ACS Applied Materials & Interfaces
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2026
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IF 7.8
Ming Zhang,Guoli Fan,Liyuan Yuan,Feng Li
Bioethanol upgrading to higher alcohols (C4–10–OH) involves several sequential reaction steps occurring at multiple different active sites. Therefore, precisely engineering heterogeneous catalysts with appropriate local chemical structures of active sites and spatial environments is highly desired for efficient ethanol tandem conversion. Herein, we constructed a novel Cu-based catalyst featuring atomically dispersed Cu sites confined in a hierarchical silicalite-1@La2O3@silicalite-1 architecture, where single Cu atoms were confined in the micropores of surface silicalite-1 (S-1) zeolite nanoislands dispersed on the outer La2O3 layer encapsulating a hollow S-1 zeolite core. By modulating the content of Cu and La species, such a constructed multihierarchical Cu@S-1@La2O3@S-1 catalyst exhibited excellent performance in ethanol conversion to higher alcohols, along with an impressively high ethanol conversion of 74.9% and C4–10–OH selectivity of 85.0%, as well as an unprecedentedly high production rate of higher alcohols (10.575 mol·gCu–1·h–1) at 275 °C, far exceeding those over state-of-the-art Cu-based catalysts. It was elucidated that surface single-atom Cu sites first notably promoted the adsorption and activation of ethanol and thus initiated its dehydrogenation to produce acetaldehyde, and subsequently, acetaldehyde intermediates migrated to the outer La2O3 layer featuring abundant medium-strength basic and acidic sites, thereby facilitating the condensation of acetaldehydes and their further dehydration. This work provides an innovative approach for rationally designing high-performance supported Cu catalysts with a spatiotemporal decoupling structure applied in advanced heterogeneous tandem catalytic processes through the design of site-specific confinement within hierarchical structures.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Shaohui Xiong,Xingyi Ou,Qingquan Liu,Yiwen Li,Juntao Tang,Guipeng Yu,Chunyue Pan,Shibo Guo,Sitong Li,Menghan Yong
Polymers of intrinsic microporosity (PIM) have attracted considerable attention in the development of mixed matrix membranes (MMMs) for CO 2 separation. A prominent challenge lies in engineering the spacing of the polymer matrix chains while eliminating non-selective interfacial defects. In this study, a CO 2 -philic triazine-based porous polymer, featuring robust hydrogen bond donating groups, was employed to fabricate a series of interfacial defect-free PIM-1 based MMMs (denoted as PIM-1/CSU-1). The interfacial adhesion and compatibility have been greatly improved due to the strengthened hydrogen bond interaction, which was systematically validated through variable-temperature infrared spectroscopy. Additionally, the formation of hydrogen bonds allowed for the regulation of the polymer matrix chain spacing, making the chain distance loose. Remarkably, the resulting membrane exhibited a CO 2 permeability of 13,429 Barrer and CO 2 /N 2 selectivity of 33.1—246.6% and 70.2% higher than pristine PIM-1, respectively, surpassing the latest Jansen/McKeown upper bound established in 2019, but also significantly exceed the performance of previously reported MMMs for CO 2 separation. The strategy of mitigating interfacial defects through the formation of hydrogen bonds between fillers and the polymer matrix emerges as a viable and effective method for fabricating gas separation membranes with exceptional separation capabilities.
研究领域:
材料科学
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高分子化学
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气体分离
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膜技术
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物理化学
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JOURNAL OF MOLECULAR STRUCTURE
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2021
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IF 3.196
Dandan Huang,Dezhi Yang,Yang Lv,Jianle Zhou,Liang Li,Jiangping Xu,Xuemei Yang,Zhengzheng Zhou
Cocrystal hydrate accounts for a small percentage of cocrystals of poorly water-soluble drugs, and still lack the explanation on its cause of formation. In this study, a cocrystal hydrate with a novel phosphodiesterase-4 (PDE-4) inhibitor, chlorbipram, is prepared and characterized using multi-techniques. The dissolution behavior, ternary phase diagram and theoretical calculations are further performed and discussed. Chlorbipram: m-Hydroxybenzoic acid (ChBP-MHBA, 1: 1) cocrystal hydrate presents approximate equivalent dissolution (1.61 mg/mL) in comparison with ChBP (1.90 mg/mL) in isopropanol/water (1: 1, v/v) solution. Ternary phase diagram plotted in ethyl acetate solvent suggests that ChBP-MHBA cocrystal hydrate has an optimum mass percentage range from (2.91%: 2.64%: 94.45%) to (3.20%: 10.74%: 86.06%) among ChBP, MHBA and ethyl acetate. There are two lattice waters in each unit cell of ChBP-MHBA cocrystal hydrate, accounting for 4.5% proportion of the cell volume using contact surface calculations. Molecular Electrostatic Potential Surface (MEPS) investigations indicate that the strong hydrogen bonds are formed within the cocrystal lattice, which are between the global minimum values of ChBP/MHBA and the global maximum values of lattice water. In summary, lattice water plays an important role in the formation of cocrystal hydrate, providing hydrogen atom donor and forming hydrogen bonds to support its three-dimensional crystal structure.
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Antioxidants
·
2021
·Vol. 10
·期 11
·1697
·
IF 6.313
Shiling Feng,Chunyan Zhang,Tao Chen,Lijun Zhou,Yan Huang,Ming Yuan,Tian Li,Chunbang Ding
Oleuropein (OLE) is a secoiridoid glycoside that mainly exists in olives with multifaceted health benefits. The present study aimed to investigate the stress resistance and lifespan extension effects of OLE inCaenorhabditis elegans. The results showed that OLE could significantly prolong the lifespan ofC. elegansby 22.29%. Treatment with OLE also significantly increased the survival rates of worms against lethal heat shock and oxidative stress. Meanwhile, OLE supplementation increased the expression and activity of antioxidant enzymes and suppressed the generation of malondialdehyde in nematodes. In addition, the results from mutants implied that OLE might mediate longevity and stress resistance via DAF-16/FoxO, which played a vital role in the insulin/IGF-1 signaling (IIS) pathway. To further identify the molecular targets of OLE, mRNA level and loss-of-function mutants of IIS-associated genes were investigated. The data revealed that OLE activated IIS by down-regulating the upstream components,daf-2andage-1. Furthermore, another stress response and longevity pathway in parallel to DAF-16, SKN-1/Nrf2, was also shown to involve in OLE-induced beneficial effects. Collectively, these results provide the theoretical basis that OLE could enhance the stress resistance and increase the lifespan ofC. elegansthrough the IIS and SKN-1/Nrf2 signaling pathways.Keywords:oleuropein;Caenorhabditis elegans;longevity;stress resistance
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2020
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IF 2.369
Xiaoda Wang,Lumin Han,Weican Wang,Ling Li,Ting Qiu
The enzymatic reaction–distillation coupling process is a promising technology to realize the chiral resolution of (R/S)-1-phenylethanol with ethyl butyrate and ethanol as acyl donor and byproduct, respectively. In order to design such a coupling process, the vapor–liquid equilibrium (VLE) data are necessary. However, these data were incomplete in literatures. In this work, the isobaric VLE experiments were conducted at 101.3 kPa for the binary systems of 1-phenylethanol + ethyl butyrate, 1-phenylethanol + ethanol, 1-phenylethyl butyrate + ethyl butyrate, 1-phenylethyl butyrate + ethanol, and 1-phenylethyl butyrate +1-pheny ethanol. Additionally, the saturated vapor pressure of 1-phenylethyl butyrate was measured in the temperature range 420–500 K and correlated with the Antoine equation. Both the Non-Random Two Liquid (NRTL) and Wilson models were used for the correlation of experimental VLE data. Both models showed satisfactory accuracy, although the Wilson model performed slightly better than the NRTL model. This work would provide important thermodynamic information for the design of enzymatic reaction–distillation coupling process to realize the chiral resolution of (R/S)-1-phenylethanol.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2023
·
IF 2.6
Chenyang Yao,Ji Mi,Pengfei Jiang,Cui Ye,Yitong Dai,Yongsheng Guo,Wenjun Fang
Active cooling by endothermic hydrocarbon fuels (EHFs) is considered as a practical approach to deal with the thermal management problem of hypersonic aircrafts. As a typical component of EHFs, decalin is usually thermally stable while it is apt to coke and has poor combustion performance. n-Hexadecane, a normal alkane with a relatively high H/C ratio, can effectively improve the combustion performance of EHFs, and 1-butanol has remarkable anti-coking properties. As a fundamental work for fuel design, decalin, n-hexadecane, and 1-butanol were selected as model compounds to construct a surrogate fuel system, which was used to investigate the effects of composition and condition on its thermophysical properties. Densities (ρ) and viscosities (η) of the ternary system of decalin (1) + n-hexadecane (2) + 1-butanol (3) and corresponding binary systems were measured at temperatures T = (293.15 to 333.15) K and pressure p = 0.1 MPa. The excess molar volumes (VmE) and the viscosity deviations (Δη) of the mixtures were calculated and fitted to several semi-empirical equations. The tendencies of VmE and Δη with composition and temperature were discussed from intermolecular force and molecular size, respectively.
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JOURNAL OF MOLECULAR LIQUIDS
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2014
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IF 2.083
Yajie Jiang,Tao Geng,Qiuxiao Li,Guojin Li,Hongbin Ju
The 1:1 salt-free catanionic surfactant dodecyltrimethylammonium decanoate (DTAD) was synthesized directly by a novel method, and the product was recrystallized to come up to purity received. Surface activity and self-assembly of 1:1 salt-free catanionic surfactant DTAD and the influences of temperature, pH and salinity on which have been studied in the present work. The critical micelle concentration (CMC), surface tension reduction (γ CMC ), surface excess (Γ max ), and mean molecular surface area ( A min ) were determined from plots of surface tension (γ) versus logarithm of surfactant concentration. The results showed that the salt-free catanionic surfactant had much lower CMC, γ CMC and A min values than their corresponding single cationic and anionic surfactants . The Gibbs energy of mixing (△ G E ) was negative, indicating the strong interaction of cationic and anionic parts. The tested temperature and salinity had no significant effect on the surface properties of DTAD. The surface activity enhanced in acidic pH and decreased slightly in alkaline pH . The aggregate structure almost had no change with temperature, but transformed into spheres with addition of inorganic salts. The pH effect was complex, the ability of vesicles formation was improved in strong alkaline condition; vesicles transformed into large disks or large cubes in acidic condition.
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STEROIDS
·
2024
·
IF 2.1
Jinwen Chen,Wei Chen,Xiaoyu Li,Yiping Ye,Wenkang Huang,Lijuan Gao,Meng Zhang
Colorectal cancer (CRC) is one of the most common gastrointestinal cancers that results in death in worldwide. The Hedgehog (HH) signalling pathway regulates the initiation and progression of CRC. Inhibiting the HH pathway has been presented as a potential treatment strategy in recent years. Cynanbungeigenin C (CBC) is a new type of C 21 steroid that has been previously reported for the treatment of medulloblastoma. However, its further investigation was limited by its poor water solubility. In this study, six new CBC derivatives were synthesized through the structural modification of CBC, and four of them showed better water solubility than CBC. Moreover, their antiproliferative activities on CRC were evaluated. It was found that CBC-1 presented the best inhibitory effect on three types of CRC cell lines, and this effect was superior to that of CBC. Mechanistically, CBC-1 inhibited the proliferation of CRC cells through regulation of mRNA and proteins of the HH pathway according to qRT–PCR and Western blotting analysis. Furthermore, Cellular Thermal Shift Assay results indicated that CBC-1 regulated this signalling pathway by targeting glioma‑associated oncogene (GLI 1).In addition, cell apoptosis was induced increasingly by transfection with GLI 1 siRNA or treatment with CBC-1 to downregulate GLI 1. Last, the in vivo results demonstrated that CBC-1 significantly reduced tumour size and downregulated GLI 1 in CRC. Therefore, this study suggests that CBC-1, a new GLI 1 inhibitor derived from natural products, may be developed as a potential antitumour candidate for CRC treatment.
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JOURNAL OF PHYSIOLOGY AND BIOCHEMISTRY
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2024
·
IF 3.7
Pei Haibing,Lin Zhiyin,Yao Kexin,Luo Yeqing,Tong Ping,Chen Hongbing,Wu Yong,Wu Zhihua,Gao Jinyan
Ovalbumin (OVA) is a major allergen in eggs and could induce severe allergic reactions in sensitive individuals, where the innate immune system works as a regulator. The mechanism of how innate immunity adjusts to food allergy is relatively well-studied, however, the effects of allergen uptake on the innate immune system remain unclear. Therefore, the Caenorhabditis elegans ( C. elegans ) model was utilized to assess the effects of OVA on its innate immune system. OVA enhanced the immune response of C. elegans with higher survival rates under Pseudomonas aeruginosa infection. Moreover, sustaining OVA treatment improved the health states that were reflected in the prolonged lifespan, alleviated oxidative stress, accelerated growth, and promoted motility. RNA-sequencing analysis and the slow-killing assays in the mutants of insulin/IGF-1 signaling (IIS)-related genes confirmed that IIS was necessary for OVA to regulate innate immunity. Besides, OVA activated SKN-1 temporarily and facilitated the nuclear localization of DAF-16 for improving immunity and health status in C. elegans . Together, OVA could enhance the innate immune responses via DAF-16 and SKN-1 pathways in the IIS of C. elegans , and this work will provide novel insights into the regulation of innate immunity by OVA in higher organisms.
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JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Yuan Li,Shengkai Sun,Hanfang Liu,Wenna Wang,Dehong Chen,Yu Yang,Feng Liu,Bin Yu,Jia Liu,Binjie Li,Lei Wang,Bin Li
Epoxidation of olefin catalyzed by titanium silicalite-1 (TS-1) can obtain important intermediate epoxides of industrial production in a green and pollution-free manner. However, due the problem of macromolecules transport path restraint, which cause the catalyst to fail in lifetime and activity. Strategically, to increase the transport channel of macromolecules and shorten the transport path, it is necessary to introduce mesoporous structures into zeolite. Here, we report a solid-state synthesis of hierarchical TS-1 zeolite by optimizing carbon black sequence. The texture property of hierarchical TS-1 can be optimized by carbon black. Most importantly, the addition sequence of carbon black can impact the porosity of hierarchical TS-1. The hierarchical zeolite is synthesized by incorporating 0.2 g carbon black into the seeds. When carbon black is firstly combined with seeds, the enhanced interaction facilitates the subsequent growth process, leading to large surface area from mesopores (121 m 2 /g) and abundant pores size (8–40 nm) and enhanced exposure of Ti active sites. The optimized hierarchical TS-1 possesses excellent catalytic performance with high conversion rate (24.4 %) and similar selectivity (93.8 %), which are 1.6 times higher than that of traditional TS-1 zeolites.
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Catalysts
·
2024
·Vol. 14
·期 12
·939
·
IF 3.8
Yuting Sun,Xinyu Chang,Junling Zhan,Chongyao Bi,Zhehan Dong,Shuaishuai Sun,Mingjun Jia
To synthesize high-quality TS-1 zeolites with enhanced catalytic performance for 1-hexene epoxidation is highly attractive for meeting the increased need for sustainable chemistry. Herein, we report that a series of framework Ti-enriched TS-1 zeolites with high crystallinity can be effectively synthesized by the hydrothermal crystallization of a composite precursor composed of diol-based polymer (containing titanium and silicon) and tetrapropylammonium bromide (TPABr). The pre-addition of a certain amount of TPABr into the polymer-based precursor plays a very positive role in maintaining the high crystallinity and framework Ti incorporation rate of TS-1 zeolites under the premise that a relatively low concentration of tetrapropylammonium hydroxide (TPAOH) template is adopted in the following hydrothermal crystallization process. The condition-optimized TS-1 zeolite with a smaller particle size (300–500 nm) shows excellent catalytic activity, selectivity, and recyclability for the epoxidation of 1-hexene with H2O2as an oxidant, which can achieve a 75.4% conversion of 1-hexene and a 99% selectivity of epoxide at a reaction temperature of 60 °C, which is much better than the TS-1 zeolites reported in the previous literature. The relatively small particle size of the resultant TS-1 crystals may enhance the accessibility of the catalytically active framework Ti species to reagents, and the absence of non-framework Ti species, like anatase TiO2, and low polymerized six-coordinated Ti species could effectively inhibit the ineffective decomposition of H2O2and the occurrence of side reactions, leading to an improvement in the catalytic efficiency for the epoxidation of 1-hexente with H2O2.
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MOLECULAR CARCINOGENESIS
·
2024
·
IF 3
Beibei Wang,Xin Fan,Lingang Wang,Xiaosong Wei
Sorbin and SH3 domain-containing 2 (SORBS2) is an RNA-binding protein and has been implicated in the development of some cancers. However, its role in bladder cancer (BC) is yet to be established. The expression of SORBS2 in BC tissues was determined from the Gene Expression Omnibus and Gene Expression Profiling Interactive Analysis databases and collected paired tumor/normal samples. The effects of SORBS2 on BC cells were detected by CCK-8, colony formation, Transwell, dual-luciferase, RNA immunoprecipitation, chromatin immunoprecipitation, and DNA pull-down assays. In vivo, BC cell growth and metastasis were studied by a xenograft subcutaneous model and a tail-vein metastasis model. The results showed that SORBS2 expression was significantly decreased in BC tissues and cells. SORBS2 overexpression inhibited cell proliferation, migration, invasion, and epithelial–mesenchymal transition in vitro and tumor growth and metastasis in vivo, while silencing SORBS2 produced the opposite effect. Mechanistically, we found that SORBS2 enhanced the stability of tissue factor pathway inhibitor (TFPI) mRNA via direct binding to its 3′ UTR. Restoration of TFPI expression reversed SORBS2 knockdown-induced malignant phenotypes of BC cells. In addition, SORBS2 expression was negatively regulated by the transcription factor specificity protein 1 (SP1). Conversely, SORBS2 can be transcriptionally regulated by SP1 and inhibit BC cell growth and metastasis via stabilization of TFPI mRNA, indicating SORBS2 may be a promising therapeutic target for BC.
研究领域:
肿瘤学
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分子生物学
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癌症研究
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