npj Science of Food
·
2023
·Vol. 7
·期 1
·1-8
·
IF 6.4
Sun Yu-Long,Ge Bing-Qiang,Li Mi-Zhuan,Wang Lei,Chen Zhong-Xiu
Investigation on the physiochemical nature involved in the production of fatty acid catalyzed by the vesicles is of importance to understand the digestion of lipid. In this paper, the effects of crowding degree, which was constructed by polyethylene glycol (PEG), on the autocatalytic production of fatty acid with different chain lengths was studied. The results showed that the higher crowding degree led to the slower production rate of decanoic acid but the faster rate of oleic acid. The reason lies in that the presence of macromolecules resulted in the increased sizes of decanoic acid vesicles, but decreased sizes of oleic acid vesicles. Meanwhile, decanoic acid vesicles in more crowded medium exhibited viscous behavior, whereas oleic acid displayed elastic behavior. This research provides useful information for understanding the unusual autocatalyzed production of fatty acid in macromolecular crowding and may also draw an attention to the physiologically relevant lipid digestion.
研究领域:
生物化学
·
生理学
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DOI
PubMed
高影响因子
eScience
·
2021
·
IF 0
Mengke Peng,Li Wang,Longbin Li,Zhongyou Peng,Xiannong Tang,Ting Hu,Kai Yuan,Yiwang Chen
The development of low-cost and eco-friendly aqueous electrolytes with a wide voltage window is the key to achieving safe high energy density supercapacitors (SCs). In this work, a molecular crowding electrolyte is prepared by simulating the crowded environment in living cells. Ion transport in the molecular crowding electrolyte can be effectively improved via reducing the molecular weight of the crowding agent, polyethylene glycol (PEG). The results show that PEG with a molecular weight of 200 (PEG200) can significantly improve ionic conductivity while maintaining a wide voltage window. These advantages enable commercial activated carbon-based SCs to work at 2.5 V with high energy density, outstanding rate performance and good stability for more than 10,000 cycles. On this basis, three series of molecular crowding electrolytes using sodium perchlorate, lithium perchlorate, and sodium trifluoromethanesulfonate as salts are developed, demonstrating the versatility of PEG200 for wide-voltage aqueous electrolytes.
研究领域:
材料科学
·
能源技术
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DOI
JOURNAL OF PHYSICAL CHEMISTRY B
·
2014
·
IF 3.377
Cao Cao,Qing-Biao Wang,Lin-Jun Tang,Bing-Qiang Ge,Zhong-Xiu Chen,Shao-Ping Deng
Autocatalytic hydrolysis of fatty acid anhydrides induced by the spontaneously formed vesicles has been studied for years. However, whether the reaction autocatalyzed by vesicles formed in diluted solutions applies also to macromolecular crowded conditions remains unknown. The aim of this study is to characterize hydrolysis behavior of fatty acid anhydrides and formation of vesicles in crowded media. Inert macromolecular crowding agents such as polyethylene glycol (PEG) and Dextran were used to probe the impact of external crowding on the autocatalytic hydrolysis of fatty acid anhydrides with varied hydrophobic chain length. Under stringent conditions of crowding, hydrolysis rates of octanoic anhydride, nonanoic anhydride, and decanoic anhydride were found to decrease, but the rates of lauric anhydride and oleic anhydride increased. These results suggest that the effect of the crowding agent on the hydrolysis of fatty acid anhydrides was chain-length-dependent. Characterization of the size and polydispersity of vesicles formed from hydrolyzed fatty acid anhydrides in crowding revealed that long-chain fatty acids formed monodisperse vesicles easier at lower concentrations of PEG. Measurement of the critical aggregation concentration of ionized fatty acid in the presence of PEG showed that crowding media promoted vesicle formation from long-chain fatty acids but inhibited those from fatty acids with fewer carbon atoms. Further investigation of the diffusion property of ionized fatty acids in crowding agents suggested that PEG might create more hydrophobic areas for long-chain fatty acids anhydrides, which subsequently promoted the unreacted anhydride in the aqueous phase to be solubilized in the formed vesicles. This research provides information for understanding the autocatalytic reaction accompanied by self-producing aggregates and the behavior of fatty acids in crowding media.
研究领域:
生物化学
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分子生物学
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DOI
PubMed
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2017
·Vol. 410
·期 2
·595-604
·
IF 3.431
Jia Man,Yang Jian,Sun Ya Kun,Bai Xi,Wu Tao,Liu Zhao Sheng,Aisa Haji Akber
We aimed to improve the imprinting effect of ionic liquid molecularly imprinted polymers (MIPs) by use of a molecular crowding agent. The ionic liquid 1-vinyl-3-ethylimidazolium tetrafluoroborate ([VEIm][BF 4 ]) was used as the functional monomer and aesculetin was used as the template molecule in a crowding environment, which was made up of a tetrahydrofuran solution of polystyrene. The ionic liquid MIPs that were prepared in the crowding environment displayed an enhanced imprinting effect. NMR peak shifts of active hydrogen of aesculetin suggested that interaction between the functional monomer and the template could be increased by the use of a crowding agent in the self-assembly process. The retention and selectivity of aesculetin were affected greatly by high molecular crowding, the amount of high molecular weight crowding agent, and the ratio of [VEIm][BF 4 ] to aesculetin. The optimal MIPs were used as solid-phase extraction sorbents to extract aesculetin from Cichorium glandulosum . A calibration curve was obtained with aesculetin concentrations from 0.0005 to 0.05 mg mL −1 (correlation coefficient R
2 of 0.9999, y = 1519 x + 0.0923). The limit of quantification was 0.12 μg mL −1 , and the limit of detection was 0.05 μg mL −1 . The absolute recovery of aesculetin was (80 ± 2)% ( n = 3), and the purity of aesculetin was (92 ± 0.5)% ( n = 5). As a conclusion, molecular crowding is an effective approach to obtain ionic liquid MIPs with high selectivity even in a polar solvent environment.
研究领域:
化学
·
分析化学
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DOI
PubMed
高影响因子
CELLULAR AND MOLECULAR LIFE SCIENCES
·
2022
·Vol. 79
·期 8
·1-15
·
IF 9.207
Chang Chia-Chun,Peng Min,Zhong Jiale,Zhang Ziheng,Keppeke Gerson Dierley,Sung Li-Ying,Liu Ji-Long
The cytoophidium is a unique type of membraneless compartment comprising of filamentous protein polymers. Inosine monophosphate dehydrogenase (IMPDH) catalyzes the rate-limiting step of de novo GTP biosynthesis and plays critical roles in active cell metabolism. However, the molecular regulation of cytoophidium formation is poorly understood. Here we show that human IMPDH2 polymers bundle up to form cytoophidium-like aggregates in vitro when macromolecular crowders are present. The self-association of IMPDH polymers is suggested to rely on electrostatic interactions. In cells, the increase of molecular crowding with hyperosmotic medium induces cytoophidia, while the decrease of that by the inhibition of RNA synthesis perturbs cytoophidium assembly. In addition to IMPDH, CTPS and PRPS cytoophidium could be also induced by hyperosmolality, suggesting a universal phenomenon of cytoophidium-forming proteins. Finally, our results indicate that the cytoophidium can prolong the half-life of IMPDH, which is proposed to be one of conserved functions of this subcellular compartment.
研究领域:
细胞生物学
·
分子生物学
·
生物化学
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DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2020
·
IF 4.049
Jian Yang,Xue Zhang,Yasen Mijiti,Yakun Sun,Man Jia,Zhaosheng Liu,Yanping Huang,Haji Akber Aisa
The topic in the present paper is to prepare molecularly imprinted polymer (MIP) using the template molecule with low purity. For the first time, a surrounding of macromolecular crowding was established to promote the formation of the complex of the template with functional monomer efficiently thus highly pure template molecule was unnecessary. In this study, the MIP monolith was synthesized using low purity lactucopicrin as template in place of highly pure one, and polystyrene was used as macromolecular crowding agent. 4-Vinylpyridine and ethyleneglycol dimethacrylate were used as functional monomer and crosslinker, respectively. Polymerization parameters, including the ratio of functional monomer/template, various template concentrations, and PS concentration on the affinity of the resulting MIP were systematically investigated. For the lactucopicrin MIP made with the purity of lactucopicrin of 92%, the imprinting factor can be up to 2.2. The resulting MIP was filled in solid phase extraction (SPE) cartridge to purify lactucopicrin from the crude extract of Cichorium glandulosum Boiss. et Huet. After two cycles of MIP SPE for the crude extract, the highest recovery and purity of lactucopicrin was 64.8% and 97.8%, respectively. The results indicated that the use of macromolecular crowding agent is an effective method for improving the performance of the MIP prepared with the template of low purity, particularly valuable to the cases in which the highly pure target molecule is hard to be obtained.
研究领域:
化学
·
生物学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Li Wen,Jinxia Zheng,Zhijie Ke,Jian Dong
Enzymes catalyze cascade reactions in a crowded cellular environment where as much as half of cell volume is occupied by various macromolecules. Nonspecific interaction between enzymes and crowders and excluded volume of the crowders can superimpose on each other and complicate catalytic activity of the enzymes. This study investigates the interaction between a β-galactosidase (β-Gal) and glycosylated acrylamide polymer (P(Glc-β-EAAm)) and unravels the macromolecular crowding effect of the glycopolymer on enzymatic cascade catalysis consisting of β-Gal, glucose oxidase and hydrogen peroxidase. Binding of the glycopolymer induced conformational alterations in β-Gal and gave rise to static fluorescence quenching and stable complex formation with β-Gal via nonspecific interaction. Fluorescence resonance energy transfer assays further demonstrated a compact association between β-Gal and glycopolymer crowders, with binding affinity correlating with the molecular weight of glycopolymer. The reduction of the apparent kinetic constants of the catalysis with the glycopolymer size showed the role of the multivalent effect in enzyme-substrate interactions. The kinetics also depended on the chain overlapping conditions of the crowders. Therefore, the macromolecular crowding effect on the cascade reaction is jointly associated with the crowder's multivalent effect, chain overlapping conditions of the crowders, in addition to the volume exclusion effect of the crowders.
研究领域:
生物化学
·
酶学
·
高分子科学
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DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2025
·
IF 15.6
Shiqiang Wei,Hongwei Shou,Zheng-Hang Qi,Shuangming Chen,Yong Han,Shucheng Shi,Yixiu Wang,Pengjun Zhang,Jialin Shi,Zijun Zhang,Yuyang Cao,Changda Wang,Jiewu Cui,Xiaojun Wu,Zhi Liu,Li Song
Electrode–electrolyte interface plays a crucial role in determining the stability and behavior of electrochemical electrodes. Although X-ray photoelectron spectroscopy has been established as a powerful analytical technique for interface chemistry, the necessity for ultrahigh vacuum remains a significant obstacle to directly detecting dynamic interfacial evolution, particularly in aqueous environments. Here, we employ tender-energy ambient pressure X-ray photoelectron spectroscopy (AP-XPS) to bridge the gap between ultrahigh vacuum and near-atmospheric pressure, enabling an in-depth investigation of the molecule-crowded aqueous interface evolution in a Zn metal anode. The results demonstrate that the persistent presence of additive molecules effectively inhibits direct contact between reactive Zn and H2O, while also facilitating uniform Zn deposition. In situ optical microscopy observations and synchrotron radiation X-ray diffraction further verified the uniform and dense Zn deposition, attributed to lateral growth induced by the (002) crystal facet evolution. As proof of its effectiveness, batteries incorporating the Zn//Zn, Zn//Cu, and full cell with the additive demonstrate significantly improved stability and reversibility. This finding opens up new avenues for exploration of interfacial chemistry at the molecule level, offering insights into the design of highly stable metal anodes of aqueous ion batteries for practical applications.
研究领域:
材料科学
·
电化学
·
表面科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2016
·Vol. 39
·期 10
·1963-1970
·
IF 2.741
Guang-Ying Sun,Chao Wang,Yu-Qin Luo,Yong-Xin Zhao,Jian Yang,Zhao-Sheng Liu,Haji Akber Aisa
The combination of molecular crowding and virtual imprinting was employed to develop a cost-effective method to prepare molecularly imprinted polymers. By using linear polymer polystyrene as a macromolecular crowding agent, an imprinted polymer recognizable to punicalagin had been successfully synthesized with punicalin as the dummy template. The resulting punicalin-imprinted polymer presented a remarkable selectivity to punicalagin with an imprinting factor of 3.17 even at extremely low consumption of the template (template/monomer ratio of 1:782). In contrast, the imprinted polymer synthesized without crowding agent, did not show any imprinting effect at so low template amount. The imprinted polymers made by combination of molecular crowding and virtual imprinting can be utilized for the fast separation of punicalagin from pomegranate husk extract after optimizing the protocol of solid-phase extraction with the recovery of 85.3 ± 1.2%.
研究领域:
分析化学
·
天然产物分离纯化
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DOI
PubMed
高影响因子
Soft Matter
·
2015
·Vol. 11
·期 29
·5940-5946
·
IF 4.029
Wangqin Song,Lvdan Liu,Guangming Liu
Macromolecular crowding plays a significant role in the solubility and stability of biomacromolecules. In this work, the thermo-sensitive poly(N-isopropylacrylamide) (PNIPAM) has been employed as a model system to study the specific ion effects on the solubility of macromolecules in crowded environments of dextran and polyethylene glycol (PEG). Our study demonstrates that crowding agents can interact with either anions or PNIPAM chains. The chaotropic anion SCN− interacts with dextran but does not interact with PEG. Both Cl− and CH3COO− do not interact with dextran and PEG. On the other hand, dextran can interact with PNIPAM as a hydrogen-bond donor, whereas PEG interacts with PNIPAM as a hydrogen-bond acceptor. The salting-in effect exerted by SCN− on PNIPAM is weakened in the crowded environment of dextran but is strengthened in the crowded environment of PEG due to the distinct anion-crowder interactions. In parallel, the salting-out effect generated by Cl− and CH3COO− on PNIPAM is weakened by the crowding of dextran but is strengthened by the crowding of PEG because of the different macromolecule–crowder interactions. Our study reveals that the ion specificity of macromolecules is altered significantly changing from dilute solutions to crowded environments.
研究领域:
生物物理学
·
高分子化学
·
细胞生物学
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DOI
高影响因子
MACROMOLECULES
·
2024
·
IF 5.1
Jianing Zhou,Tao Zheng,Huanli Qi,Yiren Wang,Mingming Ding,Lianwei Li
By using a series of mixed solutions composed of styrene oligomers (PSN, 10 < N < 550) and toluene, this work explores how the macromolecule crowding effects, including viscosity effect and conformational compression, regulates the flow-driven translocation, i.e., compression-induced fractionation (CIF), of polystyrene long chains (PS-1100k, 1.10 × 106 g/mol) through nanochannels (average pore radius r0 ≈ 10 nm). The correlation between the macroscopic critical flow rate (Qc) and apparent viscosity (ηapp) has been tested. Specifically, we have found the following: (1) ηapp of PSN–toluene mixed solutions is found to be easily regulated in a broad range (0.52 ≤ ηapp ≤ 5.02 mPa·s) by the oligomer strategy, which is beyond the window achieved by the small-molecule solvent system; (2) the translocation experiments in mixed solutions support the relation of Qc ∼ 1/ηapp predicted by de Gennes theory in the range of 0.52 mPa·s ≤ ηapp ≤ 1.53 mPa·s, but a deviation is observed when 1.53 < ηapp ≤ 5.02 mPa·s, implying the potential influence from the conformational compression of chains for CIF; (3) through a coarse-grained simulation on the blend system composed of a long chain (Nl = 100) and oligomer short chains (1 ≤ Ns ≤ 20) with varied volume fraction (φs) from 0.1 to 0.4, the simulation result shows that the degree of compression of the long chain increases with Ns and φs of oligomer short chains. Overall, the present study has preliminarily explored how the macromolecule crowding effects (viscosity effect and conformational compression) play the dominant role in regulating translocation behavior during the CIF process, which paves the foundation for understanding the transmembrane transport of biological macromolecules in the natural crowding cell environments.
研究领域:
高分子科学
·
生物物理学
·
计算模拟
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Jing Xie,Yuepeng Guan,Yaqin Huang,Yi-Chun Lu
Molecular crowding electrolytes extend the stability window of aqueous batteries with water-miscible/soluble polymers at a low concentration of lithium salts [2 m lithium bis(trifluoromethane sulfonyl)imide (LiTFSI)]. Water decomposition [especially hydrogen evolution reaction (HER)] is effectively suppressed, enabling the use of numerous negative electrodes which cannot work in traditional aqueous electrolytes. However, the mechanism underlying the cathodic stability of molecular crowding electrolytes is not yet fully understood. Here, we compare the HER suppression effect in molecular crowding electrolytes with LiTFSI and lithium perchlorate and correlate their distinct cathodic stability to the difference in the solid–electrolyte interphase (SEI). This work reveals the critical role of LiF in developing a stable SEI and suppressing the HER in molecular crowding electrolytes, providing a design path for safe, low-cost, and high-voltage aqueous batteries.
研究领域:
电化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）