CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Niu Liu,Dongfang Guo,Shiwang Gao,Hanming Liu,Hongwei Niu,Lianbo Liu,Shiqing Wang,Qi Wang,Huanjun Wang,Wei Xu,Hongjun Zhang
To elucidate the direct air capture (DAC) performance and CO 2 selective sieving mechanisms of distinct porous materials under trace CO 2 conditions, three types of materials, anion-pillared materials, open site MOFs, and amine-modified materials, were synthesized, with their DAC performance systematically characterized. DFT-D3 calculations revealed that in NbOFFiVE-1-Ni, the C···F distances (3.04 Å) between CO 2 and the pillared NbOF₅ 2− anions, as well as the O···H distances (2.89 Å) between CO 2 and pyrazine linker hydrogens, are shorter than those in SIFSIX-3-Ni and GEFSIX-3-Ni. These synergistic C···F van der Waals (vdW) and O···H hydrogen-bonding interactions afford NbOFFiVE-1-Ni the highest CO 2 binding energy (62.74 kJ/mol), exceeding that of SIFSIX-3-Ni (57.79 kJ/mol), GEFSIX-3-Ni (60.47 kJ/mol), and MIL-101(Cr) (22.86 kJ/mol). Consistently, NbOFFiVE-1-Ni exhibits the highest atmospheric CO 2 uptake (1.15 mmol/g) among these materials. Given the low atmospheric CO 2 uptake of pristine MIL-101(Cr), two amines (PEI and TEPA) were used to modify it, leveraging its abundant unsaturated metal sites to enhance CO 2 adsorption capacity. DAC performance of amine-modified MIL-101(Cr) first increased then decreased with amine loading, with optimal values of 2.07 mmol/g (50 wt% TEPA) and 1.52 mmol/g (70 wt% PEI). DFT-D3 calculations demonstrated that TEPA molecules and PEI chains bind directly to the unsaturated metal sites of MIL-101(Cr), forming tadpole-like amine-modified MOF structures with binding energies of 210.01 kJ/mol and 178.30 kJ/mol, respectively. Positron annihilation lifetime spectroscopy (PALS) confirmed that TEPA incorporation generates new cavities, microporous structures, and abundant active amine sites in MIL-101(Cr) crystals, synergistically enhancing its DAC performance.
研究领域:
材料科学
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环境化学
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物理化学
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多孔材料
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碳捕集
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Zongwei Hao,Ailong Hu,Juntao Cheng,Zhenni Ma,Zhaofeng Li,Jiali Lv,Huajian Xu,Huifang Ge,Hongyan Wang,Zhenyu Yu,Zhongwen Xie,Yiqun Du
The digestibility of starch-based foods is receiving increased attention. To date, the full understanding of how including L-theanine (THE) can modify the structural and digestive properties of starch has not been fully achieved. Here, we investigated the multi-scale structure and digestibility of maize starch (MS) regulated by THE in ultrasound field and the molecular interactions . Ultrasound disrupted the structure of starch granules and opened the molecular chains of starch, promoting increased THE binding and producing more low-order or disordered crystal structures. In this case, the aggregation of starch molecules, especially amylose , was reduced, leading to increased mobility of the systems. As a result, the apparent viscosity, G', and G" were significantly decreased, which retarded the starch regeneration. Density functional theory calculations indicated that there were mainly non-covalent interactions between THE and MS, such as hydrogen bonding and van der Waals forces. These interactions were the main factors contributing to the decrease in the short-range ordering, the helical structure, and the enthalpy change (ΔH) of MS. Interestingly, the rapidly digestible starch (RDS) content of THE modified MS (MS-THE-30) decreased by 17.89 %, while the resistant starch increased to 26.65 %. These results provide new strategies for the safe production of resistant starch.
研究领域:
食品科学
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分子生物学
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生物物理学
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Zhengwen Wei,Xiang-fei Lü,Wei Wang,Giuseppe Mele,Zhen-Yi Jiang
Phenanthrene (PTH) and 9-phenanthrol (9-PTH) exhibited severe health threats and ecological hazards, for this reason, exploring a high-efficient removing strategy for PTH and 9-PTH could be considered of great urgency. Herein the 4,4'-biphenyldicarboxaldehyde m-phenylenediamine Schiff base magnetic polymer (magnetic BIPH-PHEN) was successfully fabricated via Schiff base polycondensation reaction and the subsequently one-pot embedded method. The mutual aromatic nucleus of BIPH-PHEN polymer and PTH/9-PTH could form π–π interaction, thus improving the capture ability, the embedded Fe 3 O 4 nanoparticles provided the possibility for rapid separation. The physical and chemical properties of the magnetic BIPH-PHEN were systematically characterized. The removal rate of magnetic BIPH-PHEN towards PTH and 9-PTH was 85.65 % and 98.52 %, respectively (PTH or 9-PTH: 8 mg/L; Adsorbent: 0.2 g/L). The DFT calculations including energy calculations and electrostatic potential distribution analyzed the different bonding modes and proposed the most possible bonding modes in the adsorbent/adsorbate system. Moreover, the LUMO and HOMO orbits combined with energy gaps analysis proved the existence and specific types of the π–π interaction. The monolayer adsorption occurred on the homogeneous magnetic BIPH-PHEN surface, simultaneously the chemisorption was dominant. This work not only proposed new sights on assembling magnetic Schiff base polymer for removing polycyclic aromatic hydrocarbons, but also provided a deeper understanding of intramolecular interactions.
研究领域:
环境科学
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材料科学
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理论化学
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DOI
PubMed
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Ahsan Nazir,Ameena Tur Rasool,Chuntao Chen,Bianjing Sun,Dongping Sun
In this study, a NiO-PbBiO 2 Br photocatalyst was developed by a simple chemical precipitation approach followed by a hydrothermal process to eliminate tetracycline (TC). The resultant materials were assessed utilizing diverse characterization techniques. Compared with pure PbBiO 2 Br (49.5 %) and NiO (56.8 %), the NiO-PbBiO 2 Br composite exhibited superior photocatalytic effectiveness for removing TC under visible light and achieved a remarkable 98.4 % elimination of TC within 70 min (conditions: [TC] = 10 mg/L, pH 7 and [catalyst] = 1 g/L). The reaction rate constant (K) values are in the following order: NiO-PbBiO 2 Br (0.0591 min −1 ) > NiO (0.0119 min −1 ) > PbBiO 2 Br (0.0097 min −1 ). The markedly improved photocatalytic efficiency of NiO-PbBiO 2 Br can be ascribed to the expanded light absorption and the establishment of p-n heterojunction amid NiO and PbBiO 2 Br. The effects of several important factors, e.g. TC concentration, pH, catalyst dosage, and different water sources, were thoroughly investigated. Cycle tests were performed to confirm the stability and reusability of NiO-PbBiO 2 Br. Furthermore, electron spin resonance (ESR) and radical scavenging studies verified that the species •O 2 − , h + , and •OH play a key role in removing TC. The susceptible active regions of TC and the probable TC degradation routes were examined through density functional theory (DFT) calculations and high-performance liquid chromatography (HPLC) analyses. Thus, this work presents a new methodology for creating a photocatalyst with enhanced photocatalytic effectiveness for removing organic pollutants in water.
研究领域:
环境科学
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材料科学
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化学
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水处理
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计算化学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Jing Chen,Qin Ma,Xiaoyan Hu,Yunjing Gao,Xiaoyu Yan,Dongdong Qin,Xiaoquan Lu
In the present work, we proposed a novel naked-eye and turn-on fluorescence sensor based on the 5,10,15,20-(4-sulphonatophenyl) porphyrin (TPPS 4 )-Hg 2+ system with short assay time and high sensitivity to detect glutathione (GSH) in real samples. The TPPS 4 was the first time to detect GSH because of its high fluorescence quantum yield. The initial fluorescence from TPPS 4 was quenched by Hg 2+ with an electron transfer process. However, when put a certain concentration of GSH into this system, the fluorescence sensor was turned to the “on” state, which was related to a competitive affinity of Hg 2+ to GSH and the N atoms of porphyrin ring. Under the optimal conditions, the naked-eye detection limit was 0.43 nM and the limit of detection (LOD) was arrived to 16 fM (S/N = 3) for GSH. The linear regions are obtained by two ranges varying from 0 to 28.5 μM and from 38.15 to 61.87 μM. Furthermore, it was confirmed that the TPPS 4 -Hg 2+ fluorescence probe has excellent selectivity, high sensitivity and quick fluorescence response for GSH.
研究领域:
分析化学
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材料科学
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生物化学
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DOI
高影响因子
Analytical Methods
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2020
·Vol. 12
·期 7
·943-950
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IF 2.596
Dandan Li,Lihua Gong,Zhenyang Qiao,Congcong Zhu,Qiaojuan Jia,Huajie Kong,Shuyan Jiao
A novel highly selective colorimetric fluorescence probe, POPH, has been successfully synthesized and it shows remarkable selective and sensitive response to Cu2+ in aqueous media (HEPES buffer, pH = 7.4). The fluorescence of probe POPH immediately decreased when 1.1 equiv. of Cu2+ was added to a solution of probe POPH, accompanied by color change from wathet blue to colorless under 365 nm UV lamp illumination. The possible bonding model of probe POPH with Cu2+ was examined through HRMS, FESEM, TEM, FTIR spectroscopy and DFT calculations. Moreover, the probe POPH could be used for monitoring Cu2+ in living cells using laser scanning confocal microscopy.
研究领域:
分析化学
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材料科学
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生物化学
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理论化学
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产品关联
DOI
高影响因子
DYES AND PIGMENTS
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2023
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IF 4.5
Xiumin Liu,Hengwei Zhang,Fengting Hu,Yi Wang,Xu Fei,Jing Tian
In this paper, an efficient and novel 1,3-bis(2-pyridylimino)-4,7-dihydroxyisoinndole scaffold-based two-site fluorescent probe 1,3-bis(2-pyridylimino)-4,7-phenylene diacrylate isoindole (BPI-AC) for the sensing of cysteine (Cys) has been designed and synthesized. We have studied the chemical structure and its fluorescent properties for the novel fluorescent probe with double recognition group by means of theoretical calculations and experimental measurements, which were carried out using density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations and experiments on organic chemical synthesis. Firstly, geometries have been recorded for the fluorescent probe. Theoretical research parameters including spectroscopic parameters, molecular orbitals , reaction sites and energy barrier Δ were obtained by fitting the electron density in a multiparticle system. Additionally, the spectral characteristics , selectivity and anti-interference performance of the probe were systematically investigated and verified by in vitro experiments. The experimental results showed that by using this probe, it was possible to quantitatively detect Cys in 1% dimethyl sulfoxide-containing water solution (pH 7.4). Super large Stokes shift (265 nm) endowed the probe low background signal. Finally, according to our theoretical calculations and the available experimental data, the probe BPI-AC with dual recognition sites could distinguish the biothiols with similar structure through series recognition reaction, and the Stokes shift was large, realizing the efficient detection of Cys specificity.
研究领域:
分析化学
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理论化学
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生物化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Ruoxuan Guo,Yang Liu,Yingzhong Huo,Anrui Zhang,Jiahui Hong,Yuejie Ai
Covalent organic frameworks (COFs) are promising adsorbents for removing heavy metal ions , and have high crystallinity , a porous structure, and conjugated stability. N -containing functional groups are known to have great affinity for uranyl ions. In this work, to explore the peculiarity of the pyridine N structure as an efficient adsorbent, we chose 2,2′-dipyridine-5,5′-diamine (Bpy) and pyridine-2,5′-diamine (Py) as the core skeletons, and 1,3,5-triformylphloroglucinol (Tp) as the linker to synthesize two crystalline and stable N -containing COFs named TpBpy and TpPy, respectively, through a facile solvothermal method . Characterization results demonstrated that TpBpy and TpPy possessed regularly growing pore sizes, large specific surface areas and relatively strong thermal resistances . The results of batch experiments showed that both COF materials were capable of the effective removal of uranyl with uptake capacities of 115.45 mg g −1 and 291.79 mg g −1 , respectively. In addition, density functional theory (DFT) simulations highlighted the beneficial chelation effect of the double N structure in pyridine monomers for removing uranyl ions. Combining systematic experimental and theoretical analyses, the adsorption process and interaction mode of porous COFs and UO 2 2+ were revealed, to provide predictable support for the application of pyridine N -containing COFs in the field of environmental remediation.
研究领域:
环境科学
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材料科学
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化学工程
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理论化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xi Tao,Poyueh Pan,Taobo Huang,Long Chen,Haodong Ji,Juanjuan Qi,Fengbin Sun,Wen Liu
Sulfachloropyridazine (SCP) was commonly used as a broad-spectrum sulfonamide antibiotic and hard to be removed through traditional sewage treatment process. In this study, we developed a simple and controllable strategy to realize in-situ construction of Co(OH) 2 nanoparticles decorated urchin-like WO 3 (Co(OH) 2 /WO 3 ), which could efficiently remove SCP through peroxymonosulfate (PMS) activation. Some tiny nanoparticles of Co(OH) 2 decorated on the spines/nanorods or surfaces of urchin-like WO 3 by transmission electron microscopy (TEM) analysis. The obtained 10 wt% Co(OH) 2 /WO 3 realized completely removal of SCP (degradation efficiency 100%) with a high reaction rate constant ( k 1 ) of 0.88 min −1 within 3 min at optimal pH 7. That was because the urchin-like WO 3 with numerous adsorption functional groups on its surface ( e.g. , W = O and –OH bonds) could adsorb the Co 2+ easily to form CoOH + , which was perceived the rate-limiting step for PMS activation and generating radicals. Radical quenching experiments indicated that SO 4 •− played a more significant role than HO • radicals. Density functional theory (DFT) calculation revealed that the atoms of SCP with high Fukui index ( f − ) were active sites, which preferred to be attacked by the electrophilic SO 4 •− and HO • radicals. The toxicity of the intermediates by SCP degradation was evaluated by quantitative structure–activity relationship (QSAR) prediction through Toxicity Estimation Software Tool (T.E.S.T.). The possible degradation pathway and catalytic mechanism for SCP removal were proposed. Considering the good catalytic properties of Co(OH) 2 /WO 3 -PMS, the material will show great application potential in the removal of emerging contaminants in water.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Longde Jiang,Jingde Luan,Haowei Zhang,Yu Bai,Yu Zhang,Wengang Liu,Zheng Yan,Haiting Zhao
Photocatalytic H 2 production from seawater splitting is a promising method for sustainable energy conversion technology. The vanadium-oxygen binary doped carbon nitride (VO X -CN) is successfully prepared for H 2 production. Benefiting from the electronic structure alteration, the maximum H 2 yield on VO X -CN in artificial seawater reaches 4475.74 μmol h −1 g −1 , 10 times higher than that of CN in deionized water. The impact of ions on the photocatalytic activity of VO 2 -CN is followed by Na + > Mg 2+ > K + > Ca 2+ . The adsorption of electrolyte ions promotes the formation of delocalized electron clouds on the surface of VO 2 -CN, facilitating more electrons to participate in H + reduction. Screening based on six machine models, the decision tree regression algorithm is used to reveal the interaction between cation type, their concentration and H 2 yield. Pearson heatmap indicates that Na + , Mg 2+ , and K + ions are positively correlated with H 2 yield, whereas Ca 2+ shows a negative correlation. The interactions among Na + , Mg 2+ and K + atoms facilitate H 2 production in multi-ion system, whereas Ca 2+ ions do the opposite, especially for high concentration. This work proposes new insights into the interference on H 2 yield between the structure alteration of CN framework and the change of ion type and concentration.
研究领域:
材料科学
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催化
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能源转换
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化学工程
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机器学习
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产品关联
DOI
高影响因子
LANGMUIR
·
2026
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IF 4.4
Qi Wang,Chao Song,Zhuang Bo,Haotong Yang,Xun Gao,Jingquan Lin
This study employed density functional theory (DFT) and time-dependent density functional theory (TD-DFT) to investigate the interaction mechanism between Phenthoate and Au20 nanoclusters, and the solvent environment effect was examined under the polarizable continuum model (PCM). By comparing and analyzing theoretical Raman active spectra and experimental Raman spectra, the phenomenon of selective enhancement of specific vibrational modes in surface-enhanced Raman spectroscopy (SERS) was explained. By analyzing the molecular structure, frontier molecular orbitals (FMOs), ultraviolet–visible absorption spectra (UV–vis), noncovalent interactions (NCI), reduced density gradients (RDG), electron localization function (ELF), and localized orbital locator (LOL), the adsorption mechanism and the spectral characteristics induced by interfacial charge transfer were comprehensively revealed at the electronic level. Phenthoate chemically adsorbed onto the Au20 surface through the S atom, forming a stable complex. Meanwhile, this charge transfer mechanism effectively modulated the polarization rate of the molecule. This study provides a theoretical basis for elucidating the adsorption behavior and spectral response mechanism of organophosphorus pesticides on metal nanostructures, offering valuable insights for the design of highly sensitive SERS sensors.
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DOI
PubMed
高影响因子
Food Chemistry: Molecular Sciences
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2022
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IF 0
Guohua Yao,Muhammad Muhammad,Jiajiang Zhao,Jianguo Liu,Qing Huang
Astaxanthin is a carotenoid widely used in food additives, nutritional product and medicines, which shows many physiological functions such as antioxidant, anti-inflammatory, anti-hypertensive and anti-diabetic activities. It has been recognized that astaxanthin has all- trans and nine cis isomers, and these geometrical isomers have very different biological activities. The process of selective enrichment, metabolism and isomerization of astaxanthin in animals remains to be studied. Therefore, identifying isomers and obtaining their structural parameters are important for understanding the active mechanism of different molecular isomers. Although the traditional methods such as high-performance liquid chromatography (HPLC) and nuclear magnetic resonance (NMR) spectroscopy can be used to distinguish these isomers, these methods generally require considerable testing time, cost, sample volume, and hardly be applied in vivo. In this work, Raman spectroscopy combined with density functional theory (DFT) calculation was introduced to study different geometrical isomers of astaxanthin. The theoretical and experimental Raman spectra are in agreement, and we have demonstrated that all the known ten geometrical isomers of astaxanthin can be readily distinguished using this spectroscopic approach. The astaxanthin molecular vibrational modes, geometric structures, energies of ten geometric isomers are systematically scrutinized. Moreover, a lot of structural and Raman problems unsolved previously have been solved by the DFT-based spectral analysis. Therefore, this work provides an effective way for identification of different astaxanthin geometrical isomers, and may have important significance for promoting the research of astaxanthin isomers on biological property mechanisms and related applications in food molecular science.
研究领域:
食品科学
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分子生物学
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药物化学
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产品关联
DOI
PubMed
危险品化学品经营许可证（带存储）