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Highly selective catalytic oxidation of methane to methanol using Cu-Pd/anatase

ENERGY & ENVIRONMENTAL SCIENCE 2024年第23期17卷 9122-9133页

作者： Wang, Liqun Jin, Jingting Li, Wenzhi Li, Cunshuo Zhu, Leyu Zhou, Zheng Zhang, Lulu Zhang, Xia Yuan, Liang Univ Sci & Technol China Dept Thermal Sci & Energy Engn Lab Clean Low Carbon Energy Hefei 230023 Peoples R China Hefei Comprehens Natl Sci Ctr Inst Energy Hefei 230031 Peoples R China Anhui Univ Sci & Technol Sch Chem Engn Huainan 232001 Peoples R China Anhui Univ Sci & Technol Natl & Local Joint Engn Res Ctr Precis Coal Min Huainan 232001 Peoples R China

Direct conversion of methane into high value-added products is of great practical significance. The synergistic effect in catalysts with dual-active components show potential to increase the methanol yield and selectivity. In this work, Cu-Pd/anatase is in situ generated and exhibits a relatively high methanol yield rate of similar to 31 800 mu mol gcat-1 h-1 and near-exclusive selectivity of liquid products (methanol). The reaction mechanism behind the heterogeneous catalysis process has been investigated. It is confirmed that copper ions hold the ability to produce hydrogen peroxide which can be further promoted by anatase. Chlorine ions can promote the stable adsorption of CO and the formation of *CH3 intermediates, facilitating high activity and selectivity for methanol production. Pd and Cu cooperatively dissociate methane, which promotes the formation of key configuration metal-CH3. The (center dot)CH3 intermediate desorption will be facilitated on Cu-Pd/anatase through the manner of electron regulation, which is proved by the combination of density functional theory calculations and in situ infrared spectroscopy. Methanol is formed when a (center dot)CH3 is desorbed from a copper site and combines with a hydroxyl radical. Cu-Pd/anatase is highly efficient in converting methane to methanol, exhibiting a relatively high methanol yield rate of similar to 31 800 mu mol gcat-1 h-1 and near-exclusive selectivity of liquid products (methanol).

关键词： Catalytic oxidation

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Improvement of mechanical and barrier properties of PLA films via coated antimicrobial polyurethane

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PROGRESS IN ORGANIC COATINGS 2025年 204卷

作者： Liu, Zhixiu Wang, Junjie Wang, Haili Dong, Xiaoyu Du, Jinghua Cheng, Sheng Ding, Yunsheng Hefei Univ Technol Sch Chem & Chem Engn Dept Polymer Sci & Engn Hefei 230009 Anhui Peoples R China Anhui Prov Key Lab Adv Funct Mat & Devices Hefei 230009 Anhui Peoples R China Anhui Med Coll Hefei 230009 Anhui Peoples R China

High performance and environmentally friendly films for food packaging play an important role in improving food safety and protecting the environment after discarding. In this paper, bio-based polycarbonate diol (PCDL), isophorone diisocyanate (IPDI), isophorone diamine (IPDA), N-methyldiethanolamine (MDEA) and 1,6-dibromohexane were employed as main raw materials to prepare a series of polyurethanes with quaternary ammonium groups (QPUs). Subsequently, a bio-based coated film named as PLA-QPU was prepared by uniformly bar-coating the polyurethane slurry onto one surface of the PLA film. The mechanical testing results exhibit that PLA-QPU film has high tensile strength (63 MPa) and toughness (196 MJ/m3), and the PLA-QPU film is more stretchable with elongation at break increasing from 7 % to 47 % in comparing with uncoated PLA film. The antimicrobial testing results show that the antimicrobial ratio of the QPU film against E. coli and S. aureus was 91 % and 88 %, respectively. The water vapor barrier properties testing results reveal that PLA-QPU coated film has a significant water vapor barrier property (57.8 g/m2 & sdot;day). The PLA-QPU coated film was evaluated for packaging cherry tomatoes and it maintained fruit freshness, texture, and visual quality effectively for up to 16 days. Therefore, the high-performance PLA-QPU coated film shows great promise as sustainable in food preservation.

关键词： Polyurethane coating PLA Mechanical properties Antimicrobial properties Barrier properties

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Combined multi-omics approach to analyze the flavor characteristics and formation mechanism of gabaron green tea

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FOOD CHEMISTRY 2024年 445卷 138620页

作者： Huang, Dongzhu Zheng, Dongqiao Sun, Chenyi Fu, Maoyin Wu, Yuhan Wang, Hong Yu, Jieyao Yang, Yunqiu Li, Yeyun Wan, Xiaochun Chen, Qi Anhui Agr Univ Sch Tea & Food Sci Technol State Key Lab Tea Plant Biol & Utilizat Hefei 230036 Peoples R China Anhui Agr Univ Sch Tea & Food Sci & Technol Key Lab Food Nutr & Safety Anhui Engn Lab Agroprod Proc Hefei 230036 Peoples R China

Gabaron green tea (GAGT) has unique flavor and health benefits through the special anaerobic treatment. However, how this composite processing affects the aroma formation of GAGT and the regulatory mechanism was rarely reported. This study used nontargeted metabolomics and molecular sensory science to overlay screen differential metabolites and key aroma contributors. The potential regulatory mechanism of anaerobic treatment on the aroma formation of GAGT was investigated by transcriptomics and correlation analyses. Five volatiles: benzeneacetaldehyde, nonanal, geraniol, linalool, and linalool oxide III, were screened as target metabolites. Through the transcriptional-level differential genes screening and analysis, some CsERF transcription factors in the ethylene signaling pathway were proposed might participate the response to the anaerobic treatment. They might regulate the expression of related genes in the metabolic pathway of the target metabolites thus affecting the GAGT flavor. The findings of this study provide novel information on the flavor and its formation of GAGT.

关键词： Anaerobic treatment Volatile compounds Nontargeted metabolomics Molecular sensory science Transcriptomics Ethylene signaling

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Persistent oscillations in correlation function: from the perspective of past quantum states

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PHYSICA SCRIPTA 2025年第1期100卷 015105-015105页

作者： Xu, Qing Shen, Xiaobo Yu, Haijun HuaiNan Normal Univ Sch Elect Engn Huainan 232038 Anhui Peoples R China

The recent past quantum state formalism ( 2013 Phys. Rev. Lett. 111,160401) indicates that the outcome probability of the measurement performed on a quantum system at time t shows dependence on the measurement events recorded until that time, and is also revised by the outcomes acquired after time t . We apply the past quantum state formalism to calculate the three-time correlation function of a radiation fi eld and to analyze the conditional dynamics on the pre- and postselection by the fi rst and last detection events. The persistent oscillations in the three-time fi eld correlation function, which cannot be well understood by the usual quantum regression theorem, are straightforwardly explained by the probabilistic knowledge of the past and the future through the past quantum state reasoning.

关键词： correlation function past quantum state formalism quantum regression theorem quantum measurement

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Allelopathic effects of gramineous plant extracts on Spirogyra communis growth: insights from Zizania latifolia, Phragmites australis, and Digitaria sanguinalis

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ENVIRONMENTAL TECHNOLOGY 2025年 1-12页

作者： Xia, Ting Zhang, Ruyan Zhu, Ling Yue, Mingyang Bai, Jianyuan Zhao, Fei Nanjing Tech Univ Coll Urban Construct Puzhu Rd 30 Nanjing 211816 Peoples R China

The overgrowth of algae, such as Spirogyra communis (S. communis), has emerged as a significant ecological issue, exacerbated by the increasing problem of eutrophication in aquatic ecosystems. S. communis overgrowth can result in the deterioration of water quality and a decline in biodiversity. To mitigate the proliferation of S. communis under conditions of water eutrophication, the inhibitory effects of ethanol extracts from gramineous plants, Zizania latifolia (Z. latifolia), Phragmites australis (P. australis), and Digitaria sanguinalis (D. sanguinalis) on the growth of S. communis were investigated. The results demonstrated that the ethanol extract of D. sanguinalis at a concentration of 10 g/L exhibited the best inhibitory effect. The D. sanguinalis ethanol extracts significantly reduced the chlorophyll a (Chl-a) content and soluble protein levels in the algal cells, leading to severe oxidative damage and triggering antioxidant responses. The structure of algal cells was compromised, resulting in their inhibited growth or even death. Gas chromatography-mass spectrometry (GC-MS) analysis identified fatty acids and terpenoids as the primary allelopathic compounds responsible for algal inhibition in the D. sanguinalis ethanol extracts. In addition, the results of the ecotoxicity test indicated that at a concentration of 10 g/L, which was used to inhibit the growth of S. communis, the ethanol extract of D. sanguinalis posed less ecological risk to aquatic organisms, including zebrafish and Vallisneria natans (V. natans). Based on these findings, the ethanol extract of D. sanguinalis shows promising potential as an algal inhibitor.

关键词： Allelopathic effect Spirogyra communis Digitaria sanguinalis ethanol extract algal inhibition mechanism

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Study on Microstructure and Low-Temperature Impact Toughness in Coarse Grain Heat-Affected Zone of EH460 Steel

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STEEL research INTERNATIONAL 2025年第2期96卷

作者： Zhang, Pengyan Yang, Yi Huang, Zhenyi Yue, Qiang Zhang, Ke Anhui Univ Technol Sch Met Engn Maanshan 243000 Anhui Peoples R China

Herein, the effects of peak temperature on the microstructure and low-temperature impact toughness of coarse grain heat-affected zone (CGHAZ) of EH460 steel are investigated by Gleeble simulation welding. The low-temperature impact toughness of CGHAZ decreases with the increase of peak temperature. With the increase of peak temperature, the microstructure of CGHAZ gradually changes from bainite to a mixed structure composed of bainite, intragranular ferrite, side lath ferrite, and a small amount of grain boundary ferrite. The inclusions size decreases as the peak temperature increases. The existence of large-sized inclusions is conducive to the initiation and propagation of cracks, reducing the low-temperature impact toughness of the material. Herein, the effect of peak temperature on the microstructure and low-temperature impact toughness of coarse grain heat-affected zone (CGHAZ) is investigated by Gleeble simulation welding. As the peak temperature increases, the microstructure changes from bainite to mixed structure, the grain size increases and the inclusions size decreases (all diameters are greater than 3 mu m), which reducing the low-temperature impact *** (c) 2024 WILEY-VCH GmbH

关键词： EH460 steels Gleeble thermal simulators inclusions low-temperature impact toughnesses

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Metal-organic framework assisted preparation of α-Fe2O3 for selective catalytic reduction of NOX with NH3

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JOURNAL OF SOLID STATE CHEMISTRY 2024年 329卷

作者： Hu, Yuting Cheng, Ting Jiang, Zhaozhong Qin, Kai He, Han Zhu, Chengzhu Hefei Univ Technol Sch Resource & Environm Engn Hefei 230009 Peoples R China Hefei Univ Technol Inst Atmospher Environm & Pollut Control Hefei 230009 Peoples R China Hefei Univ Technol Anhui Higher Educ Inst Key Lab Nanominerals & Pollut Control Hefei 230009 Peoples R China Low Temp Denitrat Engn Res Ctr Anhui Prov Hefei 230001 Peoples R China

Fe-MIL-101-NH2 was prepared by solvothermal method with ferric nitrate and 2-Aminoterephthalic Acid (DBC-NH2), and Fe-MIL-101-NH2 as precursor was calcined to prepare alpha-Fe2O3 catalyst. The optimum synthesis condition and the NO conversion efficiency of alpha-Fe2O3 were systematically investigated, and its crystallinity, micro-morphology and surface acidity were characterized. The results showed that alpha-Fe2O3 over calcination at 400 degrees C for 1 h had excellent catalytic activity, SO2 tolerance, water resistance, and stability. When an initial NO concentration of 500 ppm, the gas hourly space velocity (GHSV) of 35000 h-1, and a reaction temperature of 350 degrees C, the NO conversion efficiency of alpha-Fe2O3 remained above 90 %. The crystal structure of the catalyst was alpha-Fe2O3 which retained the original octahedral morphology of Fe-MIL-101-NH2 and increased a lot of new pores, leading to more abundant Lewis acid sites for promoting NO conversion efficiency.

关键词： Nitric oxide Denitration Fe-MIL-101-NH2 NH3-SCR Stability

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Synthesis of phenol formaldehyde resin (PFR) based fluorescence resonance energy transfer (FRET) composites for double channel detection of latent fingerprints

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RSC ADVANCES 2024年第22期14卷 15647-15655页

作者： Yang, Ping Shi, Tingfei Liu, Zhiyuan Wu, Siying Cheng, Yuqi Li, Kuiliang Zhao, Hong Anhui Univ Sci & Technol Sch Chem Engn Huainan 232001 Anhui Peoples R China

A reversible two-channel fluorescent nanocomposite with fluorescence resonance energy transfer (FRET) effect was designed for the development, analysis, and characterization of latent fingerprints (LFPs). For the construction of the FRET probe, a core of mesoporous silicas (MSNs) were used to encapsulate the organic dye rhodamine 6G (RhD-6) as an acceptor, while green-emitting monodisperse phenolic resin nanoparticles (PFR NPs) were selected as a donor. The up-conversion material (UC) of NaYF4:Yb,Er was synthesized using a simple hydrothermal method, and the MSNs-RhD-6/PFR (PRM) was electrostatically adsorbed onto the UC nanoparticles using a layer-by-layer method to obtain MSNs-RhD-6/PFR-UC (PMU). Compared to ordinary single-channel materials, PMU can be excited by different light sources (365 nm UV/980 nm laser) and its fluorescence can be reversibly switched between yellow and green, demonstrating excellent light reversibility. The PMU composites were successfully used to visualize and detect LFPs on various substrate surfaces using a simple powder coating method. Due to the existing FRET effect and dual-channel characteristics, this composite material displays excellent contrast, outperforming commercially available products for wider applicability. Even on complex backgrounds and after aging or washing treatments, it still clearly recognizes fingerprints in first-, second-, and third-level details, showing its great potential in latent fingerprint detection. A reversible two-channel fluorescent nanocomposite with fluorescence resonance energy transfer (FRET) effect was designed for the development, analysis, and characterization of latent fingerprints (LFPs).

关键词： Synthesis (chemical)

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A novel process of the bulged tube manufactured by laser-induced shock wave

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JOURNAL OF MATERIALS PROCESSING TECHNOLOGY 2024年 327卷

作者： Zhang, Xingquan Hu, Rui Fang, Jinxiu Zuo, Lisheng Yin, Yuande Wang, Huiting Li, Shengzhi Minist Educ Key Lab Green Fabricat & Surface Technol Adv Met Maanshan 243002 Anhui Peoples R China Anhui Univ Technol Sch Mech Engn Maanshan 243002 Anhui Peoples R China

This study presents a novel tube-forming method that employs a pulsed laser as a stamping tool to form a smalldiameter bulged tube, which could not be easily obtained via conventional tube forming. A mechanism for the dynamic forming of a laser-induced micro-bulge was introduced, and an analytical model was developed to analyze the micro-bulging deformation induced by single laser irradiation. A finite element model was also built to simulate shock wave propagation and the dynamic progress of tube expansion. A series of validated deformation experiments were conducted. The study findings showed that the laser-induced shock wave diffused rapidly, causing the tube to expand at the shocked zone. When subjected to a one-shot laser shock, the tube underwent deformation with micro-bulging. The application of a confining layer was found to be beneficial for tube deformation. The magnitude of the tube deformation increased with the increase of laser shots. Moreover, as the laser pulse energy increased, the bulge deformation of the tube also increased. The proposed process provides an efficient alternative to form the expansion tube with a smaller diameter in the future.

关键词： Tube Laser-induced shock wave Radial expansion Bulged deformation

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Synergistic effect of Cu and Fe on g-C3N4 for selective oxidation of methane to C1 products

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MOLECULAR CATALYSIS 2024年 562卷

作者： Zhou, Zheng Miao, Meng Li, Wenzhi Jin, Jingting Wang, Liqun Zhang, Lulu Yuan, Liang Univ Sci & Technol China Lab Clean Low Carbon Energy Hefei 230023 Peoples R China Hefei Normal Univ Sch Phys & Mat Engn Hefei 230601 Peoples R China Anhui Univ Sci & Technol Natl & Local Joint Engn Res Ctr Precis Coal Min Huainan 232001 Peoples R China

The selective conversion of methane is a significant but difficult challenge. We reported a CuFe bimetallic catalyst supported by g-C3N4 for the catalytic oxidation of methane to oxygenated C1 products. Using H2O2 as the oxidant, Cu0.4Fe0.3-C3N4 catalyst had a C1 yield of 8231 mu mol center dot gcat almost all of the liquid phase products were target C1 products. The methanol selectivity on CuFe-C3N4 was 44.5 %, comparing with 20.2 % methanol selectivity on Cu-C3N4. The formation of a Cu-O-Fe site on the CuFe-C3N4 was confirmed by in situ DRIFTS and 57Fe Mossbauer spectroscopy. This Cu-O-Fe site was responsible for the improved catalyst performance. DFT calculations illustrated that at the Cu-O-Fe site, H2O2 dissociated into two center dot OH radicals instead of center dot H and center dot OOH radicals as it did at the Cu-O-Cu site. The center dot OH radicals combined with the center dot CH3 radicals from the CH4 molecules to form methanol. These findings provided valuable insights into the rational design of active sites on carbon nitride materials.

关键词： Methane oxidation Diatomic active sites DFT calculations Methanol

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