CHEMISTRY & BIODIVERSITY
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2024
·
IF 2.3
Wu-Ji Lai,Jia-Hao Lu,Wen-hao Chen,Li-he Jiang,Li-Qun Shen
Myricetin (1), Quercetin (2), Kaempferol (3) and Kaempferide (4) were flavonoids with phenolic hydroxyl groups. The antioxidant and pharmacological mechanisms of them were investigated in detail. The lowest hydroxyl dissociation enthalpies of 1, 2, 3 and 4 were calculated by DFT, respectively. The hydroxyl dissociation enthalpies of the four flavonoids at the O2 site are the highest. By analyzing the intramolecular hydrogen bonds and HOMO-LUMO orbitals of the four flavonoids, the reasons for their divergence of hydroxyl dissociation enthalpies and antioxidant mechanisms were further investigated. The UV–vis and IR spectra of four flavonoids were compared. The interactions about electrostatic attraction, p–π conjugation and hydrogen bond combined the flavonoid with the target protein closely. The root mean square deviation of peroxisome proliferator-activated receptor γ combined with 1, 2 and 3 increased, while that of PPARγ combined with 4 decreased. Graphical
CAS / MDL:
研究领域:
化学
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药理学
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计算生物学
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DOI
PubMed
高影响因子
Computational and Theoretical Chemistry
·
2024
·
IF 3
Xiong Zhang,Tingting Li,Qi Wang,Youyang Wang,Xiaodan Wu,Yingxue Jin,Wen Fang,Zhiqiang Wang
Numerous chlorophyll-based derivatives have found applications in the dye and pharmaceutical industries. Here, we report the synthesis of a poly-hydroxyl substituted chlorophyll molecule (THM) and its absolute configuration determination using experimental electron circular dichroism (ECD), nuclear magnetic resonance (NMR) spectroscopy, and density functional theory (DFT) calculations. Furthermore, the photoreaction types of THM (type I and type II) were investigated through theoretical calculations and validated by biological experiments. We provide a detailed analysis of electron transfer and excitation processes in THM through theoretical calculation of hole-electron distribution, as well as study intramolecular weak interactions and conjugation effects using Reduced Density Gradient (RDG), Interaction Region Indicator (IRI), and Natural Bond Orbital Analysis (NBO). The photoreaction types (type I, type II) of THM in tumor cells have also been investigated by biological experimental measures and theoretical calculation of the single-triplet state energy gap and hole-electron distribution. Molecular electrostatic potential has also been investigated by DFT methods to give insight into the molecular structure. This study provides useful guidance for the structural and photochemical studies of the chlorophyll-derived photodynamic therapeutic drugs.
研究领域:
化学
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生物学
·
药学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Hongxing He,Xintao Yang,Shunfei Li,Ying Xu,Siqing Ye,Mingyang Xiong,Ni Yang,Changgen Feng,Yi Zhang,Zhifeng Nie
Developing efficient adsorbent materials for gold recovery from e-waste holds critical importance for sustainable resource management and conservation. In this study, GA-PVA/PEI-Cl nanofibers are prepared using the electrospinning technique combined with quaternization modification, and the material shows fast and efficient adsorption properties. It was revealed that the kinetic equilibrium of Au(III) adsorption by GA-PVA/PEI-Cl took only 6 h, and the theoretical maximum adsorption capacity was 949.48 mg/g, which is better than most of the reported adsorbents in terms of both adsorption rate and capacity. In the simulated wastewater, GA-PVA/PEI-Cl showed excellent selectivity for Au(III) with a distribution coefficient as high as 49,249.6 mL/g. The adsorption isotherm and kinetic model fitting showed that the process was consistent with the Langmuir model and pseudo-second-order kinetic model, which belongs to the monolayer adsorption mechanism dominated by chemisorption. It was found that stable performance of the adsorbent was maintained after five adsorption–desorption cycles. Combined with DFT calculations and XPS analysis, the adsorption mechanism involves the synergistic action of multiple mechanisms: protonated amine groups (–NH 3 + , –NH 2 + ) and quaternized amine groups (−R 4 N + ) decrease the distance to AuCl 4 − through electrostatic interactions, followed by coordination of the nitrogen/oxygen groups to Au(III) and the in situ reduction of Au(III) to Au(0) via electron transfer. GA-PVA/PEI-Cl demonstrates potential as an efficient material for gold recovery from e-waste, owing to its rapid adsorption kinetics, high selectivity, and stable regeneration properties.
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高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
·
IF 4.3
Junying Hu,Jingkai Bi,Emmanuel Tuyizere,Zhiwei Men
In the spectroscopic study of polyatomic molecules, Fermi resonance (FR) is a vibrational coupling and energy transfer phenomenon that widely exists intra- and intermolecular. In particular, the FR coupling between the fundamental mode ν 1 and the doubling mode 2ν 2 of the CS 2 molecule has attracted extensive research. In this work, we investigate the effect of local field on tuning the FR of CS 2 . By analyzing the Raman spectra of CS 2 mixed with methanol and ethanol with different mole fractions, the results indicated that weak HBs interactions in binary solutions can be reflected by the linear frequency shift of the C–H bond vibrations (in methanol and ethanol) with different molar concentrations. Furthermore, the geometrical structure was optimized using DFT simulation, and the vibration analysis and interaction energy were carried out. The simulated Raman spectra are in good agreement with the experiments. In addition, high-pressure Raman spectra of CS 2 were obtained by diamond anvil cell technique (up to 9.19 GPa) and a pressure-induced phase transition was observed at 1.71 GPa. The results demonstrated that the pressure-induced polymerization phase transition of CS 2 molecules causes the close packing and more orderly arrangement of molecules, resulting in the enhancement of FR coupling. HB and high pressure tune the FR of the CS 2 molecule differently.
研究领域:
物理化学
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分子光谱学
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计算化学
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2020
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IF 2.463
Mengyi Qin,Fei Zhong,Yu Sun,Xiaoyan Tan,Kehui Hu,Huiwen Zhang,Mengke Kong,Guowei Wang,Linghua Zhuang
Two anionic surface active ionic liquids (SAILs), 3-methyl-1-ethoxycarbonylimidazolium decanesulfonate ([Etmim][C 10 H 21 SO 3 ]) and 3-methyl-1-ethoxycarbonylimidazolium dodecanesulfonate ([Etmim][C 12 H 25 SO 3 ]) were synthesized and studied. The surface properties, aggregation properties and thermodynamic parameters of [Etmim][C 10 H 21 SO 3 ] and [Etmim][C 12 H 25 SO 3 ] aqueous solutions were determined using surface tension and electrical conductivity . Micelle formation of [Etmim][C 10 H 21 SO 3 ] and [Etmim][C 12 H 25 SO 3 ] was spontaneous and entropy-driven. Density functional theory (DFT) calculation was used to optimize the configuration of the anions (C 10 H 21 SO 3 , and C 12 H 25 SO 3 ), imidazolium cation ([Etmim] + ), and SAILs ([Etmim][C 10 H 21 SO 3 ] or [Etmim][C 12 H 25 SO 3 ]) with different number of water molecules (1–3) using Gaussian 16 at B3LYP/6-31G(d,p) level. Typical hydrogen bonds , bond length changes, bond angle changes, and charge changes of typical atoms in hydrated complexes were analyzed. For imidazolium cation hydrates, H 2 O formed two types of hydrogen bonds with cation ([Etmim]+). For sulfonate anion hydrates, H 2 O formed two types of hydrogen bonds with anions ([C 10 H 21 SO 3 ]- or [C 12 H 25 SO 3 ]-). Hydrogen atoms in H 2 O formed hydrogen bonds with oxygen atoms of polar sulfonate anions in three ways: 1:1, 2:1, and 2:1. The typical electron withdrawing atoms (N and O) in imidazolium cation was beneficial for the micelles formation. The electrostatic repulsion and electrostatic attractive interaction between polar groups of SAILs affected the CMC values of [Etmim][C 10 H 21 SO 3 ] or [Etmim][C 12 H 25 SO 3 ] aqueous solutions. Binding energy (D 0 ), difference of binding energy (ΔD 0 ) of sulfonate ion hydrates and SAIL hydrates confirmed the tendency of [Etmim][C 12 H 25 SO 3 ] micelle formation was higher than that of [Etmim][C 10 H 21 SO 3 ].
研究领域:
物理化学
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计算化学
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DOI
高影响因子
MOLECULES
·
2026
·Vol. 31
·期 3
·
IF 5.1
Shuangnan Li,Linjie Wang,Yinghui Li,Zhenyu Zhang,Jidun Fang,Shiling Yuan
Soil moisture regulation is critical for vegetation restoration in arid ecosystems. Polymeric hydrogels, notably polyacrylic acid (PAA) and polyacrylamide (PAM), are widely employed as water-retaining agents to enhance soil water availability. However, the coupling between their distinct chemical structures and key performance metrics, particularly cycling stability and water retention kinetics in desert substrates, remains unclear. In this work, we present an integrated experimental–computational study to establish a “molecular structure–interfacial behavior–macroscopic property” framework for PAA and PAM. The results show that PAA exhibits a higher equilibrium water absorption (WAC ~242 g/g) and more stable water uptake capacity under cycling, whereas PAM displays much higher zero-shear viscosity and pronounced shear thinning with a yield plateau (~30 Pa). DFT and MD simulations trace these macroscopic disparities to their distinct electronic structures and hydration dynamics. Specifically, PAA’s strong electrostatic interactions and extended chain conformations promote a more rigid and ordered hydration shell, whereas PAM adopts a compact structure with greater chain mobility, resulting in a less ordered hydration layer. Collectively, these findings provide a structure-property framework for the scientifically grounded selection of water-retaining agents. The integrated experimental–computational methodology presented herein establishes a predictive framework for the rational design of functional materials in arid land restoration.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Jun Yang,Quanxi Zhu,Zhigang Xie,Yajing Wang,Jiankang Wang,Yuan Peng,Yingying Fang,Lihua Deng,Taiping Xie,Longjun Xu
It is very significant to boost separation efficiency of photoinduced charge carriers and to extend absorption light range from ultraviolet light into visible light region for photocatalysts . Here, Ti 3 C 2 incorporation boosted the separation efficiency of photogenerated carriers of MoS 2 , extended absorption light region, heightened the absorption intensity of visible light, and enhanced photocatalytic stability. The rhodamine B (RhB) solution could be completely degraded using MoS 2 /Ti 3 C 2 under visible light after only 30 min. The comparing evaluation of photocatalytic activity signified that the reaction kinetics of RhB photodegradation over MoS 2 /Ti 3 C 2 increased 1.4 and 3 times under UV light and visible light irradiation , respectively. Experimental tests and density functional theory (DFT) calculation confirmed the formation of MoS 2 /Ti 3 C 2 Schottky junction, in which Ti 3 C 2 served as electron sink. The photogenerated electrons in MoS 2 easily transferred to Ti 3 C 2 phase due to driving force of built in electric field, which realized efficient separation of photocarriers and prolonged the life span of photoproduced holes. We sincerely hoped this catalyst could be widely applied in wastewater treatment field.
研究领域:
材料科学
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环境科学
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理论计算
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Ke Wang,Chuanjiang Yang,Pengfei Zhao,Edward J. Anthony
The addition of molten Na 2 CO 3 can drastically accelerated the extremely slow sorption kinetics of Li 4 SiO 4 -based CO 2 sorbents in the sorption enhanced reforming process. However, the lack of a unified consensus about the effect of doped Na 2 CO 3 on the CO 2 capture process, now delays the development of more-effective Li 4 SiO 4 sorbents. Here, sorption tests, sturactural characterzations and periodic density functional theory calculations were combined to develop a better mechanistic understanding CO 2 sorption on Na-doped Li 4 SiO 4 . The Na-doped Li 4 SiO 4 exhibited a better CO 2 capture performance than pure Li 4 SiO 4 even below the melting point of any eutectic mixtures. Structural characterizations revealed that rather than generating physical favorable characteristics, the Na doping substituted at the Li site and created lithium–sodium orthosilicates (Li 4-x Na x SiO 4 ). Theoretical calculations agreeing with experimental results further demonstrated that Li 4-x Na x SiO 4 presented a weaker Na-O bond and generated more active phases (quasi Li 2 O groups) for larger sorption energies, more charge transfers and stronger CO 3 2– bond formation, in turn providing more reactive sites for enhanced CO 2 chemisorption as comparing with pure Li 4 SiO 4 . Finally, we propose a new and unified sorption mechanism independent of the traditional “melting layer” explanation.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Journal of Water Process Engineering
·
2026
·
IF 6.6
Yintao Li,Jianwen Wei,Linlin Geng,Dongling Zhao,Xiaobin Zhou
The treatment of copper laden wastewater, particularly from the electroplating industry with the Cu(II) ion concentration ranging from 100 to 300 mg/L, presents a significant challenge for achieving stringent discharge standards. This study reports the synthesis of a pore-expanded core-shell adsorbent with remarkable Cu(II) adsorption performance, accompanied by the electronic-scale investigation of its structure and behavior. This kind of adsorbent both enhances mass transfer and provides abundant chelating sites. It showed superior adsorption performance (122.55 mg/g at 318 K) which originates fundamentally from the electronic heterogeneity of its interfacial coordination environments. By integrating density functional theory (DFT) calculations with X-ray photoelectron spectroscopy (XPS), we systematically decouple the roles of distinct adsorption sites and quantify their electronic interactions with Cu(II). DFT reveals a broad distribution of adsorption energies (−1.650 to −5.989 eV) across three primary coordination modes. Our findings demonstrate that the high adsorption capacity stems from the coexistence of multiple site types: stable multidentate sites enable high metal loading, while electronically active sites with strong charge transfer ability facilitate rapid kinetics. Beyond the specific application, the synergistic strategy of pore-expanded structure and the atomic-scale mechanistic understanding established provide a paradigm for the rational design of advanced adsorbents.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122676
·
IF 7.5
Panjin Hu,Yongchao Miao,Wenping Chen,Qicheng Feng,Qinghuang Bao,Qian Zhang,Chao Li
To address the technical challenge of flotation separation between cassiterite and fluorite, this study introduces a biodegradable green chelating agent, tetrasodium glutamate diacetate (AYGLDA), as a novel depressant. The selective depression mechanism of AYGLDA is systematically elucidated through multi-scale research methods. Flotation experiments conducted on single minerals and artificial mixed ores demonstrate that, under optimal conditions of pH 8.0, an AYGLDA concentration of 60–90 mg/L, and a sodium oleate (NaOL) concentration of 80 mg/L, efficient separation of cassiterite and fluorite can be achieved. Under these conditions, cassiterite recovery remains high, while fluorite is significantly depressed. Advanced characterization techniques reveal that AYGLDA exhibits markedly different adsorption behaviors on the surfaces of the two minerals. Specifically, the adsorption capacity on fluorite is greater, with the Ca 2p binding energy on its surface positively shifted by 0.8 eV due to strong chemical chelation. This interaction results in the formation of a dense and rough hydrophilic adsorption layer Ra = 6.60 nm) on the fluorite surface, reducing the contact angle from 78° to 33° and enhancing surface electronegativity, thereby significantly depressing fluorite flotation by hindering NaOL adsorption. On the surface of cassiterite, the adsorption of AYGLDA is weak, resulting in the formation of a thin and flat adsorption layer that minimally impacts the electronic structure of Sn 3d. Consequently, this weak adsorption has a limited effect on the floatability of cassiterite. Analyses of solution chemistry and density functional theory (DFT) calculations further demonstrate that AYGLDA exhibits a significantly stronger complexation ability for Ca 2 + compared to Sn 4+ , leading to its preferential and stable adsorption on the surface of fluorite. This study presents an efficient and environmentally friendly depressant for the flotation separation of cassiterite and fluorite, while elucidating the selective depression mechanism based on atomic-scale differences in adsorption.
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DOI
高影响因子
Computational and Theoretical Chemistry
·
2021
·
IF 1.926
Jianqiang Zhao,Yue Zhang,Lihua Gan,Guanlei Wang
Here, we combined experimental measurements and DFT calculations to study UV–vis absorption spectra. DFT calculations of azobenzene and its derivatives proved useful for estimation of experimental spectra with near one-to-one correspondence. Calculation results show that substituents have no obvious effect on the coplanarity of benzene rings and N N bond. Potential energy surfaces were calculated for DHA and DEA. In the ground state, the inversion pathway was found to be preferred. A conical intersection was found between the ground and first excited states along the rotation pathway, indicating that the rotation mechanism is favored in the first excited state for DHA and DEA. UV–vis spectra of DHA and DEA were calculated by TD-DFT. Compared with azobenzene, the calculated wavelength of maximum absorption of DHA- trans and DEA- trans has red shift in UV–vis absorption spectra, which are in reasonable agreement with the experimental data.
研究领域:
化学
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光化学
·
理论计算
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产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2016
·Vol. 27
·期 49
·495403
·
IF 3.573
Dengfeng Wu,Haoxiang Xu,Dapeng Cao,Adrian Fisher,Yi Gao,Daojian Cheng
In order to combine the advantages of both 0D and 1D nanostructured materials into a single catalyst, density functional theory (DFT) calculations have been used to study the PdCu alloy NP-decorated Cu nanotubes (PdCu@CuNTs). These present a significant improvement of the electrocatalytic activity of formic acid oxidation (FAO). Motivated by our theoretical work, we adopted the seed-mediated growth method to successfully synthesize the nanostructured PdCu@CuNTs. The new catalysts triple the catalytic activity for FAO, compared with commercial Pd/C. In summary, our work provides a new strategy for the DFT prediction and experimental synthesis of novel metal NP-decorated 1D nanostructures as electrocatalysts for fuel cells.
研究领域:
材料科学
·
电化学
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理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）