RARE METALS
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2020
·Vol. 40
·期 6
·1571-1577
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IF 2.161
Zhu Meng-Ya,He Ping,Yang Xue-Li,Hui Guang-Ze,Tang Cheng-Chun,Pan Guo-Feng,Bie Li-Jian
Abstract P-xylene (p-C 8 H 10 ) is extremely harmful and dangerous to human health due to high toxicity and strong carcinogenicity. Exploring sensitive material to effectively detect p-xylene is of importance. In this paper, perovskite single crystal (C 4 H 9 NH 3 ) 2 PbI 4 has been successfully synthesized via solution method. The obtained product was analyzed by single crystal X-ray diffraction. With the space group Pbca, orthorhombic (C 4 H 9 NH 3 ) 2 PbI 4 layered perovskite structure consists of an extended two-dimensional network of corner-sharing PbI 6 octahedron. Single layer perovskite sheets of distorted PbI 6 octahedron alternated with protonated n-butylammonium cation bilayers, which offers many advantages and provides the possibility of forming a gas sensor device based on the change of resistances. Density functional theory (DFT) simulations regarding the adsorption energy revealed that this organic–inorganic hybrid perovskite compound has excellent selectivity toward p-xylene compared with other gases including C 2 H 5 OH, C 6 H 6 , CH 2 Cl 2 , HCHO, CH 3 COCH 3 and C 7 H 8 . The calculation of electron density, density of states and electron density difference showed the sensing mechanism of p-C 8 H 10 is mainly derived from physical adsorption–desorption in view of electron transfer. Graphic abstract For organic–inorganic hybrid perovskite (C 4 H 9 NH 3 ) 2 PbI 4 , single layer perovskite sheets of distorted PbI 6 octahedron alternated with protonated n-butylammonium cation bilayers (a), which offers many advantages and provides the possibility of forming a gas sensor device based on the change of resistances. Electron density difference calculation shows that adsorption of p-xylene molecule has an obvious effect on the electron distribution of (C 4 H 9 NH 3 ) 2 PbI 4 , results in electrically polarization as a local manner (b).
研究领域:
材料科学
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化学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2019
·
IF 2.12
Xiaopei Wang,Yuanyuan Yue,Yanyan Zhang,Zhiyue Wang,Jianming Liu,Qinghu Tang
The use of the pesticide imidacloprid can be hazardous to human health. In this work, the impacts of imidacloprid on the secondary structure of pepsin were investigated through spectroscopic techniques and simulation studies. One binding site for pepsin with strong affinity was evident from changes in the fluorescence emission spectra of pepsin in the presence of imidacloprid. Calculated thermodynamic parameters based on the van't Hoff relationship indicate the predominance of hydrophobic and hydrogen bonding interactions contributing to the imidacloprid-pepsin complex. Structural changes in pepsin were also evident from changes in the UV, FTIR , CD , three-dimensional fluorescence (3D), and synchronous fluorescence spectroscopy (SFS) of pepsin upon titration with imidacloprid. Furthermore, density functional theory (DFT) calculations and molecular docking studies revealed predominant binding of imidacloprid in the hydrophobic pocket of pepsin.
研究领域:
生物化学
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毒理学
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计算生物学
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DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2015
·Vol. 17
·期 37
·24201-24209
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IF 4.493
Zhiwei Lv,Jiahui Hu,Xuan Zhang,Lianjun Wang
In the current study, thin-film composite (TFC) nanofiltration membranes desirable for water softening were successfully developed through interfacial polymerization using N-(2-hydroxyethyl)ethylenediamine (HEDA) as the amine monomer in the aqueous phase. The hydrophilicity of the membrane surface was greatly enhanced with the introduction of the residual hydroxyl groups during the fabrication process. The TFC membranes possessed a permeate flux of 15.8 L m−2 h−1 under 0.6 MPa, with a rejection of 85.9%, 73.8%, and 99.8% for Na2SO4, MgSO4 and Congo red, respectively. The interplays of the solvent, solute and polymer matrix on the separation performance were investigated by means of the solubility parameter study. Moreover, density functional theory was employed to calculate the Fukui function by the Hirshfeld charge, which gave the global and local softness values to predict the reactivity of the atomic sites in the HEDA molecule. The findings of this study support the possible forming mechanism of the barrier layer for the first time. The TFC membrane was found to be stable and displayed good separation ability over a week-long filtration process. The combined results of this work suggest that these HEDA/TMC TFC nanofiltration membranes are promising candidates for various applications, such as desalination and dye removal from wastewater.
研究领域:
材料科学
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环境工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2020
·
IF 5.065
Dongli Wei,Jiachen Li,Zhongshan Chen,Lijun Liang,Junping Ma,Mingzhi Wei,Yuejie Ai,Xiangke Wang
A kind of magnetic covalent organic frameworks (Fe 3 O 4 @TpND) is successful synthesized by the solvothermal method . The synthesis process involves two steps, where the first step corresponding to the synthesis and amino- modification of magnetic particles (Fe 3 O 4 -NH 2 ) and the second step launched with COF polymerization outside Fe 3 O 4 -NH 2 . This kind of novel materials (Fe 3 O 4 @TpND) could inherit the physicochemical superiority of COF plane and the easy recoverability of Fe 3 O 4 . The experimental results confirm that Fe 3 O 4 @TpND possessed a favorable adsorption capacity (114.97 mg L − 1 , at 298 K and pH 6.0), rapidly uptake rate, a broad pH range, and superior renewability on the removal of bisphenol-A (BPA). To shed more light on the sorption mechanism, both of static density functional theory (DFT) calculation and molecular dynamic (MD) simulation are introduced to portray the molecular-scale interaction between TpND and BPA. By exploring the geometric structures, as well as the energetic and electronic properties of the complex, the phenolic aldehyde groups in TpND were found to exert significant contribution to capture BPA molecules via the hydrogen bonding effects. From the perspective of dynamic MD simulation, the size of BPA cluster and physical pore structure of the adsorbent also possess a remarkable aggregating effect on the sorption process. Accordingly, this study provides crucial fundamental and valuable knowledge of COF materials applied in the field of water purification .
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2020
·
IF 3.232
Qi Zhou,Yun Shen,Yin Li,Li Xu,Yingxiang Cai,Xiaohua Deng
Carbamazepine cocrystals with nicotinamide , saccharin and fumaric acid were synthesized and characterized by time-domain terahertz spectroscopy . Lattice vibrations of cocrystals with their individual constituents were investigated by means of the dispersion-corrected density functional theory with and without cell parameter constraints. The simulated THz spectra successfully reproduce the features of all the crystals in their experimental spectra. A better agreement between experimental and theoretical THz spectra is achieved when the cell parameter constraints are applied in geometry optimization. Some intensive modes of neat carbamazepine and cocrystals were discussed in terms of the motions of hydrogen bonds . The effect of lattice vibration on these cocrystallizations was further examined to gain insights into the thermodynamics. It is found that lattice vibration is favorable for all these cocrystal formations.
研究领域:
药物化学
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晶体学
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光谱学
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计算化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Wei Song,Yuxin Zhou,Zhuoyue Wang,Ji Li,Xiaolei Zhang,Caixia Fu,Xing Du,Zhihong Wang,Wenhui Qiu
Advanced oxidation process (AOPs) is one of the most effective technologies for organic pollutants removal. In this study, diverse reactive species generation and enhanced sulfamethoxazole (SMX) degradation were investigated based on persulfate (PDS) activated by Fe 2+ &dithionite (DTN). When involving Fe 2+ &dithionite in PDS, SMX degradation efficiency reached 84 % within 30 min following a pseudo-first-order kinetic, which was higher than those in Fe 2+ /PDS (50.4 %) and Fe 2+ /O 2 /DTN (41.3 %). SO 4 •− and • OH were identified as dominant reactive species with a crucial role of FeSO 3 + based on quenching experiment and electron spin resonance (ESR). The contributions of SO 4 ·− , · OH, and other species to SMX degradation were 60.1 %, 33.9 %, and 6 %, respectively. In Fe 2+ /DTN/PDS system, SMX was effectively degraded under nearly neutral pH (5.0–9.0), with activation energy of 96.04 kJ·mol −1 . The experiments and density functional theory (DFT) calculation demonstrated that three functional groups (benzenesulfonamido, benzene ring, and oxazole ring) were attacked for SMX degradation. Moreover, acute toxicity to Vibrio fischeri has enhanced in the earlier degradation process due to the intermediates and weaken with the continuous reaction. This work not only provides a high-activity SO 4 ·− -AOP for refractory pollutant treatment with possible dual radical generation resources, but elucidated diverse reactive species formation with Fe 2+ &dithionite.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
CELLULOSE
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2023
·Vol. 30
·期 6
·3523-3537
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IF 5.7
Zhang Yang,Cao Jiamin,Zhou Yuhao,Li Yan,Li Lu,Xie Xin-an
In this paper, a green approach is developed for the effective conversion of corn stalk cellulose to glycolic acid with MoO 3 . The effect of different factors (amount of MoO 3 , reaction temperature, reaction time and the concentration of cellulose) were studied on conversion of cellulose. The total organic acids (glycolic acid, formic acid and lactic acid) yield of 48.2% with 93% conversion was obtained from cellulose at the optimal conditions (0.04 mol MoO 3 , 2 wt% cellulose concentration, 210 °C, 60 min), and the maximum yield of glycolic acid was 23.4%. Furthermore, the mechanism of MoO 3 -catalyzed epimerization of glucose to mannose was investigated by performing density functional theory calculations. The results indicated that the coordination between MoO 3 and the O1 sites of glucose was optimal, and MoO 3 significantly reduces the overall reaction barrier for glucose epimerization, which is the main reason why MoO 3 can promote the conversion of cellulose to glycolic acid.
研究领域:
化学工程
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可再生资源利用
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计算化学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Ahmed M. Senan,Muhammed Tilahun Muhammed,Laila A. Al-Shuraym,Sadeq K. Alhag,Niyazi A.S. Al-Areqi,Senem Akkoç
1-Phenyl ethanol derivatives are well-known classes of drug molecules that play an important role as effective substitute analogs to anticancer and antiviral agents. In this work, phenylacetylene was selected as a simple alkyne in the presence of iron (II) phthalocyanine with NaBH 4 as a catalyst. This reaction has been proven that it is a significantly efficient catalyzed conversion of terminal and internal alkynes to 1-phenyl ethanol derivatives as secondary alcohols followed by the addition and elimination mechanism. However, such drug design by compiling the redox reaction and its sequence essentially requires exact stoichiometry of iron phthalocyanine to alkynes. The products were characterized using flash column chromatography with an eluent ratio of PE: EA (5: 1 / V: V), gas chromatography, 1 H, and 13 C NMR spectroscopy. The potential of the synthesized compounds to bind to protein kinase B was investigated through molecular docking to dig out their probable anticancer activity. Compound 7 (1-(4-bromophenyl) ethan-1-ol) exhibited the highest binding potential. However, the binding potential of all the compounds was less than the standard parent compound. In addition, the density functional theory (DFT) studies of the compounds were also applied which revealed that compound 1 might have the highest chemical stability.
研究领域:
药物化学
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计算化学
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癌症研究
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yun Liu,Guijiang Liu,Yanyan Yu,Yunying Wang
The burgeoning interest in single atom catalysts (SACs) stems from their exceptional oxidase-mimicking capabilities, driving substantial advancements in this field. Nevertheless, a critical knowledge gap remains regarding the influence of Zn incorporation on the oxidase-like activity of atomically dispersed Fe-N-C catalysts. This study successfully synthesized and comprehensively characterized three distinct SACs (FeZn SAC-N@C, Fe SAC-N@C, and Zn SAC-N@C) using TEM, HAADF-STEM, XRD, XPS, BET, ICP-MS, and XAFS techniques. Activity assays revealed that FeZn SAC-N@C exhibited the highest oxidase-mimicking activity, with Fe SAC-N@C displaying moderate activity, whereas Zn SAC-N@C did not exhibit oxidase-like behavior. The superior oxidase-like activity of FeZn SAC-N@C is attributed to its enhanced O 2 activation capacity, characterized by a high free energy of 0.90 eV in the rate-determining reaction step, surpassing those of Fe SAC-N@C (0.85 eV) and Zn SAC-N@C (0.71 eV). EPR and DFT calculations elucidated the catalytic mechanism of FeZn SAC-N@C, involving the generation of O 2 − radicals. As a proof-of-concept, FeZn SAC-N@C demonstrates potential as a colorimetric sensor for detecting ascorbic acid and nitrite, achieving a limit of detection of 0.77 μM for ascorbic acid and 0.16 μM for nitrite. These findings open a new avenue for configuring bimetallic atomically dispersed catalysts with oxidase-like activity in future research.
研究领域:
生物化学
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材料科学
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催化反应
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Liu,Chao Pan,Xianjie Li,Hailin Zhang,Zhijie Shang,Hongbing Song
Oxidation, a pivotal process in organic synthesis, is essential for the conversion of various biomass derivatives, including 5-hydroxymethylfurfural (HMF), into valuable chemicals. This research employs poly(ionic liquid)s (PILs) as supports to fabricate Au/PILs catalysts, which are subsequently utilized in the oxidative esterification of HMF to produce dimethyl 2,5-furandicarboxylate (FDMC). The modification of PILs demonstrates that catalyst’s performance is optimized when the PILs anion (IL: EGDMA = 1: 4) is [Tf 2 N - ]. The presence of the [Tf 2 N - ] group is essential for charge transfer between the carrier and the active metal Au, thereby enhancing the catalytic reaction. Thermogravimetric analysis (TG) reveals the exceptional thermal stability of the 2 % Au/PILs-Tf 2 N-14 catalyst. The efficient conversion of HMF to FDMC is achieved using the 2 % Au/PILs-Tf 2 N-14 catalyst at 120°C, 12 h, with CH 3 ONa (0.75 equiv.) and 2 MPa O 2 , yielding a HMF conversion ( C HMF ) of 96.41 % and a FDMC selectivity ( S FDMC ) of 100 %. The heterogeneous catalyst 2 % Au/PILs-Tf 2 N-14 maintains high catalytic activity after multiple cycling experiments. A catalyst based on precious metal-loaded PILs was utilized to achieve efficient and selective conversion of HMF to FDMC under low loading conditions. This approach not only offers valuable insights for future research but also promotes the shift towards renewable energy sources. Additionally, the adsorption behavior of O 2 on Au 8 clusters and the interaction between the reaction substrate HMF and [Tf 2 N - ] were examined through density functional theory (DFT) calculations, providing theoretical backing for further investigation.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Fu Li,Qian Huo,Xiaomei Zhou,Shasha Fang,Fei Han,Jingnan Yang,Qingxin Guan,Wei Li
Photothermal CO 2 into methanol is an effective approach to address energy and environmental challenges, but the low conversion and poor selectivity limit its large-scale application. Here, 0.5Cu@CeO 2 with atomically dispersed active sites and abundant Frustrated-Lewis-pairs (FLPs) was synthesized using coordination complex precipitation reaction. The substitution of Cu 2+ with Ce 3+ results in the formation of new FLPs, which promotes the upward shift of conduction band (CB) and enhances the reducing capability of catalyst. Moreover, the more sensitive and stronger capability of photogenerated carriers also endows 0.5Cu@CeO 2 with stronger CO 2 reduction capability. The photothermal methanol yield of 0.5Cu@CeO 2 reached 1896.02 μmol·g cat –1 ·h –1 . The DFT results demonstrate the FLPs structure of 0.5Cu@CeO 2 promotes parallel adsorption of CO 2 and *CO species. Meanwhile, the presence of O v inhibits the dissociation of oxygen species, consequently boosting the methanol synthesis. The construction of FLPs structure introduces a novel method to enhance CO 2 conversion utilizing photothermal catalysis.
研究领域:
催化
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材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Changqing Gui,Zirui Wang,Changjian Ling,Zhongfeng Tang
Molten salt-doped MgO adsorbent is considered one of the most promising CO 2 adsorbents in the field. In this work, MgO-based adsorbents were prepared by one-step calcination using MgCl 2 ·6 H 2 O as magnesium source. The CO 2 adsorption performance of MgO-based adsorbents was investigated via different methods. Results showed that the maximum CO 2 adsorption capacity of MgO doped by LiNO 3 -NaNO 3 -KNO 3 was 57.1% at the CO 2 concentration of 80% and 350 ℃, and the MgO-based adsorbents showed good regeneration. The nanosheet structure of the MgO-based adsorbents decreased with the increase in the number of cycles, whereas the crystal structures of MgO and alkali metal nitrates did not change because of multiple decarbonization. DFT computation revealed selective adsorption of CO 2 on different crystal faces of MgO. The (200) crystal face of molten salt-doped MgO did not have CO 2 trap ability. In addition, the doped nitrate did not directly participate in the reaction but reduced the adsorption energy of MgO carbonation. The adsorption energies of the MgO (220) and (222) crystal faces after doping with nitrate were reduced to − 2.07 and − 3.26 eV, respectively. The overall energy level of adsorption decreased as the number of resonance peaks and the stability of the structure increased. This study explains why MgO currently fails to reach the theoretical adsorption capacity and reveals the underlying mechanism of molten salts.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）