Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Lingchao Kong,Qinyu Wang,Yeyin Zhang,Yi Wang,Chunmiao Zheng
The rapid expansion of the textile dyeing industry has created an urgent need for high-performance dye wastewater treatment materials due to the limitations of traditional adsorbents in efficiency and separability. Herein, we report the synthesis of ultralight, cost-effective aerogel adsorbents by introducing triethylenetetramine (TETA) into α-cellulose (CU). The resulting CU/TETA-0.25 aerogel displays outstanding adsorption capacities for Congo Red and indigo dyes, reaching 575.7±20 mg/g and 516.4±20 mg/g, respectively. Remarkably, less than 1 g of this aerogel continuously filters over 35 L (50 mg/L) of deeply colored red–blue dye wastewater to near transparency. Its high adsorption efficiency remains stable even under simultaneous exposure to multiple ions, organic compounds, and pH fluctuations. Mechanistic insights, derived from SEM, EDX, and XPS analyses and first-principles calculations (including molecular structure optimization, frontier molecular orbital distribution, weak interaction, and charge density difference), confirm that the –OH and –NH₂ groups on CU/TETA-0.25 drive dye adsorption through hydrogen bonding, supplemented by electrostatic and van der Waals interactions. Owing to its mass-producibility, lightweight nature, and low cost, CU/TETA-0.25 holds great promise for large-scale applications in mitigating water pollution caused by mixed dyes.
研究领域:
环境科学
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材料工程
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吸附技术
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计算化学
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废水处理
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Heng Lin,Zhouheng Xia,Kunpeng Xue,Xiaojing Zhou,Yifan Yao,Na Ma,Wei Dai
To address the challenge of balancing adsorption kinetics and capacity for the capture and separation of PFOA, there is an urgent need for the development of MOF materials with defect-free crystal structures and a well-defined hierarchical “micro-mesoporous” pore structure. This will enhance the performance of fast adsorption rates, high adsorp-tion capacity, and high selectivity. In this study, we report a core-shell structure UiO-66-NH2-on-MIL-101(Cr) composite material, which achieves efficient PFOA ad-sorption and exceptional environmental stability through the synergistic effects of Zr4+/Cr3+ unsaturated metal sites, the amino-functionalization of UiO-66-NH2, and the optimization of high surface area (SBET = 1927 m2/g) with a hierarchical pore structure (micro- mesoporous cooperation). Density functional theory (DFT) calculations, com-bined with XPS and FT-IR analysis, reveal that the primary adsorption mechanism in-volves strong coordination interactions between the PFOA carboxylate groups and met-al clusters (Cr/Zr-O) (Eb = -178.02/-121.72 kcal/mol), supplemented by hydrogen bonding (O-···H-N/H-O), π-CF hydrophobic interactions, and electrostatic attraction (verified by changes in Zeta potential (Δζ = 36.1 mV) and electrostatic potential (ESP)). Batch experiments show that at pH = 3, an adsorbent dose of 14 mg, and room temper-ature (298 K), the composite material exhibits remarkable adsorption capacity (qmax = 860 mg/g), following pseudo-second-order kinetics and Langmuir adsorption isotherms. Thermodynamic analysis confirms that the adsorption process is exothermic (ΔH = -16.33 kJ/mol) and spontaneous (ΔG < 0), with the entropy-driven hydrophobic effect offsetting some of the exothermic contributions. In extreme environmental tests (pH = 2/12, 100°C boiling water), the composite maintains its crystal structure and adsorption performance (XRD/SEM), exhibiting a capacity retention rate exceeding 85% after five regeneration cycles. This study presents a new strategy for designing PFOA adsorbents with dual metal node electronic synergistic and coordination microenvironment optimi-zation, multi-scale topological stability construction, and molecular recognition mecha-nisms, offering significant environmental application value.
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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吸附技术
✓ 已验证
DOI
高影响因子
Journal of Hazardous Materials Advances
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2023
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IF 0
Shahzad Afzal,Andleeb Mehmood,Lingyue Jin,Ke Pan,Munir Ahmad,Dandan Duan,Yang Wei,Waseem Raza,Tianwei Hao,Hafiz Muhammad Adeel Sharif,Muhammad Sohail,Fengyuan Chen
An economical and environment-friendly material as a catalyst is highly desirable to activate peroxymonosulfate (PMS) into reactive oxygen species (ROS). Cobalt-doped dumbbell-shaped manganese oxide (CoX˗MnO x where X = 1.0, 6.0, 12.0, 18.0, and 24.0 mM) was synthesized as a PMS-activator for degrading organic pollutants in wastewater. We have developed a green, facile, and low-temperature route without any organic solvents, and templates to synthesize Co-doped dumbbell-shaped MnO x with hierarchical porosity. It is the first-ever research to use these materials for peroxymonosulfate activation. The microstructure contained nanoparticles that self-assembled into a maze-like dumbbell-shaped mesostructure. Phenol degradations after 9 min of Co18-MnO x /PMS, MnO x /PMS, Co 3 O 4 /PMS, PMS, and adsorption were 100%, 27%, 33%, 17%, and 5%, respectively. The Co18-MnO x morphology, microstructure, textural properties, and catalytic efficiency were well-retained after recycling. Compared to SO 4 ·− and · OH, 1 O 2 and O 2 ·− were the dominant ROS. The balance among redox couples of different species (Co 2+ /Co 3+ , Mn 3+ /Mn 4+ , O 2− /O 2 ) and PMS decomposition enabled ROS production. The high catalytic activity was assigned to the Mn/Co synergism, hierarchical microstructure, and ROS. Furthermore, the DFT study investigated the difference between the activation mechanism of PMS (adsorption and electron transfer) on MnOx and Co-MnOx surfaces. Our research devised a facile procedure to synthesize other transition metals doped MnO x for advanced oxidation processes and multipurpose applications.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yixin Pan,Bo Sun,Yingying Zhou,Jian Jiao,Liping Deng,Xiaowu Dong
This study reported a Ni 0 @ZIF-8 nanocomposite synthesized via co-precipitation that synergistically integrated the high adsorption capacity of ZIF-8 with the redox activity of zero-valent nickel (Ni 0 ) for efficient uranium(VI) extraction. The composite with an optimized 1:1 ZIF-8:Ni 0 molar ratio achieved an exceptional adsorption capacity of 830.5 mg/g. Kinetic and thermodynamic analyses confirmed chemisorption-dominated monolayer adsorption following pseudo-second-order kinetics (R 2 > 0.999) and spontaneous endothermic behavior. Mechanistic investigations through spectroscopy and density functional theory (DFT) calculations revealed a dual-function mechanism that ZIF-8 facilitated U(VI) capture through electrostatic/coordination interactions, while Ni 0 mediated partial reduction of U(VI) to U(IV) via electron transfer, enhancing immobilization stability. Notably, only Pb 2+ , Cu 2+ , Cr 6+ , and organic ligands inhibited adsorption through redox competition and solution complexation. Comparative studies demonstrated minimal matrix interference-deionized water versus seawater systems exhibit merely 4.7 % deviation in adsorption efficiency at trace U(VI) concentrations (0.1–0.6 mg/L). Critically, direct uranium extraction from unprocessed natural seawater (ambient U: 4.27 μg/L) with only pH adjustment (5.0) achieves 86.02 % efficiency at ultra-low adsorbent dosage (0.001 g/L), yielding residual uranium concentrations of 0.597 ± 0.04 μg/L. By harmonizing adsorption and redox pathways, Ni 0 @ZIF-8 overcome limitations of conventional materials, establishing itself as a paradigm-shifting solution for uranium remediation in complex ionic matrices and real marine environments.
研究领域:
环境科学
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材料化学
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核化学
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水体修复
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密度泛函理论
✓ 已验证
产品关联
DOI
高影响因子
HYDROMETALLURGY
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2023
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IF 4.7
Changye Mang,Guanghui Li,Yanhu Chen,Jun Luo,Mingjun Rao,Tao Jiang
Partial neutralization is typically used to remove Fe 3+ ions from the acid leach solution of laterite. However, during this process, significant amounts of Mg 2+ , Ni 2+ , Co 2+ , and SO 2– 4 are lost. With increasing initial Fe 3+ concentration and solution pH, the severity of loss increases, with the precipitation of Fe 3+ . In this study, the mechanisms of ion co-precipitation during partial neutralization were investigated. Based on density functional theory calculations, a precipitation pathway through the formation of [Fe 4 (OH − ) 2 (SO 2– 4) 4 ]•[2SO 2 – 4 •yH 2 O]•[M 2+ ] was proposed. The differential charge density diagram indicated that the O atoms acted as the charge acceptors and maintained the precipitate structure. The coordination between M 2+ and SO 2– 4 could be destroyed via intense agitation, releasing approximately 100% of Mg 2+ , Ni 2+ , and Co 2+ ions from the precipitates to the solution. Furthermore, the addition of cationic or anionic surfactants limited the formation of these coordination bonds. The highest retention percentages of Mg 2+ , Ni 2+ , and Co 2+ in solution were 99.4, 99.6, and 99.9%, respectively, after adding 2 × 10 −5 mol/L of sodium dodecylbenzenesulfonate (CTAB). In addition, a high temperature could break these coordination bonds. The retention percentages of Mg 2+ , Ni 2+ , and Co 2+ increased from 82.6, 85.2, and 86.5% to 99.9, 99.6, and 99.8%, respectively, as the temperature increased from 25 to 65 °C. These results confirmed the rationality of the proposed structure of the precipitate.
研究领域:
化学工程
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材料科学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yongjun Song,Aimin Wang,Songyu Ren,Yanyu Zhang,Ruiyan Fan,Ying Liu,Zhongguo Zhang
The utilization of hybrid electro-Fenton (EF) processes has gained considerable attention, which can combine the advantages of two or more treatment methods resulting in efficient removal of refractory pollutants from water. Here, an electro-controlled membrane coupling heterogeneous EF (EM-HEF) system was constructed for the degradation of acetaminophen (APAP) in water. In the EM-HEF system, a bifunctional ACF/CC-FeOCl-Cu cathode material was synthesized to enhance the HEF reaction, while a tubular Ti microfiltration membrane was used as both cathode and membrane. Degradation experiments indicated the EM-HEF system exhibited remarkable removal efficiency (97.0 %) towards APAP within 30 min under the conditions of flow rate at 60 mL min −1 , initial pH at 7.1, and current density at 3 mA cm −2 . Notably, the cathode materials showed low metal leaching rate and high APAP removal rate in the 10 cyclic experiments. The common inorganic anions (Cl − , HCO 3 − , HPO 4 2− , and NO 3 − ) did not inhibit the removal of APAP significantly, whereas humic acid exhibited a more pronounced inhibitory effect only at concentrations exceeding 10 mg L −1 . Quenching experiments and electron spin resonance (ESR) tests confirmed the pivotal role of hydroxyl radicals in the decomposition of APAP. Combining density functional theory (DFT) and LC-MS results, three pathways were proposed. The overall toxicity of intermediates was relieved during EM-HEF degradation of APAP. Furthermore, it also achieved good performance in the treatment of landfill leachate, with increasing BOD 5 /COD ratio from 0.11 to 0.34. This work provides an efficient strategy for the removal of refractory pollutants in water.
研究领域:
环境科学
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水处理
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化学工程
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材料科学
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计算化学
✓ 已验证
产品关联
DOI
高影响因子
Computational and Theoretical Chemistry
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2025
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IF 2.8
Xianliang Gong,Yue Zhang,Zhouyu Jiang,Cunbin Du,Arshad Khan,Rabia Usman
Charge transfer (CT) cocrystals formed via non-covalent interactions play a pivotal role in governing their optical behaviors. A CT cocrystals were synthesized using 1,2,4,5-tetracyanobenzene (TCNB) as the electron acceptor and chalcone (E)-3-(anthracen-9-yl)-1-(pyridin-3-yl)prop-2-en-1-one (A3BPO) as the electron donor. Structural analysis through single-crystal X-ray diffraction (SC-XRD) unveiled that this cocrystal predominantly comprise a mixed stacking arrangement guided by face-to-face π···π interactions, with the overall stability of CT cocrystal stacking bolstered by auxiliary hydrogen bonds. The relationship between structure and properties was scrutinized using various analytical techniques including Powder X-ray diffraction (PXRD), FT-IR, UV–visible absorption, and fluorescence spectroscopy. Density functional theory (DFT) simulations elucidated that the modified optical properties primarily stem from CT between acceptor and donor. These findings contribute significantly to a clearer understanding of how stacking modes in CT cocrystals influence the interplay between CT and optical properties.
研究领域:
材料科学
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物理化学
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晶体工程
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光学材料
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理论化学
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有机电子学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Jun Yao,Zhuang Xie,Xiang Zeng,Li Wang,Tingting Yue
Cholesterol is one of the most significant indicators to assess health status. Lanthanide metal-organic frameworks (Ln-MOFs) have a unique luminescence mechanism, which makes it possess tremendous potential in biomonitoring. Thus, on the basic of intramolecular charge transfer theory and quenching effect, the metal-organic frameworks (MOFs) doped by europium was constructed to respond to the cholesterol in serum. The charge transfer direction and the sensing mechanism of fluorescent probe were explained in detail by cross-corroboration of experiment and calculation. The possible sensing mechanism was explained at the molecular level with density functional theory (DFT). With the excitation of 350 nm, the emission peaks at 458 nm and 615 nm which corrsponded to MIL-53(Fe) and Eu centers, appeared enhancement and quenching respectively. To investigate the emission law, the density of states and partial density of states were used to explain the internal electron migration of the probe and the possible sensing mechanism. The results showed the electron transfer efficiency of MIL-53(Fe) was enhanced after Eu 3+ doping, which brought a remarkable improvement in response sensitivity. Meanwhile, the higher energy possessed by the excited state of Eu will lead to the capture of its own electrons by hydrogen peroxide, thus reducing the number of electrons returned to the ground states of Eu and eventually leading to the fluorescence quenching of 615 nm. We anticipate the proposed research is to be an emerging method in cholesterol determination and have further development in all walks of life.
研究领域:
生物化学
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材料科学
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分析化学
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计算化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Shi-Xian Guan,Tao Xu,Jian-Yong Zhang,You-Guo Luo,Xingwu Zhai,Na Zhang,Yong-Zheng Fang,Qin-Fei Ke
Herein, we developed a multimodal antibacterial nanoplatform via synergism effect including knife-effect, photothermal, photocatalytic induced reactive oxygen species (ROS), and Cu 2+ inherent attribute. Typically, 0.8-TC/Cu-NS possesses higher photothermal property with the higher photothermal conversion efficiency of 24% and the moderate temperature up to 97 °C. Meanwhile, 0.8-TC/Cu-NS exhibits the more active ROS, 1 O 2 and ·O 2 - . Hence, 0.8-TC/Cu-NS possesses best antibacterial properties against S. aureus and E. coli in vitro with efficiency of 99.94%/99.97% under near-infrared (NIR) light, respectively. In the therapeutic practical use for wound healing of Kunming mice, this system exhibits outstanding curing capacity and good biocompatibility. Based on the electron configuration measurement and density functional theory (DFT) simulation, it is confirmed that the electrons on CB of Cu-TCPP flow fleetingly to MXene trough the interface, with redistribution of charge and band upward bending over Cu-TCPP. As a result, the self-assembled 2D/2D interfacial Schottky junction have made great favor to accelerate photogenerated charges mobility, hamper charge recombination, and increases the photothermal/photocatalytic activity. This work gives us a hint to mostly design the multimodal synergistic nanoplatform under NIR light in biological applications without drug resistance.
研究领域:
材料科学
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纳米技术
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生物医学工程
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化学
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生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sustainable Materials and Technologies
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2024
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IF 8.6
Lei Guo,Yan-He Chen,Li-Mei Xu,Xiao-Lu Chen,Jin-Qiu Shen,Jian-Yong Zhang,Zhen-Jiang Liu
Herein, a fern-like p-n heterojunction by anchoring Ni 3 Fe-LDH nanoplates onto Co 3 O 4 nanoneedles have been optionally constructed. Essentially, p-n heterojunction ensured to induce strong built-in electric field, and inherit interfacial electron redistribution. Based on their compatible and well-matched electronic band structures, a staggered type-II photo-generated electron/holes transfer pathway have been elaborated by density functional theory calculation (DFT), in situ irradiation X-ray photoelectron spectroscopy (XPS), and fluorescent decay. This band bending and charge migrating module conferred the architecture with strong redox ability, sufficient exciton dissociation, and admirable optoelectronic characteristics. Moreover, the heterostructure acquired broad absorption spectrum to exhibit outperforming photocatalytic effect. Totally, this electron redistribution at the hierarchical interface, a type-II scheme charge-transfer pathway and the oxygen defects would lead to high efficiency in solar light assisted N 2 reduction. Typically, Co@Ni 3 Fe-2 catalyst exhibited the highest NH 3 production rate of 16.15 μg h −1 mg cat. −1 and Faraday efficiency (FE) of 31.57% at −0.6 V vs. RHE in 0.1 M Na 2 SO 4 solution. Fortunately, with light exposure, the NH 3 production rate and FE could increase by 27.9% and 18.1% than that under dark. This work would provide a plausible attitude towards the design of high efficient photocatalyst for artificial photosynthesis with multi-functionalized coupling effect.
研究领域:
材料科学
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催化
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光化学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Zhaoying Li,Feixing Li,Yaohui Fan,Zijun Zhang,Mengyu Wan,Songsong Zhang,Lianghuan Wei,Weizun Li,Xianghao Zha
Co-pyrolysis of polypropylene (PP) waste and cotton stalks (CS) addresses the dual environmental challenges of plastic pollution and agricultural residue disposal while leveraging their complementary properties (PP: H-rich; CS: C, O-rich) for enhanced H 2 production. This study investigated the hydrogen production mechanism of lignocellulose via microwave-assisted catalytic fast co-pyrolysis (co-MACFP) experiments and density functional theory (DFT) theoretical calculations for the conversion of CS and PP. Co-MACFP (550 °C) with a SiC absorber was applied to PP-CS blends (1:1 ratio), mesoporous HZSM-5 (tetrapropylammonium hydroxide (TPAOH)-modified, HT-1.0), and Ni-loaded HT-1.0 catalysts. The reaction mechanisms were determined via DFT simulations using β- d -glucopyranose and propylene as molecular models. The concentration of H 2 obtained from the co-pyrolysis of CS and PP (the ratio is 1:1) was 32.7 vol% without catalysts, which exceeds the average concentration of 28.4 vol% ((27.1 + 29.7)/2) at 550 °C, indicating a synergistic effect between CS and PP. In addition, synergistic effects boost the H 2 yield to 38.0 vol% with Ni-HT1.0 (vs. 32.7 vol% without catalysts), exceeding the theoretical averages from the individual feedstocks. PP-derived H· radicals (energy barrier: 454.8 kJ/mol) attack CS intermediates as the dominant low-energy pathway (204.4 kJ/mol), suppressing CO/CO 2 formation via DFT. This integrated strategy enables efficient waste valorization and generation of green hydrogen. Future work should scale up catalyst synthesis and explore hybrid processes to improve economic viability.
研究领域:
化学工程
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环境科学
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材料科学
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能源技术
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计算化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Chemistry and Ecotoxicology
·
2025
·
IF 8.2
Gao Feiyue,Zhou Chuncai,Li Chen,Xu Shihai,Li Zhiguo,Li Xin,Liu Guijian
The novel ultra-micro porous carbon sheet (PCs) with exceptionally high surface area (3034 m 2 /g) were synthesized through green potassium citrate (K 3 C 6 H 5 O 7 ) activation for efficient thallium(I) [Tl(I)] removal from wastewater. The static adsorption results revealed that PCs achieved exceptional removal efficiencies above 95 % across pH 6–12, maintained high selectivity against competing ions (K + , Na + , Cl − , F − ) and organic interferents, and retained above 80 % capacity after five regeneration cycles. Adsorption followed Pseudo-second order kinetics and Freundlich isotherm models, indicating multilayer adsorption on heterogeneous surfaces, with thermodynamics confirming spontaneous exothermic processes. The density functional theory (DFT) calculation results demonstrated that lone pair electrons involved in complexation and π-electrons participating in coordination were supplied by oxygen-containing functional groups and aromatic rings, respectively. The sorption mechanisms included surface complexation, ion exchange, electrostatic attraction, and cation-π interaction. The column sorption results demonstrated the influent flow rate, bed height, and initial Tl(I) concentration-dependent removal performance. The Tl(I)-containing wastewater at ppm level could meet the discharge standard by optimizing influent flow rate and bed height in column adsorption. The dynamic sorption process was described properly by Thomas and Yoon-Nelson models. This study provides a systematic theoretical foundation for designing porous carbons in Tl-contaminated water remediation.
研究领域:
环境科学
·
材料工程
·
水处理技术
·
物理化学
·
计算化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）