INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 19
·14805
·
IF 5.6
Xiao Xia,Jun Ma,Fei Liu,Haifeng Cong,Xingang Li
In the heavy petroleum industry, the development of efficient demulsifiers for the effective breaking of interfacially active asphaltenes (IAA)-stabilized water-in-heavy oil (W/HO) emulsions is a highly attractive but challenging goal. Herein, a novel nitrogen and oxygen containing demulsifier (JXGZ) with strong hydrogen bonding has been successfully synthesized through combining esterification, polymerization and amidation. Bottle tests indicated that JXGZ is effectual in quickly demulsifying the IAA-stabilized W/HO emulsions; complete dehydration (100%) to the emulsions could be achieved in 4 min at 55 °C using 400 ppm of JXGZ. In addition, the effects of demulsifier concentration, temperature and time on the demulsification performance of JXGZ are systematically analyzed. Demulsification mechanisms reveal that the excellent demulsification performance of JXGZ is attributed to the strong hydrogen bonding between JXGZ and water molecules (dual swords synergistic effect under hydrogen bond reconstruction). The interaction of the “dual swords synergistic effect” generated by two types of hydrogen bonds can quickly break the non-covalent interaction force (π-π stacking, Van der Waals force, hydrogen bonds) of IAA at the heavy oil–water interface, quickly promote the aggregation and coalescence of water molecules and finally achieve the demulsification of W/HO emulsions. These findings indicate that the JXGZ demulsifier shows engineering application prospects in the demulsification of heavy oil–water emulsions, and this work provides the key information for developing more efficient chemical demulsifiers suitable for large-scale industrial applications.Keywords:demulsifier;hydrogen bonds;interactions;water-in-heavy oil emulsions
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高影响因子
Acta Biomaterialia
·
2023
·
IF 9.7
Yifei Wang,Jia Wang,Yunke Jiao,Kangli Chen,Tianhao Chen,Xinping Wu,Xingwu Jiang,Wenbo Bu,Changsheng Liu,Xue Qu
Chemodynamic therapy (CDT) based on generating reactive oxygen species (ROS) is promising for cancer treatment. However, the intrinsic H 2 O 2 is deficient for CDT, and glutathione (GSH) eliminates ROS to protect tumor cells from ROS cytotoxicity. Herein, we propose a strategy to switch the electron flow direction of GSH for O 2 reduction and ROS generation rather than ROS clearance by using P(DA-Fc) nanoparticles , which are polymerized from ferrocenecarboxylic acid (Fc) coupled dopamine. P(DA-Fc) NPs with phenol-quinone conversion ability mimic NOX enzyme to deprive electrons from GSH to reduce O 2 for H 2 O 2 generation; the following •OH release can be triggered by Fc. Semiquinone radicals in P(DA-Fc) are significantly enhanced after GSH treatment, further demonstrated with strong single-electron reduction ability by calculation. In vitro and in vivo experiments indicate that P(DA-Fc) can consume intrinsic GSH to produce endogenous ROS; ROS generation strongly depends on GSH/pH level and eventually causes tumor cell death. Our work makes the first attempt to reverse the function of GSH from ROS scavenger to ROS producer, explores new roles of PDA-based nanomaterials in CDT beyond photothermal reagents and drug carriers, and provides a new strategy to improve the efficiency of CDT. Statement of Significance P(DA-Fc) nanoparticles performing tumor microenvironment response capacity and tumor reductive power utilize ability were fabricated for CDT tumor suppression. After endocytosis by tumor cells, P(DA-Fc) deprived GSH of electrons for H 2 O 2 and •OH release, mimicking the intrinsic ROS production conducted by NADPH, further inducing tumor cell necrosis and apoptosis. Our work makes the first attempt to reverse the function of GSH from ROS scavenger to producer, explores new functions of PDA-based nanomaterials in CDT beyond photothermal reagents and drug carriers, and provides a new strategy to improve CDT efficiency.
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PROGRESS IN ORGANIC COATINGS
·
2023
·
IF 6.6
Jinglong Pan,Xi Liu,Xiangkang Cao,Xiaoze Ma,Yunfei Hu,Guangyi Cai,Xinxin Zhang,Zehua Dong
Environmentally friendly antifouling coatings have received increasing attention in the field of marine infrastructures. In this work, a carboxy-betaine salicylate surface-modified silica nanofiller (QAs-SA@SiO 2 NPs) was synthesized and doped in polyurethane coatings (PU) to gain durable antifouling properties. The modified silica NPs were prepared by the covalent bond grafting method and then dispersed in PU paint to produce a kind of composite anti-fouling coating (QAs-SiO 2 PU). It is noted that the QAs-SiO 2 PU coating can adjust the release rate of salicylate according to environmental pH value. Once the salicylate layer was dissolved, the inner amphoteric carboxy-betaine molecules would be exposed to form a hydrated layer on QAs-SA@SiO 2 NPs, thus realizing a step-by-step antifouling performance. The experimental results show that the 7 wt% addition of QAs-SA@SiO 2 filler in the PU coating can reduce protein adhesion by 99.1 %, bacterial adhesion by 99.8 %, and chlorella adhesion by 95.0 %, presenting a significant mussels-repellence ability compared to the pristine PU coating. This work may provide a promising approach to designing eco-friendly and durable marine anti-fouling and anti-corrosion coatings.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Yanxiao Yang,Yunfeng Guo,Zhe Qiu,Weihua Gong,Yonggui Wang,Yanjun Xie,Zefang Xiao
Metal-organic frameworks (MOFs) are characterised by high porosity levels and controllable structures, making them ideal adsorbents for wastewater. However, obtaining substrate materials with mechanical stability, excellent pore accessibility, and good processability for compositing MOF crystal powders to adsorb multiple pollutants in complex aqueous environments is challenging. In this study, porous MOFs@ modified cellulose sponge (MCS) composites were fabricated using MCS as a scaffold to provide anchoring sites for the coordination of Zr 4+ ions and further in situ synthesis of MOFs, namely UiO-66@MCS and UiO-66-NH 2 @MCS, which effectively removed heavy metal ions and organic dyes. MOFs@MCS composites exhibit excellent water and dimensional stability, maintaining the pore structure by ambient drying during reuse. Compared with UiO-66@MCS composite, UiO-66-NH 2 @MCS composite exhibited a higher adsorption capacity of 224.5 mg·g −1 for Hg 2+ and 400.9 mg·g −1 for methylene blue (MB). The adsorption of Hg 2+ onto the MOFs@MCS composites followed the Langmuir and pseudo-second-order models, whereas the Freundlich and pseudo-second-order models were more suitable for MB adsorption. Moreover, the MOFs@MCS composites exhibited excellent reusability and were selective for the removal of Hg 2+ . Overall, this approach effectively combines Zr-based MOFs with mechanically and dimensionally stable porous cellulose sponges, rendering the approach suitable for purifying complex wastewater.
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MOLECULES
·
2023
·Vol. 29
·期 1
·171
·
IF 4.6
Wenjie Li,Shenghui Hao,Hengyang Li,Qi An,Lina Yang,Bing Guo,Zijing Xue,Yongli Liu,Long Guo,Yuguang Zheng,Dan Zhang
Metabolic product accumulation exhibited variations among mulberry (Morus albaL.) leaves (MLs) at distinct growth stages, and this assessment was conducted using a combination of analytical techniques including high-performance liquid chromatography (HPLC), gas chromatography–mass spectrometry (GC-MS), and liquid chromatography–mass spectrometry (LC-MS). Multivariate analysis was applied to the data, and the findings were correlated with antioxidant activity and α-glucosidase inhibitory effects in vitro. Statistical analyses divided the 27 batches of MLs at different growth stages into three distinct groups. In vitro assays for antioxidant activity and α-glucosidase inhibition revealed that IC50values were highest at the Y23 stage, which corresponds to the ‘Frost Descends’ solar term. In summary, the results of this study indicate that MLs at different growth stages throughout the year can be categorized into three primary growth stages using traditional Chinese solar terms as reference points, based on the observed variations in metabolite content.Keywords:Morus albaL.;primary metabolites;secondary metabolites;different growth stages;antioxidant activity
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ACS Biomaterials Science & Engineering
·
2022
·
IF 5.395
Yan Wang,Shuhui Gao,Kongying Zhu,Lixia Ren,Xiaoyan Yuan
Cryopreservation of red blood cells (RBCs) is imperative for transfusion therapy, while cryoprotectants are essential to protect RBCs from cryoinjury under freezing temperatures. Trehalose has been considered as a biocompatible cryoprotectant that naturally accumulates in organisms to tolerate anhydrobiosis and cryobiosis. Herein, we report a feasible protocol that enables glycerol-free cryopreservation of human RBCs by integration of the synthesized trehalose lipids and dissociative trehalose through ice tuning and membrane stabilization. Typically, in comparison with sucrose monolaurate or trehalose only, trehalose monolaurate was able to protect cell membranes against freeze stress, achieving 96.9 ± 2.0% cryosurvival after incubation and cryopreservation of human RBCs with 0.8 M trehalose. Moreover, there were slight changes in cell morphology and cell functions. It was further confirmed by isothermal titration calorimetry and osmotic fragility tests that the moderate membrane-binding activity of trehalose lipids exerted cell stabilization for high cryosurvival. The aforementioned study is likely to provide an alternative way for glycerol-free cryopreservation of human RBCs and other types of cells.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Jingshun Zhuang,Saerona Kim,Mairui Zhang,Jiae Ryu,Jeeranan Nonkumwong,Laongnuan Srisombat,Kwang Ho Kim,Jeong Jae Wie,Gyu Leem,Chang Geun Yoo
Lignin is a promising feedstock for renewable fuels and chemicals due to its aromatic skeleton and natural abundance. Lignin can be converted to diverse aromatic monomers as well as dicarboxylic acids depending on the applied conversion technologies. Despite its great potential, its native and processing-induced heterogeneity and complexity limit the conversion efficiency and product selectivity. In this study, magnesium ferrite (MgFe2O4) nanoparticle–peracetic acid (PAA) has been investigated as an efficient catalyst–oxidant incorporation for catalytic oxidative depolymerization of lignin under mild conditions. Typically, the increase in processing severity can enhance the lignin conversion while it results in the further decomposition of aromatic compounds to dicarboxylic acids. However, in this study, the incorporation of MgFe2O4 nanoparticles and PAA not only enhanced the total product yield but also improved the selectivity of aromatic monomers. The oxidative depolymerization system using the catalyst–oxidant combination resulted in 46 wt % of total oil product with a 61% selectivity of aromatic monomers under mild temperature (90 °C). In addition, this combination catalyst showed relatively good cycling stability based on the total product yield after recycling five times via magnetic separation. Overall, MgFe2O4 nanoparticles play an important role as a co-catalyst with a PAA oxidant in the oxidative conversion of lignin with an enhanced conversion efficiency and recyclability, and it will facilitate the valorization of lignin in future bio-based fuels and chemicals.
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FUEL
·
2023
·
IF 7.4
Linjie Guan,Meiyu Liu,Honghai Liu,Li Zhang,Yiming Zhang,Yucai Qin,Binbin He,Yi Mei,Yun Zu
The regulation of the engineering regionally spatial framework aluminum (Al F ) distribution in MFI channels has been considered as an effective way for the production of light olefins by targeted fluid catalytic cracking (TCO) technology. In this work, ZSM-5 zeolites with controlled Al F distributions are facilely synthesized by tuning the combinations of pentaerythritol (PET), tetrapropylammonium (TPA) and Na cations. The Al F atoms in the prepared HZ5-[PET + Na] and HZ5-[TPA] samples are enriched in the straight channels and intersection channels, respectively, which are favorable to the n-butane monomolecular reaction pathway, promoting the propylene production. Whereas the Al F atoms in the HZ5-[TPA + Na] sample are simultaneously distributed in both the straight and intersection channels, the n-butane molecules preferentially take place monomolecular reaction in the straight channels to generate carbonium ions (e.g., C 2 H 5 + , C 3 H 7 + and C 4 H 9 + ). Subsequently, all of them enter into the intersection channels to induce the occurrence of bimolecular reaction. Such a process is conducive to the formation of ethylene. These insights can help to clarify the catalytic behavior of regional framework acid sites in ZSM-5 channels and then provide an effective approach to design efficient TCO catalysts.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Xiaobo Xu,Xiaozhen Ma,Xiaolin Wang,Jin Zhu,Jinggang Wang,Ning Yan,Jing Chen
Using sustainable biomass feedstock to prepare biobased chemical products is attracting increasing attention. Betulin is a natural cyclic aliphatic diol that can be extracted in large quantities from the bark of birch trees. In this study, a series of bio-based polyurethane (PU) elastomers with excellent mechanical properties, solvent resistance, and thermal stability were synthesized under catalyst-free conditions using betulin and castor oil (CO) as the bio-based polyols. The chemical structure and properties of the bio-based PU elastomers were systematically investigated according to the effect of the hydroxyl ratio between betulin and CO. Due to the presence of abundant hydrogen bonds and rigid ring planes in the PU structure, and a higher cross-link density, the obtained PU elastomers had excellent mechanical properties. They achieved a maximum tensile strength of 31.6 MPa with the tensile strain reaching more than 200% and were able to withstand 1 × 105 times their weight. The thermal decomposition temperature of the betulin-derived PUs was over 300 °C. This study showcased a strategy to synthesize sustainable high-performance PU materials with a high biomass content (>75%).
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2023
·Vol. 37
·期 10
·e7230
·
IF 3.9
Dingning Chen,Haojie Yu,Li Wang,Sergey Z. Vatsadze,Jinyi Liu,Yu Wang
Ferrocene-based compounds are promising burning rate catalysts due to their attractive catalytic activity, flammability, and non-toxic performance. Unfortunately, the high-migration issue of the ferrocene-based catalysts makes it challenging to store composite solid propellants for a long time. Therefore, a dendrimer containing ferrocene units with anti-migration ability was designed herein. The introduction of polar groups provides a large number of interaction sites for anti-migration, and no migration of the dendrimer in the propellant was observed after 4 weeks of the aging test. For catalytic performance, the results showed that the thermal decomposition temperature of ammonium perchlorate could be reduced from 404°C to 369°C by adding 3 wt% ferrocene-based dendrimer. Moreover, compared with the propellant mixed with Catocene, the propellant containing ferrocene-based dendrimer showed a lower pressure exponent (0.47) and a higher burning rate (2.03 mm·s −1 , at 0.1 MPa).
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MOLECULES
·
2023
·Vol. 28
·期 14
·5523
·
IF 4.6
Qing Li,Yujuan Guo,Meijia Wu,Fei Deng,Jieying Feng,Jiafeng Liu,Sheng Liu,Chaoliu Ouyang,Wengui Duan,Shunmin Yi,Guangfu Liao
A series of highly fluorinated polyimide/allomelanin nanoparticles (FPI/AMNPs) films were prepared with FPI as the matrix and AMNPs as the filler. Due to the formation of hydrogen bonds, significantly reinforced mechanical and UV-shielding properties are acquired. Stress–strain curves demonstrated a maximum tensile strength of 150.59 MPa and a fracture elongation of 1.40% (0.7 wt.% AMNPs), respectively, 1.78 and 1.56× that of pure FPI. The measurements of the UV-vis spectrum, photodegradation of curcumin and repeated running tests confirmed the splendid UV-shielding capabilities of FPI/AMNPs films. The enhancement mechanisms, such as synergistic UV absorption of the charge transfer complexes in FPI and AMNPs and photothermal conversion, were the reasons for its exceptional UV shielding. The excellent comprehensive properties above enable FPI/AMNPs nanocomposites to be potential candidates in the field of UV shielding.Keywords:polyimide;allomelanin;mechanical properties;UV-shielding properties;nanocomposite
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ACS Catalysis
·
2023
·
IF 12.9
Xugang Yang,Zaihao Yuan,Minghao Zhou,Feng Chen,Bo-Qing Xu,Hui Shi
Lewis acidic heterogeneous catalysts are known to be active for transfer hydrogenation of carbonyl compounds, which occur naturally or can be derived from renewable feedstocks. While previous studies have explored a myriad of Zr-based catalytic systems toward the Meerwein–Pondorf–Verley (MPV) reductions, few have determined intrinsic, site-specific rates under strict kinetic control across a sufficiently wide range of process conditions, causing misconceptions about the true potentials of these catalysts for the targeted transformations. Here, we present a quantitative assessment on the intrinsic activities of four types of Zr catalysts that are purportedly promising candidates for the MPV reductions; the selected catalysts contain active Zr sites within diversified local coordination and secondary solvating environments. A comprehensive kinetic study of ethyl levulinate (EL) MPV reduction in 2-butanol, combined with in situ quantitative titration of the active sites by selective poisoning with alkylphosphonic acid titrants of Lewis acid sites during the reaction, reveals dramatic differences in the relative fraction of active sites (13–78% of total Zr) and turnover rates (>300-fold) among the studied catalysts. Mechanistically, the hydride shift invariably remains as the sole rate-limiting step, regardless of the catalyst; the free energy barriers in both first-order and zero-order kinetic regimes and kinetic isotope effects, however, differ significantly among the catalysts. Through mechanism-based rate equations and transition-state-theory treatments, we further delineate that the wide variations in enthalpic and entropic components not only suggest disparate transition state structures and energetics but also reflect varying adsorption thermodynamics that are influenced by both reactant coordination at and solvent restructuring near the active sites.
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