Journal of Physical Chemistry C
·
2024
·
IF 3.3
Zhi-Qiang Wang,Wanjun Guo,Shengchao Jia,Yaxuan Jing,Shiting Li,Yong Guo,Xiaohui Liu,Xue-Qing Gong,Yanqin Wang
The selective production of primary amines through reductive amination has received increasing attention due to their extensive applications, while efficient reductive amination is still challenging. Herein, a novel strategy was developed to realize the efficient reductive amination of carbonyl compounds with NH3 via d–d orbital coupling strategies in RuCo alloys. The designed series of RuCo alloy catalysts not only exhibited excellent performance in conversion of various substrates but also demonstrated universal applicability across different supports. The key role of RuCo alloy is its unique ability to effectively catalyze the ammonolysis of a Schiff base, the rate-determining step in reductive amination. Theoretical studies reveal that the d–d orbital coupling strategies break the five d orbital equivalent contributions of metal (Co or Ru) atoms, and the d orbitals primarily contribute through the dz2 and dx2-y2 orbitals of Ru and the dz2 orbital of Co on the RuCo(001) surface, which significantly driving the homolytic NH3 dissociation during the ammonolysis of the Schiff base. Furthermore, stable Co–H covalent bond species and RuCo-NH2 half-ionic and half-covalent bond species on the RuCo(001) surface were generated with lower energy levels. This work not only achieves efficient reductive amination but also provides an atomic orbital-level understanding of the d–d orbital coupling strategies for heterogeneous catalysis.
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Frontiers in Chemistry
·
2024
·
IF 3.8
Zhenghua Zhang,Yang Tian,Wenjun Gao,Yubin Hu,Liangping Luo,Lichang Lei,Shasha Shen,Dan Han
Objectives: Immune checkpoint inhibitors (ICIs) have demonstrated potential in inhibiting the growth of malignant pleural mesothelioma (MPM), and their efficacy is associated with the expression of programmed death-ligand 1(PD-L1). This study evaluated a PD-L1-targeted nanoprobe for detecting PD-L1 expression in a nude mouse model of malignant pleural mesothelioma (MPM).Methods: A PD-L1-binding peptide (WL-12) was conjugated with superparamagnetic iron oxide nanoparticles (SPIONs) to create the nanoprobe WL-12@Fe₃O₄. The nanoprobe’s stability, biotoxicity, targeting ability, and in vivo magnetic resonance (MR) imaging effects were assessed and compared to non-targeted Fe₃O₄ nanoparticles. ΔT2 values and PD-L1 expression were measured in H226 and MSTO-211H tumor tissues over 4 weeks to analyze correlations.Results: The WL-12@Fe₃O₄ nanoprobe demonstrated uniform distribution and a spherical shape, with a larger size (43.82 nm) and lower surface potential (−9.34 ± 0.54 mV) compared to Fe₃O₄ (32.67 nm, −20.20 ± 0.88 mV, P < 0.05). The XPS and FT-IR analysis results indicate the successful coupling of WL-12 with Fe3O4. It was well dispersed in serum and saline and showed no cytotoxicity or organ damage in vivo. The probe selectively accumulated in PD-L1-expressing MPM cells, especially MSTO-211H, and exhibited significantly higher uptake in high PD-L1-expressing H460 cells (930.22 ± 11.75 ng/mL) compared to low PD-L1-expressing A549 cells (254.89 ± 17.33 ng/mL, P < 0.05). Tumor iron levels in the WL-12@Fe₃O₄ group were significantly elevated (141.02 ± 17.33 μg/g) compared to controls (36.43 ± 3.56 μg/g, P < 0.05), with no significant differences in other organs (P > 0.05). The T2 values of H226 and MSTO-211H tumors decreased after probe injection, with ΔT2 values significantly higher in the targeted group than the nontargeted group (P < 0.05). ΔT2 values increased over 4 weeks, correlating strongly with PD-L1 expression (P < 0.05).Conclusion: The PD-L1-targeted nanoprobe with MRI is a promising tool for noninvasive, real-time assessment of PD-L1 expression in MPM.
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AQUACULTURE
·
2025
·
IF 3.9
Yao Wang,Mengmeng Wang,Zhiyang Lin,Guangshuo Wang,Yunlong Qin,Mingzhu Liu,Fei Ling,Haifeng Jiang,Tianqiang Liu,Gaoxue Wang
Micropterus salmoides rhabdovirus (MSRV) is a highly pathogenic rhabdovirus that has caused significant economic losses in the aquaculture industry of largemouth bass. To date, there is no approved treatment for MSRV infection. In order to address this urgent need, virtual screening of the natural product monomer compound library targeting MSRV glycoprotein was conducted and the antiviral activity of 13 natural compounds identified in the screening was studied. Among these compounds, Aloe emodin (AE) exhibited high binding affinity and antiviral activity, inhibiting MSRV replication in grass carp ovary (GCO) cells with a half-maximal inhibitory concentration (IC 50 ) of 2.55 μM. Additionally, viral titers and cytopathic effects (CPE) were significantly reduced in the presence of AE. AE was demonstrated to directly destroy MSRV virions and inhibit their adsorption to GCO cells according to ultracentrifugation assay and viral binding assay. In vivo studies demonstrated that AE injection increased the survival rate of MSRV-infected largemouth bass by 63.3 %, which was 46.7 % higher than that of the virus group. RT-qPCR and pathological tissue section results demonstrated that AE treatment could significantly reduce viral loads in the liver, spleen, and kidney on days 1, 4, and 7 post-infection, and AE effectively mitigated tissue damage caused by MSRV infection. Circular dichroism (CD) spectroscopy and Isothermal titration calorimetry (ITC) showed that AE induced changes in the secondary structure of the MSRV glycoprotein and exhibited high affinity for the glycoprotein (Kd = 2.803 × 10 −5 M, ΔG = −25.99 kJ/mol). These results suggested that AE was a natural product with potent anti-MSRV activity through direct targeting of the glycoprotein.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
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IF 4.9
Dongxu Zhang,Xin Wang,Cheng Liu,Lechun Song,Huiyuan Li,Qiyu Huang,Jianfeng Zhang
Hydrate formation is one of the major flow assurance issues for the subsea multiphase pipelines. The effects of the interaction between heavy fractions of crude oil components on hydrate behaviors are still not well understood. In this study, the effects of resins on hydrate formation behaviors in asphaltene-containing emulsions were investigated using a high-pressure reactor apparatus. The results indicated that both resins and asphaltenes inhibited hydrate nucleation and increased the induction time. Furthermore, considerable synergistic effects of asphaltenes and resins on the hydrate formation behaviors were discovered in the water-in-oil emulsions, depending on the aggregation state of asphaltenes. The addition of resins was observed to disperse the asphaltene aggregates significantly and enhance the inhibitory effect of asphaltenes on hydrate nucleation. Additionally, the calculated results of gas consumption showed that the presence of resins can decrease the growth rate of hydrates in the asphaltene-containing emulsions. A potential mechanism was presented to illustrate how resins affect hydrate formation in an emulsion with varying asphaltene aggregation states. These findings offer a better knowledge of the synergistic effects between the heavy components of resins and asphaltenes and have potential application in the hydrate management of crude oil pipelines.
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JOURNAL OF SEPARATION SCIENCE
·
2024
·Vol. 47
·期 11
·2400113
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IF 2.8
Masoumeh Firouzy,Alireza Ghiasvand,Payman Hashemi
An amide-based covalent organic framework (COF) was successfully synthesized using the reaction between 1,3,5-trimesoyl chloride and ethylenediamine. The structure and morphology of the COF were characterized using Fourier-transform infrared spectra, nuclear magnetic resonance spectroscopy, X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and Brunauer-Emmett-Teller surface area analysis. The COF was employed as a solid-phase extraction adsorbent for the sampling and preconcentration of chlorophenols from industrial wastewater samples prior to high-performance liquid chromatography with ultraviolet detection. The experimental parameters influencing the extraction efficiency including type and volume of eluent solvent, sample solution volume, salt concentration, sample flow rate, and sample solution pH were investigated and optimized using a response surface methodology employing Box-Behnken-design. Under optimized conditions, calibration curves exhibited good linearities over the range of 0.003–10 µg/mL with determination coefficients (R 2 ) ranging from 0.9982 to 0.9999. The method's limits of detection ranged from 0.001 to 0.01 µg/mL. Good repeatability was achieved with relative standard deviations below 4.7%. The developed procedure utilizing the COF adsorbent was successfully applied to determine chlorophenols accurately and precisely in various industrial wastewater samples.
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PHYSICS OF FLUIDS
·
2024
·Vol. 36
·期 1
·
IF 4.1
Yu Jia-Jia,Jiang Lu-Yang,Huang Li,Li Gu-Yuan,Bake Maitiniyazi,Li You-Rong
Hydrodynamic cavitation, which occurs when the local pressure is below the saturated vapor pressure in hydrodynamic flow, is ubiquitous in fluid dynamics and implicated in a myriad of industrial and biomedical applications. Although extensively studied in isotropic liquids, corresponding investigations in anisotropic liquids are largely lacking. In this paper, the hydrodynamic cavitation in the bluff body bypass flow of nematic liquid crystal 5CB in the microchannel is experimentally investigated. By 5CB, we mean the thermotropic liquid crystal 4′-pentyl-4-biphenylcarbonitrile. When the Reynolds number is in the range of 3 × 10 −4 < Re < 1.2 × 10 −3 , a special flow phenomenon behind the bluff body is observed, namely, the disclination loop. The critical Reynolds number of cavitation inception varies with the shape of the bluff body, while the lowest value corresponds to the triangular bluff body. The hydrodynamic cavitation occurs in the Stokes flow regime with the Reynolds number significantly lower than 0.1 for all bluff bodies. There is a close relation between the oscillation behavior of cavitation domains and the structure of the bluff body. In addition, the pressure difference between the inlet and outlet of the microchannel shows linear relation with the Reynolds number rather than the quadratic relation for isotropic fluids, which proves the presence of shear thinning in the flow of nematic liquid crystals. The study in this paper on the hydrodynamic cavitation of nematic liquid crystal can broaden the research on providing new approaches for the enhancement of fluid mixing and heat transfer in microfluidic chips.
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Heritage Science
·
2024
·Vol. 12
·期 1
·1-13
·
IF 2.6
Wu Huihua,Xie Quanhua,He Yuanyuan,He Xuefeng,Zhou Yuan,Liu Yang,Liu Yufei,Liu Yang,Wan Bo,Zhong Nianbing
Temperature changes during the chemical corrosion of stone cultural relics affect the condensation and evaporation of water and chemical reactions between soluble substances and corrosive solutions. This ultimately leads to changes in the internal structure and composition of the artifacts, which in turn lead to changes in the microstrain of cultural relics. To obtain in-situ real-time information on changes in the temperature and microstrain of stone cultural relics during chemical corrosion damage, a fiber Bragg grating (FBG) detection system was developed. The detection principle for the temperature and microstrain of sandstone was provided. Thermal field emission scanning electron microscopy, X-ray diffraction, and mercury intrusion porosimetry were used to characterize the surface morphology, composition, and pore structure of the sandstone samples, respectively. The temperature and microstrain changes of the sandstone samples under deionized water with different acidic/alkaline and salt solutions and at different temperatures were examined online in situ using the FBG measurement system. The results indicate that the dissolution of sandstone in the acidic solution (H 2 SO 4 and NaHSO 4 ) resulted in an exothermic chemical reaction as well as the dissolution of sandstone in the neutral salt solution (Na 2 SO 4 ) and alkaline solution (NaOH and Na 2 CO 3 ) led to material conversion and exothermic chemical reaction; the deionization reaction belongs to the dissolution reaction. The NaHSO 4 solution caused the most serious corrosive disease on the sandstone surface. When the temperature of the NaHSO 4 solution was 60 °C, the temperature and microstrain of the sandstone reached 63.9 °C and 253.6 με, respectively. The results of this study can support the research of revealing the corrosion mechanism of sandstone in different environments.
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CARBON
·
2024
·
IF 10.5
Yongqing Shen,Peizhi Liu,Yangrui Li,Jianghong Wu,Yanhui Song,Junjie Guo
The structural stability of supported metal nanoparticles determines the activity and longevity of heterogeneous catalysts. Unfortunately, the chemical/thermal working environment inevitably accelerates metal sintering to larger crystallites that leads to the degradation of catalytic performance. Here, we demonstrate that the distribution of defects in carbon support as an inherent parameter plays a crucial role in catalyst sintering. Based on in-situ transmission electron microscopy studies, the strong metal-support interaction between platinum (Pt) nanoparticles and defect-rich graphene nanoflakes largely suppresses metal sintering up to 700 °C. Particularly, the optimal carbon support can be achieved in the annealing process, in which the mass transfer and charge transport can be enhanced by accurately manipulating the distribution of defects in carbon matrix and graphitization degree. It is worth noting that the screened Pt/GNs-300 exhibits impressive oxygen reduction reaction performance with high half-wave potential (0.91 V), mass activity (108.1 A g –1 Pt ) and excellent stability. By its ascendancy in ORR, the Pt/GNs-300 exhibits a high open-circuit voltage of 1.41 V and a maximum power density of 198.6 mW cm −2 in Zn-air battery, implying its brilliant practicability. This work paves a pathway for achieving sinter-resistant metal-loaded catalysts in energy electrocatalysis.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Lingjuan Tang,Zhiyao Zhang,Ling Sun,Xu Gao,Xinyue Zhao,Xinru Chen,Xingyu Zhu,Aixue Li,Lijun Sun
Abscisic acid (ABA) plays an important regulatory role in plants. It is very critical to obtain the dynamic changes of ABA in situ for botanical research. Herein, coupled with paper-based analysis devices, electrochemical immunoelectrodes based on disposable stainless steels sheet were developed for ABA detection in plants in situ. The stainless steel sheets were modified with carbon cement, ferrocene-graphene oxide-multi walled carbon nanotubes nanocomposites, and ABA antibodies. The system can detect the ABA in the range of 1 nM to 100 μM, with a limit of detection of 100 pM. The ABA content in tomato leaves under high salinity was detected in situ. The trend of ABA changes was similar to the expression of SlNCED1 and SlNCED2. Overall, this study offers an approach for in situ detection of ABA in plants, which will help to study the regulation mechanism of ABA in plants and to promote the development of precision agriculture.
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ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Cheng Qu,Yuchuang Geng,Zhongxiang Ding,Yuzhu Li,Hao Jiang,Mengke Su,Honglin Liu
A feedback inhibition effect of high autoinducer levels on metabolite secretion in Chromobacterium subtsugae (C. subtsugae) was evidenced by in situ spatiotemporal surface-enhanced Raman spectroscopy (SERS) profiling. The hierarchical hydrophobic plasmonic array in agar medium is structured by oil/water/oil (OL/W/OH) triphasic interfacial self-assembly. The hydrophobic layer acts as a “door curtain” to selectively permit adsorption of a quorum sensing (QS)-regulated fat-soluble metabolite, i.e., violacein (Vio), and significantly blocks nonspecific adsorption of water-soluble proteins, etc. The SERS profiling clearly evidences that the diffusion of N-hexanoyl-l-homoserine lactone (C6-HSL) in agar medium quickly triggers the initial synthesis of Vio in C. subtsugae CV026 but surprisingly inhibits the intrinsic synthesis of Vio in C. subtsugae ATCC31532. The latter negative response might be related to the VioS repressor of ATCC31532, which negatively controls violacein production without influencing the expression of the CviI/R QS system. Moreover, two sender–receiver systems are constructed by separately coculturing CV026 or ATCC31532 with Hafnia alvei H4 that secretes large amounts of C6-HSL. Expectedly, the cocultivation similarly triggers the initial synthesis of Vio in CV026 but seems to have a quite weak negative effect on the intrinsic synthesis in ATCC31532. In fact, the negative regulation in ATCC31532 might be affected by a diffusion-dependent concentration effect. The H4 growth and its secretion of C6-HSL are a slow and continuous process, thereby avoiding the gathering of local high concentrations. Overall, our study put forward an in situ SERS strategy as an alternative to traditional bioluminescent tools for highly sensitively analyzing the spatiotemporal communication and cooperation in live microbial colonies.
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MOLECULES
·
2024
·Vol. 29
·期 8
·1703
·
IF 4.2
Meihua Liang,Yong Yan,Jiaxuan Yang,Xiaodong Liu,Rongrong Jia,Yuanyuan Ge,Zhili Li,Lei Huang
Microelectromechanical systems (MEMS) gas sensors have numerous advantages such as compact size, low power consumption, ease of integration, etc., while encountering challenges in sensitivity and high resistance because of their low sintering temperature. This work utilizes the in situ growth of Zeolitic Imidazolate Framework-8 (ZIF-8) followed by its conversion to N-doped ZnO. The results obtained from scanning electron microscopy (SEM) and transmission electron microscopy (TEM) indicate that the in situ derivation of ZIF-8 facilitates the adhesion of ZnO particles, forming an island-like structure and significantly reducing the interfaces between these particles. Furthermore, powder X-ray diffraction (XRD) analysis, elemental mapping, and X-ray photoelectron spectroscopy (XPS) analysis confirm the conversion of ZIF-8 to ZnO, the successful incorporation of N atoms into the ZnO lattice, and the creation of more oxygen vacancies. The ZIF-8-derived N-doped ZnO/MEMS sensor (ZIF (3)-ZnO/MEMS) exhibits remarkable gas sensitivity for ethanol detection. At an operating temperature of 290 °C, it delivers a substantial response value of 80 towards 25 ppm ethanol, a 13-fold enhancement compared with pristine ZnO/MEMS sensors. The sensor also exhibits an ultra-low theoretical detection limit of 11.5 ppb to ethanol, showcasing its excellent selectivity. The enhanced performance is attributed to the incorporation of N-doped ZnO, which generates abundant oxygen vacancies on the sensor’s surface, leading to enhanced interaction with ethanol molecules. Additionally, a substantial two-order-of-magnitude decrease in the resistance of the gas-sensitive film is observed. Overall, this study provides valuable insights into the design and fabrication strategies applicable to high-performance MEMS gas sensors in a broader range of gas sensing.
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Foods
·
2024
·Vol. 13
·期 10
·1561
·
IF 4.7
Qiaoyi Zhou,Jinjing Gao,Xueyan Sun,Yicheng Liang,Minqi Ye,Dongxia Liang,Caijin Ling,Binghu Fang
Tea plants have a long cultivation history in the world, but there are few studies on polysaccharides from fresh tea leaves. In this study, tea polysaccharides (TPSs) were isolated from fresh tea leaves. Then, we investigated the characteristics of TPSs during in vitro simulated digestion and fermentation; moreover, the effects of TPSs on gut microbiota were explored. The results revealed that saliva did not significantly affect TPSs’ molecular weight, monosaccharide composition, and reducing sugar content, indicating that TPSs cannot be digested in the oral cavity. However, TPSs were partially decomposed in the gastrointestinal tract after gastric and intestinal digestion, resulting in the release of a small amount of free glucose monosaccharides. Our in vitro fermentation experiments demonstrated that TPSs are degraded by gut microbiota, leading to short-chain fatty acid (SCFA) production and pH reduction. Moreover, TPSs increased the abundance of Bacteroides, Lactobacillus, and Bifidobacterium but reduced that of Escherichia, Shigella, and Enterococcus, demonstrating that TPSs can regulate the gut microbiome. In conclusion, TPSs are partially decomposed by gut microbiota, resulting in the production of SCFAs and the regulation of gut microbiota composition and function. Therefore, TPSs may be used to develop a prebiotic supplement to regulate the gut microbiome and improve host health.
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