Materials
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2023
·Vol. 16
·期 4
·1568
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IF 3.4
Feng Wang,Yaoqi Gu,Jianrui Zha,Shuya Wei
Ca(OH)2nanoparticles are effective materials for cultural heritage restoration, hazardous substance absorption and photocatalyst. However, many methods are complex, and the particle sizes are usually above 80–100 nm, involving mediocre efficacy for application in the stone restoration field. In this work, Nano Ca(OH)2with diameters less than 70 nm and composited with Graphene Quantum Dots (GQDs) were successfully synthesized in aqueous media. The morphology and structure of the nanoparticles were investigated with TEM, HRTEM, XRD, Raman and FTIR. The particle size distribution and relative kinetic stability of the Ca(OH)2in ethanol were performed using a laser particle size analyzer and spectrophotometer. Firstprinciple calculations based on the spin-polarized density functional theory (DFT) were carried out to study the reaction process and combination model. The nanoparticles, as prepared, are composed of primary hexagonal crystals and high ammoniated precursors, which have a positive effect on reducing the grain size, and interacted with the GQDs hybrid process. According to the First-principle calculations results, the energy variation of the whole reaction process and the bonding mode between Ca(OH)2and GQDs can be understood better.Keywords:Ca(OH)2;Graphene Quantum Dots;DFT;complex;nanoparticles
研究领域:
材料科学
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化学
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Xu Tang,Wenjing Shen,Dongyi Li,Binrong Li,Yemei Wang,Xianghai Song,Zhi Zhu,Pengwei Huo
The novel Co-doping combined with mesoporous g-C 3 N 4 -based photocatalyst was constructed, and the Co-CN showed impressive photocatalytic reduction CO 2 activity. Employing the DFT computation, we discussed the possible Co doping sites on g-C 3 N 4 framework, as well as the effects of band gaps, optical properties , and various densities of state (DOS) on photocatalytic activity. The adsorption energy calculation proved that the substitution and interstitial doping Co atoms in g-C 3 N 4 crystal unit cell was the stable configuration. The coexistence substitution and substitution the monolayer g-C 3 N 4 showed serious deformation. It indicated that the introduction of Co atoms leads g-C 3 N 4 molecular orbital redistribution and Co tends to occupy the conduction band, due to its weak electronegativity. Moreover, the DFT and experiment results pointed out that the doped-Co narrowed g-C 3 N 4 bandgap and increased light absorption from 450 to 800 nm, the improved charge carrier separation efficiency was originated from Co atom the unfilled 4 f and the empty 5d orbital act as electron capturing center. This research indicates the availability of transition metal g-C 3 N 4 with conducive photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Mengyuan Zhang,Xiaolan Duan,Ying Gao,Shuangshuang Zhang,Xiaoyan Lu,Kongliang Luo,Jian Ye,Xiaopeng Wang,Qiang Niu,Pengfei Zhang,Sheng Dai
Tuning surface oxygen vacancies is important for oxide catalysts. Doping elements with different chemical valence states or different atomic radii into host oxides is a common method to create oxygen vacancies. However, the concentration of oxygen vacancies in oxide catalysts is still limited to the amount of foreign dopants that can be tolerated (generally less than 10% atoms). Herein, a principle of engineering the configurational entropy to tune oxygen vacancies was proposed. First, the positive relationship between the configuration entropy and the formation energy of oxygen vacancies (Eov) in 16 model oxides was estimated by a DFT calculation. To verify this, single binary oxides and high-entropy quinary oxides (HEOs) were prepared. Indeed, the concentration of oxygen vacancies in HEOs (Oβ/α = 3.66) was higher compared to those of single or binary oxides (Oβ/α = 0.22–0.75) by O1s XPS, O2-TPD, and EPR. Interestingly, the reduction temperatures of transition metal ions in HEOs were generally lower than that in single-metal oxides by H2-TPR. The lower Eov of HEOs may contribute to this feature, which was confirmed by in situ XPS and in situ XRD. Moreover, with catalytic CO/C3H6 oxidation as a model, the high-entropy (MnCuCo3NiFe)xOy catalyst showed higher catalytic activity than single and binary oxides, which experimentally verified the hypothesis of the DFT calculation. This work may inspire more oxide catalysts with preferred oxygen vacancies.
研究领域:
材料科学
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催化化学
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理论计算
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PubMed
高影响因子
Water
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2023
·Vol. 15
·期 10
·1920
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IF 3.4
Yishu Cai,Fan Chen,Lingfang Yang,Lin Deng,Zhou Shi
Nanoplastics have gradually become a concern due to the wide use of plastics. Nanoplastics in aqueous phase can be exposed to users through water supply networks and cannot be efficiently removed by conventional water treatment processes. This work studied the degradation of polystyrene nanoplastics (PS-NP) by two commonly used advanced oxidation systems: UV/NaClO and UV/peroxymonosulfate (PMS). Results showed that almost no turbidity was detected in the PS-NP solution (5.00 mg/L) after treated by both UV/NaClO and UV/PMS for 360 min, suggesting the excellent turbidity removal ability. Yet, scanning electron microscope (SEM) and total organic carbon (TOC) removal tests demonstrated that PS-NP could not be completely degraded by UV/NaClO. The mineralization rate using UV/NaClO was only 7.00% even when the NaClO concentration increased to 5.00 mM, and many PS-NP particles could still be observed in SEM images. By contrast, the mineralization rate reached 63.90% in the UV/PMS system under the identical experimental conditions, and no spherical particles appeared in the SEM results. Density functional theory (DFT) calculations revealed that the different reaction sites and energy barriers of SO4•−and•Cl on PS-NP resulted in the differences in mineralization rates and degradation intermediates. The degradation pathway of PS-NP by UV/NaClO and UV/PMS was proposed accordingly. Additionally, the intermediates toxicity evaluation by a luminescent bacteria test showed that the inhibition rate in the UV/NaClO system (2.97%) was not markedly different from that in the control group without any treatment (1.98%); while that in UV/PMS system increased sharply to 98.19%. This work demonstrated that UV/PMS was more effective in PS-NP degradation than UV/NaClO, and the chemical risks of degradation intermediates were non-negligible.Keywords:nanoplastics;polystyrene degradation;mechanisms;DFT calculation;toxicity assessment
研究领域:
环境科学
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化学工程
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毒理学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 6
·3565-3574
·
IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
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IF 4.3
Mengjing Feng,Zhigang Lei,Chengmin Gui
The dissolution mechanism of the poorly water-soluble drugs ibuprofen and aspirin in ionic liquids (ILs) was investigated by experiment, quantum chemical calculations, and molecular dynamic simulations. A comprehensive screening of 420 IL candidates was conducted using the COSMO-RS model, resulting in the selection of three cations ([EMIM] + , [HMIM] + , [P 4441 ] + ) and three anions ([TFA] − , [N(CN) 2 ] − , [CH 3 SO 4 ] − ) based on their viscosity and drug solubility. After evaluating solubility, viscosity, and cost, [EMIM][TFA] was identified as the optimal solvent. In this system, the [TFA] − forms hydrogen bonds with the drug molecules, while the [EMIM] + primarily participates in van der Waals (vdW) interactions. The solubility of ibuprofen and aspirin in [EMIM][TFA] reaches as high as 544.93 mg/mL and 387.29 mg/mL, respectively, at 323.15 K. Atoms in molecules analysis suggests that hydrogen bonding between the three anions and the drug facilitates drug solubilization; in addition, although individual vdW interactions are weak, the multisite vdW interactions between the three cations and the drug molecules exhibit significant synergy, resulting in an overall enhancement of the solubilization. Overall, drug solubilization in ILs is primarily driven by hydrogen bonding with anions and vdW interactions with cations, presenting a novel strategy for designing green and efficient drug carriers.
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DOI
高影响因子
FUEL
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2022
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IF 8.035
Shijie Wang,Yihang Chen,Yu Jia,Chen Wang,Guizhuan Xu,Youzhou Jiao,Chao He,Chun Chang,Qianhui Guo
An effective catalytic strategy for the conversion of glucose to 5-ethoxymethylfurfural (EMF) catalyzed by ultrastable Y zeolite (USY) in a co-solvent system was developed. Effects of co-solvent and reaction conditions were first investigated. Tetrahydrofuran (THF) with low dipolarity/polarizability (π*) was screened as the appropriate co-solvent, and a higher EMF yield of 41.46% was obtained as the ratio of ethanol to THF was 7:3. The macroscopic reaction kinetic study indicated that THF can protect EMF from easy degradation to EL. Moreover, the reusability and the characterization of USY verified the feasibility of USY as an efficient solid acid catalyst. In this study, density functional theory (DFT) calculations for the catalytic mechanism and solvent effect at the molecular scale were performed for the first time. The extra-framework aluminum species (EFAL), in which Al 3+ played an essential role in the reaction as the preferred EFAL species, and THF can reduce the energy barrier of USY-catalyzed glucose isomerization . Meanwhile, the inhibitory effect of THF on EMF alcoholysis was explored via the frontier molecular orbital theory. The results showed that THF increased the LUMO energy of EMF compared with ethanol and γ-valerolactone, which decreased its susceptibility to nucleophilic attack and reduced the adverse alcoholysis of EMF and humins formation. This study provided an enlightening reference for the efficient synthesis of EMF from carbohydrates catalyzed by solid acid catalyst under solvent effect.
研究领域:
化学工程
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催化化学
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计算化学
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DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2026
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IF 4.8
Zhanji Li,Jingyao Wei,Hanqian Ye,Yanhong Zheng,Haimei Yang,Chen Su,Lujian Mo,Tinghao Jiang,Chunke Nong,Zhongsheng Yi
Halogenated bisphenols (HBPs) are widely detected environmental contaminants present in water systems, soil, and biota. The incorporation of halogen substituents (Cl, Br) enhances their environmental persistence and potential toxicological effects. Understanding the cellular responses to HBPs exposure in living organisms is therefore essential for evaluating their human health implications. This study comprehensively characterizes the binding patterns and interaction mechanisms of HBPs with the G protein-coupled estrogen receptor (GPER) through an integrated approach combining multispectral analysis, molecular dynamics (MD) simulations, and quantum chemical calculations. Computational results reveal that hydrogen bonding and van der Waals interactions primarily mediate GPER-HBPs binding, with binding affinity modulated by both halogen atom count and the chemical nature of bridging groups between benzene rings. Binding of HBPs induces significant structural alterations in GPER, including conformational rearrangements, molecular compaction, enhanced hydrophobicity, and modifications to the microenvironment and secondary structure. Fourier-transform infrared (FT-IR) and three-dimensional fluorescence spectroscopy confirm secondary structure reorganization, particularly evidenced by reduced β-sheet content. Stern-Volmer analysis establishes static quenching as the dominant mechanism, correlated with specific HBPs binding modes and sites. Density functional theory (DFT) calculations identify hydrogen bonds, halogen bonds, and electrostatic interactions as key driving forces, supplemented by weaker intermolecular contributions. These insights advance the assessment of health risks associated with HBPs-type environmental pollutants.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jiangtao Meng,Benjun Yang,Lei Ren,Fengling Yang,Jingkuan Li,Jing Wang
Understanding nitrogen transformation mechanisms during pyrolysis of protein-rich biomass is crucial for biofuel, chemical production, and emission control. Using representative amino acids (Aspartic acid, Histidine, Leucine, and Phenylalanine) spanning polar/non-polar types, we pyrolyzed them at key temperatures to establish molecular conformation‑nitrogen partitioning relationships. Polar amino acids (aspartic acid and histidine) preferentially formed char-N (20–38 wt%) through bimolecular cross-linking at 750 °C. Conversely, non-polar leucine and phenylalanine enriched nitrogen in the tar phase due to side-chain inertness, which simultaneously hindered nitrogen migration to char. Significantly, steric hindrance governed reaction pathway selectivity. In phenylalanine, for instance, the phenyl ring reduced the cyclization barrier by 54.35 kcal/mol versus straight-chain dehydrogenation, facilitating preferential formation of nitrogen-containing chemicals such as indole and phenylacetonitrile via dehydrogenation/decarboxylation reactions in the primary pyrolysis of phenylalanine and secondary cracking of its tar. This work establishes molecular-level theoretical foundations for targeted synthesis of nitrogenous chemicals and NOx precursor emission control during nitrogen-rich biomass pyrolysis.
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高影响因子
Advanced Sustainable Systems
·
2025
·
IF 6.1
Duo Xu,Wenzhe Zhang,Zhiwei Chu,Qiangyu Zong,Fang Liu,Li Yang,Yuanzhuo Jing,Yingjie Li
Carbon black-loaded activated carbon (CB-loaded AC) is a cost-effective catalyst for CH 4 decomposition to produce H 2 . CB induces defects on the AC surface, enhancing catalytic activity. Current studies on the role of defects in promoting CH 4 decomposition are primarily experimental, with unclear mechanisms. Hence, exploring the reaction mechanism of defects in CH 4 decomposition is crucial. In this work, the Grand Canonical Monte Carlo (GCMC) and Density Functional Theory (DFT) are used to construct defects (Mono-Vacancy defect, Di-Vacancy defect, and Stone-Wales defect) on the AC surface, determining the catalytic mechanism of defects in CH 4 decomposition. The results show that during the CH 4 decomposition (C─H bond cleavage) phase, defective AC reduces the energy barriers for CH 4 decomposition. Under identical conditions, the rate-determining step of C─H bond cleavage in CH 4 occurs more readily on AC with Mono-Vacancy, Di-Vacancy, and Stone-Wales defects, with corresponding reductions in energy barriers of 4.64, 2.36, and 3.12%, respectively. The total energy barriers for the reaction are reduced by 12.95, 27.58, and 8.43%, respectively. This indicates that the defects significantly lower the energy barrier for CH 4 decomposition, thereby facilitating the reaction and confirming that these defects act as active sites for the catalytic decomposition of CH 4 on AC.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yongchao Miao,Qicheng Feng,Shuming Wen,Zhengyong Song
Surfactants of different kinds are important in the flotation of metal oxide ores. In this paper, a combined organic surfactant was formed through self-assembly of salicylhydroxamic acid (SHA) and isopropanolamine dodecylbenzenesulfonate (DBIA). The effects of SHA and DBIA on the flotation behavior of cassiterite were investigated. Density functional theory (DFT) calculations were used to clarify the microscopic adsorption mechanism of SHA and DBIA on the cassiterite surface. The flotation performance of the combined surfactant was investigated to determine the optimum ratio. Subsequently, the self-assembly behavior of the surfactants in aqueous solutions was examined using surface tension tests and molecular dynamics simulations. Flotation experiments and zeta potential, X-ray photoelectron spectroscopy (XPS), atomic force microscope (AFM), contact angle, and adsorption capacity analyses were used to explore the flotation behavior and adsorption mechanism at the solid–liquid–gas boundary. The maximum flotation recovery of cassiterite were 45.73 % and 71.25 % when SHA and DBIA were used alone. By contrast, with the developed combined surfactant, the flotation recovery at the same reagent concentration was 84.92 %. The SHA/DBIA surfactant co-adsorbed at the aqueous solution interface, which decreased the surface tension of the solution to 4.943 × 10 −4 mol/L and resulted in formation of a stable foam layer. These effects altered the surface properties of cassiterite and enhanced its surface hydrophobicity. Overall, this study provides valuable mechanistic insights into the enhanced chelation complexation of self-assembled surface collectors with metal oxides.
研究领域:
矿物加工工程
·
表面化学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Jiakang Han,Zihao Qiu,Gerile Naren,Rui Meng,Zikang Hu
In recent years, rare earth complexes containing amino acids have attracted much attention in numerous fields, such as light, electricity, catalysis, biological activity, drugs, etc. The rare earth element terbium is considered an important fluorescent metal due to its special electronic structure. It has excellent photophysical properties, such as high color purity, large Stokes shift, long excited state lifetime, and profuse energy levels. It has been used in the fields of fluorescent probes, medical radiation, and chemical sensors. Considering their wide applications, a series of acyl amino acid terbium complexes were synthesized using N-acyl amino acids as ligands, and their structures and photophysical properties were studied. The analysis of the theoretical and experimental results demonstrates that the energy transfer efficiency from ligands to the terbium ion emission levels increases with increasing alkyl carbon chain length, leading to differences in the luminescent intensity of the complexes. The energy transfer efficiency from ligands to rare earth ions was the result of a combination of the relative positions between the resonance energy levels of the central rare earth ion and the lowest triplet state energies of ligands as well as the intersystem crossing probability of the ligands. Moreover, the density functional theory (DFT) was used to determine the geometric structures and obtain 1 H NMR and FT-IR spectra of the terbium complexes. Their structures were further examined by comparing the calculated with the experimental spectra. The results show that the ligands coordinate to the central Tb 3+ through the bidentate chelation mode and that the theoretically determined structure was reliable.
研究领域:
化学
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材料科学
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光物理学
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DOI
高影响因子
危险品化学品经营许可证（带存储）