JOURNAL OF MOLECULAR MODELING
·
2015
·Vol. 21
·期 11
·1-9
·
IF 1.736
Dai Zhengqiang,Liu Junbo,Tang Shanshan,Wang Yan,Wang Yiming,Jin Ruifa
Recently, a series of computational and combinatorial approaches were employed to improve the efficiency of screening for optimal molecularly imprinted polymer (MIP) systems. In the present work, we investigated MIP systems based on enrofloxacin (ENRO) as the template molecule and either 2-vinyl-4,6-diamino-1,3,5-triazine (VDAT), 4-vinylpyridine (4-Vpy), acrylamide (AM), or trifluoromethacrylic acid (TFMAA) as the functional monomer. The optimized geometries of these systems, the optimal molar ratios of template to functional monomer, and the active sites in the systems were all identified using density functional theory (DFT) at the B3LYP/6-31G( d , p ) level of theory. The imprinting mechanism was investigated by calculating the hydrogen nuclear magnetic resonance ( 1 H NMR) spectra of the systems. The simulated results revealed that the MIP system corresponding to a 1:7 complex of TFMAA and ENRO contained the most H-bonds and presented the lowest (i.e., most negative) binding energy and the strongest interactions. MIPs of ENRO with the four functional monomers were prepared based on the optimal molar ratios of template to functional monomer determined in the simulations. Adsorption experiments suggested that TFMAA has the highest affinity (saturated adsorption 30.25 mg/g) among the four monomers for the template. Thus, we determined the optimal monomer and imprinting ratio for ENRO-imprinted MIPs and predicted their adsorption characteristics.
The preparation and extraction processes of MIPs with ENRO as template, TFMAA as functional monomer, and EDMA as cross-linker
研究领域:
材料科学
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化学工程
·
计算化学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 16
·23822-23838
·
IF 0
Yu Heng,Zhang Hongliang,Zhang Chenyang,Sun Wei,Han Mingjun,Wang Rong,Wei Xin,Li Songjiang
The rapid development of industrial society is also accompanied by the generation of a large amount of heavy metal wastewater, which has caused serious harm to the ecological environment and human society. Natural sphalerite has an important value in the environmental field due to its own semiconducting properties. In order to effectively remove Ag + from wastewater containing silver, this study develops a natural mineral-based Ag + adsorbent material (sphalerite) based on elemental affinity qualities and mineralization principles. The results of batch experiments showed that the initial Ag + concentration of 50 mg/L reduced to 0.094 mg/L with a reaction duration of 15 min, a sphalerite dose of 5 g/L, an initial particle size of −400 mesh (38 μm), a reaction temperature of 25 °C, and a pH of 5. The highest adsorption capacity is 19.77 mg/g, and the adsorption behavior is consistent with the Freundlich isotherm model and pseudo-second-order adsorption kinetics. The results of solution chemical analysis indicate that the presence of Ag + is primarily influenced by the presence of S 2− . Further analysis using SEM-EDS, FTIR, and XPS techniques reveals that Ag + is chemically adsorb onto the mineral surface, resulting in the formation of Ag 2 S. DFT calculations further confirm the overlap between the Ag 4d orbitals and the S 3p orbitals on the surface of sphalerite, further confirming its chemical adsorption. Mulliken populations suggest that charge transfer occurs between Ag + and S atoms in the sphalerite surface. This research systematically reveals the Ag + adsorption mechanism on sphalerite surface and expands research ideas for treating heavy metal wastewater.
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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物理化学
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计算化学
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DOI
Materials
·
2025
·Vol. 18
·期 17
·4148
·
IF 3.2
Xiang Liu,Fujiang Huang,Xiang Shi,Hangmin Xu,Jian Xu,Xingwang Zhu
Alongside the gradual progress of industrialization and the continuous development of human society, the problems of environmental pollution and energy crisis have become increasingly prominent. Semiconductor photocatalysis is a promising solution to these challenges. The photocatalytic reduction of CO2by TiO2to produce carbon monoxide and methane is a process which has been identified as a means of developing clean energy. In this paper, two-dimensional TiO2(2D-TiO2) was synthesized via a one-step solvothermal method, and one-dimensional TiO2(1D-TiO2) was obtained through a hydrothermal process. Their photocatalytic CO2reduction performances were systematically investigated. The results show that 2D-TiO2exhibits superior catalytic activity compared to 1D-TiO2, which can be attributed to its lamellar structure, larger specific surface area, and improved hydrophilicity, providing more active sites and faster reaction kinetics. To further reveal the reaction mechanism, density functional theory (DFT) calculations were carried out using VASP with the GGA–PBE functional, PAW potentials, and a plane-wave cutoff energy of 520 eV. A 3 × 3 × 1 Monkhorst–Pack grid was used for Brillouin zone integration, and all possible adsorption configurations of CO2*, COOH*, and CO* intermediates on the 2D-TiO2surface were evaluated. The results confirm that 2D-TiO2stabilizes key intermediates more effectively, thereby lowering the energy barrier and facilitating CO2reduction. These findings demonstrate that structural modulation of TiO2significantly influences its photocatalytic performance and highlight the great potential of 2D-TiO2for efficient CO2conversion and clean energy applications.
研究领域:
材料科学
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物理化学
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纳米科技
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能源化学
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环境催化
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jiayi Shan,Fei Ying,Linrui Li,Yubo Pan,Ziwen Shi,Jijia Liang,Yunfei Gao,Fengyun Wang,Mingzhu Xia
The development of high-efficiency adsorbents for addressing Pb(II) contamination in aquatic environments remains an urgent challenge in environmental remediation. This study presents a novel thiol-functionalized ZIF-8-based adsorbent (ZIF-8-TMT) with a stable 3D framework and abundant thiol groups, designed to overcome the limitations of conventional adsorption materials. The synthesized ZIF-8-TMT demonstrated a substantial BET surface area (456.58 m 2 /g) and numerous active adsorption sites, exhibiting exceptional Pb(II) adsorption capacity (494.9 mg/g) that surpassed most previously reported adsorbents. Systematic characterization revealed that the composite achieved rapid adsorption kinetics, with approximately 80 % removal efficiency within 30 min, and maintained excellent regenerability - showing negligible capacity reduction after three adsorption-desorption cycles and retaining over 60 % removal efficiency after five cycles. The adsorption mechanism was comprehensively investigated through Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and computational simulations including density functional theory (DFT), bond order density (BOD), and natural adaptive orbital (NAdO) analyses. Results indicated that the superior adsorption performance originated from synergistic effects between electrostatic interactions and dual coordination involving the N3 atoms in 2-methylimidazole ligands and thiol (-SH) groups from TMT. This study not only provides fundamental insights into the coordination chemistry of Pb(II) adsorption but also demonstrates the practical potential of ZIF-8-TMT for wastewater treatment applications, offering a promising solution for heavy metal pollution control with its combination of high capacity, rapid kinetics, and excellent reusability.
研究领域:
环境科学
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材料化学
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重金属修复
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吸附技术
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DOI
高影响因子
Journal of Physical Chemistry C
·
2025
·
IF 3.2
Yanan Qiao,Ziqian Gao,Rui Hua,Houde She,Helin Ye,Lei Wang,Jingwei Huang,Qizhao Wang
In this study, hollow CuPc nanotubes were synthesized using a one-step solvothermal technique and loaded with TiO2 nanoparticles based on electrostatic interactions thereby overcome the inherent limitations of TiO2. The interfacial electric field formed by electrostatic coupling between CuPc and TiO2 effectively promoted spatial charge separation, as evidenced by a 12-fold enhancement in CO yield compared to pure TiO2 under visible light irradiation. Through energy band analysis and DFT calculations, the Z-type heterojunction mechanism between CuPc and TiO2 has been revealed. This mechanism facilitates the migration of photogenerated electrons from the conduction band of TiO2 to the lowest unoccupied molecular orbital of CuPc, while directing holes to migrate in the opposite direction. This spatial charge separation preserves the electrons’ high reduction capability, allowing them to participate effectively in the CO2 reduction reaction. This work highlights the potential of Z-scheme heterojunctions in designing efficient photocatalysts for CO2 reduction, offering a foundation for future research in advanced photocatalytic materials.
研究领域:
材料科学
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纳米技术
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环境科学
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物理化学
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能量转换
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yu Liu,Tianyi Hu,Shufei He,Likui Feng,Qingliang Zhao,Junqiu Jiang,Liangliang Wei
Inspired by the high sustainability, energy saving, cleanliness of photocatalysis (PC) with respect to antibiotics decomposition, we developed a stable, highly efficient Bi 2 Ti 2 O 7 @Bi 2 S 3 /polyurethane (BTO@Bi 2 S 3 /PU) photocatalytic system. It exhibited the best degradation performance with the removal of 82.08 % oxytetracycline (OTC) within 180 min under the optimal reaction parameters. Systematic characterization of BTO@Bi 2 S 3 /PU revealed its wider light-harvest capacity, higher electron–hole (e − –h + ) separation efficiency, lower interface resistance, and better redox potential in heterojunction. Based on electrochemical characterization and density functional theory calculation, the construction of Z-scheme BTO@Bi 2 S 3 photocatalyst substantially optimized the band structure. Moreover, the redox cycles of Bi 3+ /Bi 5+ and Ti 4+ /Ti 3+ further enhanced the charge transfer rate during the photoactivation process. For the OTC photodegradation pathways, ·OH, h + , ·O 2 − , and 1 O 2 dominated the pollutant decomposition and the toxicity of intermediates were decreased. Overall, the BTO@Bi 2 S 3 /PU photocatalytic system may provide a universal and stable technique for advanced photoheterojunction applications and wastewater purification.
研究领域:
环境科学
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材料科学
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毒理学
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DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Yuanyuan Cui,Gang Fu,Jiaxing Wen,Li Yang,Jiaxu Zhang,Jianmin Sun
The direct synthesis of cyclic carbonates from olefins involves a tandem process of olefin epoxidation and CO 2 cycloaddition, but designing a single catalyst with multiple active sites remains a challenge. In this work, a series of dual ligands quaternized Zr-based MOFs (Zr-Bpydc(Py + Br − )/CoTCPP-x, x = 1–5) were successfully synthesized by co-assembling 2,2′-bipyridine-5,5′-dicarboxylic acid (Bpydc) and cobalt(II) 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (CoTCPP) with Zr 6 clusters, followed by post-synthetic quaternization to incorporate nucleophilic Br − sites. Among them, Zr-Bpydc(Py + Br − )/CoTCPP-4 exhibited the best catalytic performance under mild reaction conditions (80 °C, 1.0 MPa, 12 h), achieving styrene conversion of 94.2 % and styrene carbonate (SC) selectivity of 66.5 %, significantly outperforming most previously reported heterogeneous catalytic systems under cocatalyst-free conditions. The excellent catalytic activity was attributed to the synergistic effect among redox-active Co 2+ sites, Lewis acidic Zr 4+ and Co 2+ sites, Br − sites, and basic pyridyl sites. Importantly, the catalyst also demonstrated broad substrate applicability and good recyclability, with negligible activity loss over five consecutive cycles. Furthermore, density functional theory (DFT) calculations elucidated the energy profile and reaction pathway of the styrene oxidative carboxylation reaction, revealing the cooperative roles of multiple active sites in both epoxidation and CO 2 cycloaddition reactions. Therefore, this work proposes a strategy based on the synergy of multiple active sites for developing efficient and recyclable heterogeneous MOF catalysts for CO 2 conversion.
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高影响因子
RSC Advances
·
2014
·Vol. 4
·期 98
·55445-55451
·
IF 3.708
Qi Liu,Kai Chen,Qiang Wang,Jueping Ni,Yufeng Li,Hongjun Zhu,Yuan Ding
A series of anthranilic diamides analogs (5a–x) containing 1,3,4-oxadiazole rings were synthesized and characterized by 1H NMR, 13C NMR and mass spectrometry. The structure of N-(4-chloro-2-methyl-6-(5-(thiophen-2-yl)-1,3,4-oxadiazol-2-yl)phenyl)methacrylamide (5u) was determined by X-ray diffraction crystallography. The insecticidal activities of these new compounds against diamondback moth (Plutella xylostella) were evaluated. Preliminary bioassays indicated that some of these compounds exhibited good insecticidal activities against P. xylostella, especially 3-bromo-N-(4-bromo-2-methyl-6-(5-(pyrazin-2-yl)-1,3,4-oxadiazol-2-yl)phenyl)-1-(3-chloropyridin-2-yl)-1H-pyrazole-5-carboxamide (5d), which displayed 100%, 80.95% and 57.14% activity against P. xylostella at 40 μg mL−1, 10 μg mL−1 and 4 μg mL−1, respectively. The relationship between structure and insecticidal activity was discussed. The density functional theory (DFT) studies could be helpful to understand the various insecticidal activities.
研究领域:
农药化学
·
有机化学
·
昆虫学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Xueying Wang,Zhengyan Lv,Lan Zhang,Ni Su,Changyu Lu,Yuhui Wang,Wei Huang
To tackle the dual water environment issues of emerging contaminants and algal blooms in social development, this study employed photocatalytic technology to degrade tetracycline (TC) and inactivate Microcystis aeruginosa (M. aeruginosa) , focusing on the underlying mechanisms and ecological risks. The ZnIn 2 S 4 /Zn 2 SnO 4 heterojunction facilitated efficient charge separation via a Z -scheme transfer mechanism. Under optimal conditions, the system achieved 91.1% TC degradation and 89.6% M. aeruginosa inactivation in single-pollutant systems, while in a coexisting system, it maintained high efficiencies of 87.9% and 83.2%, respectively. Furthermore, Excitation-Emission Matrix (EEM) spectra revealed that protein-like substances released during the inactivation of M. aeruginosa transformed into humic-like substances and the possible degradation processes of TC and Microcystin-leucine arginine (MC-LR), were analyzed. Ecological Structure-Activity Relationship Model (ECOSAR) combining microbial diversity analysis based on 16S rRNA gene high-throughput sequencing results confirmed a significant reduction in ecological toxicity after treatment. This study offers potential tech and theoretical support for composite water issues of emerging contaminants and algal blooms.
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2026
·
IF 5.9
Xingyu Zhang,Runyang Liu,Xiaoling Cheng,Bo Chen,Fanchao Xu,Yulai Wang,Jianjun Lian,Qiaoping Kong
Fluoride-containing wastewater has posed severe threats to the ecological environment and human health. Current mainstream treatment technologies still suffer from difficulties in the deep purification of low-concentration fluoride, poor adaptability to complex actual wastewater, and high treatment costs. Therefore, the development of environmentally friendly and cost-effective functional materials is a critical approach to achieve efficient treatment of such wastewater. This study addresses this need by synthesizing a lanthanum-based metal-organic framework (La-MOF) adsorbent through hydrothermal method by using terephthalic acid derived from waste polyethylene terephthalate (PET) plastics as organic ligand. The synthesized La-MOF exhibited stable fluoride ions removal performance across a wide pH range, achieving 90% removal efficiency and maximum adsorption capacity of 52.0 mg/g at optimal pH 4. The adsorption process of fluoride ions by La-MOF was accurately represented by the Langmuir isotherm model, and the kinetics obeyed the pseudo-second-order kinetic model. Thermodynamic analysis revealed that elevated temperatures were conducive to the adsorption of fluoride ions. Competitive ion experiments show that PO 4 3− , HCO 3 − , ciprofloxacin, and tetracycline have a certain impact on the removal of fluoride ions when their concentrations exceed 20 mg/L. Besides, ion exchange, electrostatic attraction, and coordination are the primary mechanisms for fluoride removal. Life cycle assessment shows that using PET as a synthetic material for La-MOF reduces the environmental footprint of waste plastics and also lowers the cost of synthetic materials. Fixed-bed column dynamic tests with real wastewater demonstrated that La-MOF maintained good treatment efficiency over five cycles. The results indicate that the La-MOF not only exhibits excellent removal performance toward low-concentration fluoride, but also achieves the synergistic treatment goal of “treating waste with waste”, demonstrating a very broad application prospect.
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DOI
高影响因子
POLYMER
·
2026
·
IF 5.1
Chuang Wang,Fan Zhang,Yuwei Gao,Chi Chen,Zaiqin Zhang,Hongliang Zhang
As reactive network modifiers in epoxy resin systems participate directly in the curing and crosslinking process, they inevitably affect the stoichiometric balance, crosslinked network structure, and insulation performance of the material. By constructing BDGE and HDGE bisphenol A epoxy/anhydride systems with different modifier contents and epoxy to anhydride equivalent ratios, the effects of network structure regulation on the thermal and electrical properties of the systems are systematically investigated through glass transition temperature, dielectric spectra, volume resistivity, and dielectric breakdown strength measurements, together with molecular dynamics and density functional theory calculations. The results show that increasing modifier content and chain length promotes network loosening and leads to decreases in glass transition temperature, volume resistivity, and dielectric breakdown strength. Molecular dynamics and density functional theory results further indicate that the observed deterioration in insulation-related properties is more closely associated with increased free volume and weakened electron confinement, whereas the HOMO–LUMO bandgap differences among the representative segments are relatively small. These results provide a basis for understanding the structure property relationship and for optimizing the formulation design of epoxy insulating materials.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Ziming Xin,Chendao Ruan,Jing Wang,Yuejin Zhang,Jiyan Shi
Fe/Mg co-modified biochar enabled simultaneous PFAS adsorption and Cr(VI) reduction–immobilization. • Acid-washed Fe₄Mg₁-NBC showed enhanced removal, pore accessibility, and regenerability. • Experiments and DFT confirmed hierarchical pores, bimetallic sites, and interfacial synergy as key mechanisms. Simultaneous removal of per - and polyfluoroalkyl substances (PFAS) and hexavalent chromium (Cr(VI)) from water remains challenging because of their divergent adsorption, redox, and interfacial behaviors. Herein, Fe/Mg co-modified N-doped biochar (Fe₄Mg₁-NBC) was fabricated through a hydrothermal synthesis strategy followed by pyrolysis and acid washing for the synergistic remediation of PFAS/Cr(VI) co-contaminated water. The optimized Fe/Mg ratio regulated the pore architecture and surface chemistry, producing a hierarchically porous, partially graphitized carbon matrix enriched with oxygen-containing groups and highly dispersed Fe–O/Mg–O active sites. Fe₄Mg₁-NBC exhibited superior removal performance toward PFOA, PFOS, PFBA, PFBS, and Cr(VI) in both single-solute and binary systems, with favorable adsorption under weakly acidic conditions and moderate temperatures. Acid washing further improved performance by eliminating inactive residues, opening blocked pores, and exposing additional active sites, while more than 90% of the initial adsorption efficiency was retained after five regeneration cycles. XPS analysis revealed Fe 2+ /Fe 3+ transformation and Metal–F interactions, indicating that Cr(VI) removal proceeded through Fe-mediated reduction followed by Cr(III) immobilization, whereas PFAS uptake involved electrostatic attraction, coordination, hydrophobic interaction, and pore filling. DFT calculations further demonstrated that Fe/Mg co-doping markedly enhanced PFAS adsorption affinity, decreasing the adsorption energy from +0.43 eV on pristine biochar to −1.24 eV on Fe/Mg-NBC. Co-adsorption configurations also suggested that Fe and Mg sites provided complementary functions for Cr(VI) activation and PFAS stabilization in mixed systems. These findings establish Fe₄Mg₁-NBC as a reusable multifunctional adsorbent for efficient treatment of PFAS/Cr(VI)-contaminated water. Download: Download high-res image (167KB) Download: Download full-size image
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DOI
高影响因子
危险品化学品经营许可证（带存储）