SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2026
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IF 4.8
Chen Zheng,Shuang Li,Wenhui Fang,Wei Zhang,Zhiwei Men
The competition between the intramolecular hydrogen bonds (intra-HBs) in astaxanthin (AST) and the intermolecular hydrogen bonds (inter-HBs) between AST and ethanol (EtOH) controls the structural stability of AST in the solution during the cooling process. This study employs an integrated approach combining Moving window Two-Dimensional (MW2D) correlation Raman spectroscopy and density functional theory (DFT) simulations to investigate the interaction between ethanol (EtOH) and astaxanthin (AST) across a temperature range of 303 K–83 K. The MW2D analysis indicates that, below 253 K, EtOH reorganizes into cooperative multimers prior to any conformational change in AST. DFT simulations demonstrate that EtOH multimers weaken the intramolecular hydrogen bonds (intra-HBs) in AST through O H⋯O C interactions. These findings clarify the apparent contradiction between the extended conjugation length of AST and weakened inter-HBs.
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高影响因子
POLYHEDRON
·
2026
·
IF 2.8
Innocent Tayari Mwizerwa,Jiayi Tang,Tianlei Huang,Li Zelong,Zhuyu Sun,Xiaoxiang Zhao
Graphitic carbon nitride photocatalytic efficiency is hindered by limited active sites and fast electron-hole recombination. A facile two-step calcination strategy was used to fabricate iron and nickel co-doped g-C 3 N 4 (Fe/Ni-g-C 3 N 4 ) for enhanced photocatalytic degradation of Rhodamine B (RhB) under visible light irradiation. This increased specific surface area (11.2 m 2 /g for Fe 3 /Ni 1 -g-C 3 N 4 compared to 10.3 m 2 /g for pure g-C 3 N 4 ), improved visible light harvesting, and triggered a prolonged charge carrier lifetime. The Fe 3 /Ni 1 -g-C 3 N 4 catalyst showed superior performance, with a kinetic rate constant of 0.04481 min −1 , which is three times greater than that of its other counterpart photocatalysts. It also exhibited excellent stability, degrading over 90% of RhB for three consecutive cycles. Meanwhile, mechanistic study of radical quenching tests and DFT calculations showed degradation via h + radicals, initiating deethylation and hydroxylation reactions that mineralized RhB into CO 2 and H 2 O. Finally, this report provides the synergy of Fe/Ni and an avenue for efficient and stable metal-doped graphitic carbon nitride photocatalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Huining Zhang,Baixiang Wang,Yakun Dong,Jianping Han,Yi Zhao
To effectively address the potential threats posed by microplastics (MPs) to the environment and human health, this study drew inspiration from the naturally occurring biocompatible substance dopamine. We prepared poly(dopamine) (PDA)-modified graphene oxide (GO) ink and successfully constructed a poly(dopamine)-functionalized graphene macro-adsorption network (3DGO/PDA) via direct ink writing (DIW) printing technology. The incorporation of PDA significantly enhances the adsorption active sites of 3DGO/PDA, endowing it with outstanding adsorption performance toward polystyrene (PS) microspheres. Concurrently, the exceptional three-dimensional network pore structure of 3DGO/PDA provides efficient mass transfer pathways and abundant pore space for the adsorption and storage of polystyrene. Experimental results indicate that under pH= 5 conditions, 3DGO/PDA3 achieves an 86 % (PS initial concentration of 200 mg/L, temperature of 313.15 K) removal rate for polystyrene, maintaining stable adsorption performance after multiple cycles. Density functional theory (DFT) calculations indicate that the adsorption of PS onto the adsorbent involves a synergistic interaction of multiple mechanisms, with amino-dominated chemical adsorption playing a dominant role. Therefore, by combining the functionalization design of polydopamine with 3D printing technology and leveraging density functional theory calculations at the electronic level, the enhanced adsorption mechanism was systematically elucidated. This provided new design ideas and a theoretical basis for the development of efficient microplastic adsorption materials.
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CHEMOSPHERE
·
2024
·
IF 8.1
Meng Wang,Rongkang Yan,Meng Shan,Shasha Liu,Hai Tang
Adsorptive separation membranes are widely utilized for the removal of toxic dyeing pollutants from dyeing wastewater. However, developing novel adsorption membranes with large adsorption capacities and enhanced adsorption performance for dyes in actual wastewater poses a significant challenge. This study focuses on the fabrication of crown ether-containing copolymer porous membrane (CRPM) and investigation of the adsorption performance of dyes from aqueous solutions. The morphology structure and pore size distribution revealed that the membrane was endowed with rich micropores and hierarchical porous structures. Three typical cationic dyes (MB, RhB, CV) and an anionic dye (MO) were selected to evaluate the adsorption behavior. The results of adsorption isotherms and kinetics demonstrated that the adsorption data could be well-fitted using the Freundlich and pseudo-first-order kinetic models, the thermodynamic parameters revealed that the adsorption process of dyes on CRPM is a spontaneous endothermic reaction. The membrane exhibited excellent adsorption performance for cationic dyes, with RhB displaying a higher maximum adsorption capacity than previously reported porous membranes. Notably, dynamic adsorption-desorption filtration demonstrated a rapid removal efficiency, with RhB, MB, and CV achieving removal rates of 99.09%, 98.63%, and 99.14% respectively, after five cycles. The filtration volume of the CRPM membrane was 2.4-fold greater than that of a traditional PVDF membrane when applied to actual dyeing wastewater. DFT theoretical calculations were employed to elucidate the adsorption mechanism. These calculations confirmed the significant roles of electrostatic interactions, H-bonds and π–π interactions in facilitating the high-efficiency adsorption of cationic dyes. These findings highlight the potential of the crown ether-containing copolymer as a promising material for adsorption separation membranes in the treatment of dyeing wastewater.
研究领域:
环境科学
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材料科学
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高分子化学
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分离科学
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物理化学
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2016
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IF 5.393
Ting Liu,Lucheng Xue,Xin Guo,Yu Huang,Chuguang Zheng
To investigate the mechanism of Hg0 adsorption on the α-Fe2O3(001) surface in the presence of HCl, which is considered to be beneficial for Hg0 removal, theoretical calculations based on density functional theory as well as corresponding experiments are carried out. HCl adsorption is first performed on the α-Fe2O3(001) surface, and the Hg0 adsorption on HCl-adsorbed α-Fe2O3(001) surface is subsequently researched, demonstrating that HCl dissociates on the surface of α-Fe2O3, improving the Hg0 adsorption reactivity. With further chlorination of the α-Fe2O3(001) surface, FeCl3 can be achieved and the adsorption energy of Hg0 on the FeCl3 surface reaches −104.2 kJ/mol, representing strong chemisorption. Meanwhile, a group of designed experiments, including Hg0 adsorption on HCl-preadsorbed α-Fe2O3 as well as the coadsorption of both gaseous components, are respectively performed to explore the pathways of Hg0 transformation. Combining computational and experimental results together, the Eley–Rideal mechanism with HCl preadsorption can be determined. In addition, subsequent X-ray photoelectron spectroscopy analysis verifies the appearance of Cl species and oxidized mercury, exhibiting the consistency with experiments.
研究领域:
环境化学
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计算化学
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表面科学
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污染控制
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Peizhen Zhang,Chenxi Li,Lili Huo,Lixin Zhao,Zonglu Yao
To enhance the application potential of straw-based biochar in CO 2 capture, this study prepared nano-MgO-supported biochar (MgO/BMBC) via a combined ball-milling and MgO-modified pyrolysis activation process. The CO 2 adsorption performance of the material was systematically investigated, and the adsorption mechanism was elucidated through structure-property relationship analysis and density functional theory (DFT) calculations. The results indicate that wet-milled biochar (W-MgO@BMBC) exhibits a hierarchical pore structure and a specific surface area of 323.14 m 2 ·g −1 . This method promotes the formation of a hierarchical porous structure, the presence of oxygen-containing basic groups, and the loading of MgO. The maximum CO 2 capture capacity reached 1.29 mol·kg −1 under conditions of 273 K and 1 bar, with the mechanism of action being a synergistic effect of physical and chemical adsorption. The CO 2 /N 2 selectivity is 40.28, and after five cycles, the adsorption capacity loss is significant at approximately 40%, necessitating further improvement. DFT calculations indicate that enhancing the affinity between MgO/BMBC and CO 2 and facilitating electron transfer reduces the adsorption energy, thereby improving CO 2 capture performance. This study provides a new strategy for the preparation of highly efficient, low-cost solid CO 2 adsorbents.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Taozhong Zhang,Wanzhong Yin,Jin Yao,Wenju Sun,Xiaoqi Ban,Weifan Du
Glutathione (GSH) was first introduced for efficient pyrite depression under neutral pH conditions. • GSH enabled efficient flotation separation of molybdenite from pyrite, maintaining high selectivity. • GSH interacted with pyrite through dominant Fe–S coordination and markedly enhanced surface hydrophilicity. The selective separation of molybdenite from pyrite remains a longstanding challenge in sulfide flotation, while conventional lime-based alkaline depression is often associated with high reagent consumption, environmental concerns, and reduced molybdenite recovery. In this study, glutathione (GSH) was employed as a selective organic depressant for pyrite in a molybdenite–pyrite flotation system. At pH 7.0 and 40.0 mg/L GSH, micro-flotation tests showed excellent selectivity, reducing pyrite recovery to 2.75% while maintaining molybdenite recovery above 95%. Bench-scale flotation of an actual molybdenum ore confirmed the practical applicability of GSH, producing a Mo concentrate with 49.67% Mo grade and 81.28% recovery. The selective depression mechanism was clarified by integrating adsorption measurements, zeta-potential analysis, wettability measurements, XPS, and DFT calculations. The results revealed stronger interfacial affinity of GSH for pyrite than for molybdenite, enhancing pyrite hydrophilicity. XPS analysis indicated that –SH, –C=O, and –NH 2 groups participated in interactions with surface Fe sites, while DFT identified Fe–S coordination between –SH and surface Fe atoms as the dominant adsorption mode responsible for selective surface regulation and effective pyrite depression. These findings clarify the interfacial mechanism underlying GSH-mediated selective pyrite depression and provide a promising strategy for efficient molybdenite–pyrite flotation separation under neutral conditions. Download: Download high-res image (248KB) Download: Download full-size image
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Taoheng Zhang,Yuchen Liu,Jie Jiang,Chenyang Li,Wenze Guo,Ling Zhao,Zhenhao Xi
Polymeric ferric sulfate enables efficient esterification of 2,6-NDA to 2,6-NDC. • Polynuclear hydroxo iron clusters are identified as the catalytically active species. • Methoxy assisted proton transfer is proposed to lower the reaction energy barrier. • 2,7-NDA induced catalyst deactivation is clarified at the molecular level. Poly(ethylene naphthalate) (PEN) is a high-performance polyester renowned for its excellent barrier and mechanical properties. The production of high-molecular-weight PEN with superior mechanical performance is commonly achieved through the transesterification of dimethyl-2,6-naphthalenedicarboxylate (2,6-NDC), which is more readily purified than its acid counterpart. In this study, polymeric ferric sulfate (PFS) was developed as a highly efficient catalyst for the esterification of 2,6-naphthalenedicarboxylic acid (2,6-NDA) to 2,6-NDC. Under optimized conditions of 200 °C for 80 min with a catalyst content of 0.2 wt%, a conversion exceeding 95% was achieved. Deactivation studies and EPR spectroscopy, complemented by DFT calculations of the broken symmetry states, confirmed that the active species are polynuclear hydroxo complexed iron clusters exhibiting antiferromagnetic coupling. Mechanistic insights revealed that proton transfer mediated by methoxy groups significantly lowers the reaction energy barrier, a process validated by topological analysis. UV–Vis spectroscopy combined with TDDFT simulations further demonstrated the formation of catalytically active methoxy coordinated iron species in the methanolic PFS solution. This work provides a molecular level understanding of polynuclear iron catalysis for the synthesis of monomers for high performance polyesters. Download: Download high-res image (120KB) Download: Download full-size image Graphical abstract showing the catalytic mechanism of methyl esterification of 2,6-naphthalenedicarboxylic acid over polymeric ferric sulfate.
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ENVIRONMENTAL RESEARCH
·
2026
·
IF 8.2
Minghuan Wang,Hekai Zhang,Yunfei Song,Yilei Zhu,Yaning Zong,Peng Wei,Zheng Guo,Li Yin,Jianwei Fu
s The practical application of metal-organic framework (MOF)-derived catalysts in advanced oxidation processes (AOPs) is often hindered by challenges in recoverability and stability in complex water matrices. To overcome these limitations, we developed a scalable strategy to fabricate N-doped carbon nanofibers with coexisting atomic Co sites and metallic Co nanoparticles (Co-N/C) by electrospinning a ZIF-67/polyacrylonitrile (PAN) composite followed by controlled pyrolysis. This integrated design yields a catalyst with a hierarchical porous structure and a high specific surface area (317.55 m 2 g -1 ), which synergistically enhances mass transfer and exposes abundant active sites. The optimized Co-N/C catalyst demonstrates ultrafast catalytic activity, achieving over 98% degradation of methylene blue (MB) within 5 minutes via efficient peroxymonosulfate (PMS) activation. Mechanistic studies, supported by quenching experiments and density functional theory (DFT) calculations, reveal that the degradation proceeds via a nonradical-dominated pathway, with singlet oxygen ( 1 O 2 ) generated through interfacial electron transfer playing the primary role, while sulfate (SO 4 • - ) and hydroxyl (•OH) radicals from Co 2+ /Co 3+ redox cycling serve a secondary function. The catalyst exhibits excellent operational robustness, maintaining high efficiency (>92%) across a broad pH range (3-9) and showing remarkable reusability with minimal activity loss over five consecutive cycles. Furthermore, ecological structure-activity relationship (ECOSAR) modeling indicates a significant reduction in the environmental toxicity of the degradation intermediates. This work provides not only an effective and eco-friendly candidate for dye wastewater remediation but also fundamental insights into the rational design of MOF-derived functional materials for superior, nonradical-predominant AOPs.
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高影响因子
FOOD RESEARCH INTERNATIONAL
·
2026
·
IF 8.8
Xiangfei Hu,Qiannan Jiang,Zongcai Tu,Yueming Hu,Hui Wang
Pulsed electric field accelerated oxidation of arginine and glutamic acid. • Arginine had higher susceptibility to electric field due to its charged guanidino. • Density functional theory revealed electric field-altered oxidation pathways. • Electric field reduced energy barriers of β-cleavage through electronic polarization. Pulsed electric field (PEF) processing promoted oxidation of charged residues of proteins, while its mechanism remained vague. In this study, polarization and oxidation of arginine (Arg) and glutamic acid (Glu) induced by PEF treatment (5–20 kV/cm for 4 h) was investigated through experimental characterization and density functional theory (DFT) computation. The results demonstrated that PEF treatment restrained the vibrational dipole moment of N H and C O within Arg and Glu side-chain, respectively. In Arg, H 4 -H 6 signals shifted to a lower magnetic field with pronounced broadening, while C 1 , C 4 , C 5 , and C 7 shifted to a higher magnetic field accompanied by the appearance of C=N-related resonances. In contrast, Glu's carbon skeleton shifted slightly to a lower magnetic field without structural conversion. Furthermore, residues were oxidatively degraded with electric field intensity extended, accompanied by impaired positive of Arg and negative charge of Glu. DFT revealed strong polarization of electron distribution within molecular framework, where 0.017 a.u. treatment partially detached the electrons from backbone of carbon-centered radicals. Thermodynamic calculations verified that electric-field alignment with molecular dipoles markedly reduced the energy barrier of β-cleavage, yielding distinct volatile profiles characterized by multi-site cleavage and N-heterocycle in Arg, and predominant aldehydes and acids in Glu. These findings clarified electric field-induced oxidation pathways and provided the theoretical guidance of PEF processing for improved quality stability. Download: Download high-res image (151KB) Download: Download full-size image
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·124912
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IF 7.5
Yichang Qin,Jiesheng Hong,Hangrui Zhang,Xiaotao Peng,Gang Lu
This study investigated the degradation of three sulfonamide antibiotics, sulfamethizole (SMT), sulfapyridine (SPD), and sulfadiazine (SDZ), in a UV/peracetic acid (UV/PAA) system and developed an interpretable machine learning framework to predict their normalized concentration (C/C 0 ) evolution. UV/PAA markedly accelerated degradation compared with UV or PAA alone, with pseudo-first-order rate constants following the order SPD (0.331 min −1 ) > SMT (0.273 min −1 ) > SDZ (0 .1 53 min −1 ). UPLC-QTOF-MS and DFT analyses indicated common transformation pathways but distinct electronic characteristics among the three sulfonamides. The prediction framework integrated a full feature set comprising six reaction variables and three DFT-derived molecular descriptors. The reaction variables included UV intensity, PAA concentration, reaction time, UV fluence, PAA exposure, and UV-PAA coupling. Among six regression models evaluated using curve-level partitioning, support vector regression (SVR) achieved the best performance and maintained high predictive accuracy in the independent hold-out validation set (R 2 = 0.963). Ablation analysis showed that the combined reaction variables provided marginal improvement, whereas the DFT-derived molecular descriptors substantially enhanced prediction. SHAP analysis identified reaction time, UV fluence, and PAA exposure as the dominant contributors, while the molecular descriptors captured electronic differences. The approach provided an interpretable basis for predicting sulfonamide degradation performance and could support water treatment optimization.
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高影响因子
Materials Today Chemistry
·
2025
·
IF 6.7
Shouyu Lu,Lei Sun,Shun Liu,Ping He,Jiang Wu,Mei Ma,Yang Ling,Hong Yao,Guangqian Luo,Dapeng Wang
A Fe 2 O 3 /CaSiO 3 composite adsorbent was synthesized using calcium nitrate as a precursor for the adsorption and removal of As 2 O 3 from high-temperature flue gas at temperatures ranging from 1073 K to 1273 K. A combination of experimental investigations and theoretical calculations was employed to analyze the impact of Fe-doped calcium silicate on its arsenic adsorption performance, as well as to elucidate the adsorption mechanism of the Fe 2 O 3 /CaSiO 3 composite material for As 2 O 3 . The experimental results demonstrated that the incorporation of Fe 2 O 3 resulted in an enhanced pore structure within the material. When the molar ratio of Fe:Si was set at 1:5, the Fe 2 O 3 /CaSiO 3 adsorbent exhibited optimal As 2 O 3 adsorption capacity at 1273 K, achieving a remarkable value of 996.0 mg/kg—significantly higher than that observed with pure calcium silicate. During the adsorption process, the doped iron oxide released additional free electrons, thereby facilitating the conversion of lattice oxygen into chemisorbed oxygen. Furthermore, density functional theory (DFT) calculations were utilized to further investigate the microscopic mechanisms underlying the behavior of the Fe 2 O 3 /CaSiO 3 composite adsorbent. The findings indicated that Fe sites within Fe 2 O 3 /CaSiO 3 served as primary active sites and electron transport channels for this material, promoting both separation and conversion processes involving lattice oxygen. During arsenic adsorption, significant orbital hybridization occurred between Fe atoms and O atoms in As 2 O 3 , which contributed to enhancing stability within the chemisorption system. Overall, Fe 2 O 3 /CaSiO 3 displayed exceptional performance in terms of arsenic adsorption capabilities along with notable anti-sintering properties, positioning it as a promising composite material for effective arsenic removal under high-temperature conditions.
研究领域:
环境科学
·
材料科学
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危险品化学品经营许可证（带存储）