
食品科学
·
微生物学
·
营养学
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产品关联
DOI
PubMed
高影响因子
PeerJ
·
2019
·
IF 2.353
Weilong Zhang,Yang Wu,Jin Wang,Juan Liu,Haifeng Lu,Shuijing Zhai,Qiaohui Zhong,Siyu Liu,Wanying Zhong,Chunling Huang,Xiaoxiang Yu,Wenhui Zhang,Yongheng Chen
Rutile nano-titanium dioxide (RNTD) characterized by loose particles with diameter in 20–50 nm has a very large surface area for adsorption of Tl, a typical trace metal that has severe toxicity. The increasing application of RNTD and widespread discharge of Tl-bearing effluents from various industrial activities would increase the risk of their co-exposure in aquatic environments. The adsorption behavior of Tl(I) (a prevalent form of Tl in nature) on RNTD was studied as a function of solution pH, temperature, and ion strength. Adsorption isotherms, kinetics, and thermodynamics for Tl(I) were also investigated. The adsorption of Tl(I) on RNTD started at very low pH values and increased abruptly, then maintained at high level with increasing pH >9. Uptake of Tl(I) was very fast on RNTD in the first 15 min then slowed down. The adsorption of Tl(I) on RNTD was an exothermic process; and the adsorption isotherm of Tl(I) followed the Langmuir model, with the maximum adsorption amount of 51.2 mg/g at room temperature. The kinetics of Tl adsorption can be described by a pseudo-second-order equation. FT-IR spectroscopy revealed that -OH and -TiOO-H play an important role in the adsorption. All these results indicate that RNTD has a fast adsorption rate and excellent adsorption amount for Tl(I), which can thus alter the transport, bioavailability and fate of Tl(I) in aqueous environment.
研究领域:
环境科学
·
化学
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DOI
PubMed
高影响因子
NUCLEAR TECHNOLOGY
·
2022
·
IF 1.667
Yanhui Wang,Qiao Jiang,Yexin Yang,Jianfeng Cheng,Chenyang Bao,Yuelong Pan,Yu Liu,Gang Yang,Yangchun Leng,Xianguo Tuo
The alteration of the morphology of bentonite, a key barrier to isolating high-level radioactive waste in deep geological repositories under long-term interaction with groundwater, was studied. Bentonite colloids were prepared from Gaomiaozi bentonite, and its various properties were analyzed by various characterization methods. The effects of various factors on the adsorption of Cs(I) and Co(II) on bentonite colloids were investigated by batch static adsorption experiments. The results showed that the colloids were mainly composed of montmorillonite and were lamellar in shape, with a zeta potential of −enton mV and an average size of approximately 209.10 nm. The adsorption of Cs(I) and Co(II) by the colloids was a rapid process, and 31.78 and 88.24 mg/g, respectively, were adsorbed at equilibrium. Pseudo-second-order kinetic fitting showed that chemisorption plays a dominant role and acid-base interactions affect adsorption by influencing the stability of colloids and the chemical form of simulated nuclides. This work can be helpful for evaluating the safety of waste repositories.
研究领域:
环境科学
·
放射性废物管理
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产品关联
DOI
高影响因子
AUSTRALIAN JOURNAL OF CHEMISTRY
·
2022
·Vol. 75
·期 5
·345-352
·
IF 1.224
Yuzheng Shi,Xicheng Xie,Lumei Wang,Linzheng Wang,Lingyun Li,Zhiyu Yan,Guoqing Shen,Yuzheng Shi,Xicheng Xie,Lumei Wang,Linzheng Wang,Lingyun Li,Zhiyu Yan,Guoqing Shen
This paper describes a fluorometric assay for the determination of carbendazim (CBZ) in aqueous samples based on an unmodified CBZ-specific aptamer and the fluorescent intercalator SYBR Green I (SG-I). The CBZ aptamer has double-stranded parts and G-quadruplex spatial structures, which can be recognized by SG-I. It leads to strong fluorescent emission of SG-I. In the presence of CBZ, the aptamer will bind to CBZ to form stable compounds due to its specific affinity. This will induce the conformational change of the aptamer. SG-I will then detach from the aptamer, leading to the decrease of its fluorescence. Therefore, the concentration of CBZ is determined through the changes in fluorescence of the system. This fluorometric biosensor for CBZ detection is constructed with a linear range from 3.58 to 230 nM with a limit of detection (LOD) of 3.58 nM. With great sensitivity and selectivity, this assay is efficient and convenient with a < 40 min operation time. Meanwhile, the average recovery of CBZ is 99.87–101.77% in the application of actual water samples with relative standard deviations (RSD) ranging from 1.97 to 2.63%.
研究领域:
分析化学
·
环境科学
·
生物技术
✓ 已验证
DOI
高影响因子
NANO
·
2017
·
IF 1.025
Xiqing Liu,Xiao Wei,Yeqing Xu,Hongji Li,Kai Lu,Kun Wang,Yongsheng Yan
In this paper, a novel fluorescent nanoswitch based on carbon dots (CDs) was developed for the sensitive and selective determination of Hg 2 + and I − . The CDs were obtained by simple hydrothermal process and had a strong fluorescence emission at 440 nm. The fluorescence of the CDs can be selectively quenched by Hg 2 + ion, and then the I − was added into the system, which can interact with Hg 2 + and recover fluorescence of the CDs. Under optimal conditions, the quenching fluorescence intensity on addition of Hg 2 + has obtained a satisfactory linear relationship covering the linear range of 0–50 μ M with the linear relationship ( R 1 2 = 0 . 9 9 9 1 ), and the limit of detection is 0.047 μ M. The additions of I − could lead to the fluorescence intensity of the solution of CDs and Hg 2 + (50 μ M) recover rapidly, which is linearly related ( R 2 2 = 0 . 9 9 5 7 ) to the concentration of I − in the range from 0 to 70 μ M, the detection limit for I − was calculated to be 0.084 μ M. Moreover, the developed method to detect Hg 2 + and I − was evaluated in real examples, and the fluorescence switching can sensitively and selectively detect Hg 2 + and I − over some potentially interfering ions, the recoveries were up to 97.8–107.0% and 96.7–106.6%, respectively.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
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