JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Ming-Xing Li,Yan-Shu Xiong,Qi-Qi Huang,Yi-Wen Luo,Wei Wei,Hai-Qin Lu,Fang-Xue Hang,Wen Li,Fujie Liu,Kai Li
Wastewater contains various organic contaminants that pose great hazards to human health and the environment. A protein/polysaccharide-derived aerogel, namely, ICMA, was developed as a high-performance adsorbent for the simultaneous and efficient removal of diverse contaminants from wastewater, including melanoidin (MLE), Congo red (CR), and diclofenac (DIC). Metal organic framework (UiO-66-NH 2 ), as a regulatory factor, significantly improved the porosity and pore volume of the ICMA to enhance the capture performance of contaminants. The ICMA exhibited outstanding adsorption efficiency owing to the incorporation of ample polyamine functional groups and its well-developed pore structure, large porosity and pore volume, and remarkable heat resistance. The equilibrium capture capacities of the ICMA were 1364, 2031, and 539 mg/g for MLE, CR, and DIC, respectively, with corresponding removal efficiencies all exceeding 90%. Furthermore, the ICMA can capture cationic dyes through MLE/CR/DIC-bridging interactions. After five cycles, the used ICMA can still maintain a high contaminant removal rate/amount, demonstrating good reusability. The classic adsorption model showed that the capture of contaminants by the ICMA is a double-layered and heterogeneous adsorption orientation. A brand new LWAMTM model demonstrated that the adsorption mass–transfer process is jointly determined by the external mass conveyance, pore diffusion, and adsorption on the active site. Multiple characterizations indicated that the contaminant adsorption onto the ICMA was mainly facilitated by charge interactions, with H-bonds playing a secondary role. Quantum chemical theory simulations further provide insights into the atomic-level mechanisms involved in the capture of contaminants. Hirshfeld surface analysis revealed that the ICMA functions as both an H-bond acceptor and a donor during contaminant adsorption. Scale-up and upgrade adsorption were performed to treat actual/simulated wastewater, establishing the groundwork for the industrial implementation of the ICMA.
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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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Ahsan Nazir,Ameena Tur Rasool,Chuntao Chen,Otabek Mukhitdinov,Doniyor Jumanazarov,Dongping Sun
In this study, novel Z-scheme AgI@PbBiO 2 Br heterojunctions were prepared using a simple in situ precipitation approach to effectively degrade organic pollutants and inactivate gram-negative Escherichia coli (E. coli) and gram-positive Staphylococcus aureus (S. aureus) bacteria when exposed to visible light. The prepared materials were comprehensively evaluated using several analytical procedures. The 20 %-AgI@PbBiO 2 Br presented the best photocatalytic performance of all the catalysts prepared. The rhodamine B (RhB) molecules were significantly reduced within 70 min (98.72 %), showing a much higher degradation efficiency than bare AgI (73.58 %) and PbBiO 2 Br (46.77 %) under the same conditions. The degradation of methyl orange (MO), neutral red (NR), and tetracycline (TC) by 20 %-AgI@PbBiO 2 Br was also examined, resulting in nearly total elimination of MO, NR, and TC pollutants, respectively. In addition, the antibacterial efficacy of 20 %-AgI@PbBiO 2 Br against E. coli and S. aureus reaches about 99.99 %. The improved photodegradation efficacy of AgI@PbBiO 2 Br is owing to the construction of a heterojunction between AgI and PbBiO 2 Br, which increases effective charge separation and visible light absorption, thus enabling the decomposition of pollutants. Cycling experiments confirmed the stability and reusability of the material, demonstrating exceptional photocatalytic durability. The photocatalytic mechanism was thoroughly examined by reactive species capture assays and ESR analysis, confirming that holes and superoxide radicals are crucial in the photodegradation system. Additionally, the density functional theory (DFT) simulations and liquid chromatography-mass spectrometry (LC-MS) helped to clarify the susceptible active sites and possible degradation pathways of RhB. Overall, this work underlines the considerable ability of AgI@PbBiO 2 Br heterojunctions to effectively remove persistent pollutants from wastewater.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120938
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IF 7.2
Jinmei He,Mengge Cao,Jiehui Li,Dachuan He,Yuhang Gao,Menglin Zhu,Jin Zhang,Lei Zhu,Mengnan Qu
In recent years, the increasing discharge of microplastics (MPs) and oil pollutants into aquatic environments has posed serious ecological and health concerns, driving the urgent need for efficient and sustainable removal technologies. In response to this challenge, this study successfully prepared a multifunctional superhydrophobic sponge (HFNA) with photothermal conversion capability and magnetic responsiveness via a simple dip-coating method, which can be used for the adsorption of microplastic particles (MPs) and oil pollutants in aquatic environments. By introducing polydopamine (PDA) onto the melamine sponge (MF) skeleton, incorporating high specific surface area Ni-MOF, and adding Fe 3 O 4 with magnetic driving capability, the material’s adsorption capacity toward MPs was enhanced. The HFNA achieved a maximum removal efficiency of 99.3 % for MPs and exhibited excellent removal performance for various oil pollutants, while its photothermal effect effectively reduced crude oil viscosity, improving adsorption efficiency. Subsequently, the adsorption mechanism of the material was further revealed through density functional theory (DFT) calculations. The analysis showed that Ni-MOF and MPs exhibit excellent HOMO-LUMO energy level matching, with a small energy gap (ΔE gap ), facilitating electron transfer from MPs to Ni-MOF. At the same time, electrostatic potential and charge distribution maps indicated the presence of multiple high electron affinity sites on the surfaces of Fe 3 O 4 and Ni-MOF, which help in the enrichment of MPs. Theoretical results were highly consistent with experimental data, establishing a complete correlation mechanism from electronic structure to adsorption performance and material construction, thus providing important theoretical support for the rational design of MOF-based adsorbent materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Juntian Li,Zhiling Xu,Junhui Zhou,Xinjie Wang,Jiachun Cao,Qianyu Li,Teng Wang,Juan Li,Didi Li,Zhimin Ao
Designing multifunctional catalysts for low-temperature co-oxidation of volatile organic compounds (VOCs) and CO is challenging, as conventional catalysts cannot simultaneously achieve VOCs activation and CO poisoning resistance below 200 °C—where CO preferentially adsorbs and severely inhibits VOCs oxidation. Herein, we proposed a density functional theory (DFT)-guided atomic engineering strategy integrating d-band center modulation and adsorption energy screening to construct metal-organic frameworks (MOFs)-hosted Au-Pt single-atom alloys (SAAs). By leveraging the coordination confinement of UiO-66 to stabilize Au-Pt SAAs sites, the optimized Au-Pt SAAs/UiO-66 catalyst achieved exceptional performance in co-oxidation of toluene and CO, attaining 90 % toluene conversion at 160 °C with robust stability under CO-poisoning conditions. Mechanistic studies and DFT calculations revealed that atomically dispersed Au sites induced Pt δ− -Au δ+ charge polarization on Pt nanoparticles charge polarization via interfacial electron transfer, weakening CO adsorption while enhancing toluene activation through dual-pathway mechanisms (Eley-Rideal and Langmuir-Hinshelwood) mechanisms. This synergy decouples the traditional trade-offs between activity and stability, offering a 4.7-fold higher turnover frequency than conventional Pt catalysts. Our work established a paradigm for electronic cooperativity in MOF-hosted SAAs, providing atomic-level insights into the design of multifunctional catalysts for environmental remediation.
研究领域:
催化
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材料科学
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环境化学
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理论化学
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纳米技术
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xianhong Deng,Wenbin Wu,Shuangqin Tian,Yi He,Shujie Wang,Bifang Zheng,Kai Xin,Ziqin Zhou,Lihong Tang
In this study, we employed a straightforward in-situ synthesis strategy to fabricate multi-site adsorption functional composites known as aminated chitosan@ZIF-8 (AmCs@ZIF-8) for the efficient removal of Cu(II) and Congo red. The AmCs@ZIF-8 adsorbed Cu(II) at pH 5 and Congo red at pH 3 with excellent removal efficiency values of 94 % and 100 % respectively. The maximum adsorption capacity for Cu(II) and Congo red are obtained as 785 mg g −1 and 1156 mg g −1 , respectively. Interestingly, AmCs@ZIF-8 composites exhibited an excellent removal efficiency (>80 %) after reusing them for four sequential cycles. Analysis of the adsorption isotherm and kinetic data indicated that chemisorption primarily governed the adsorption of Cu(II) and Congo red by AmCs@ZIF-8. Furthermore, we elucidated the adsorption energy of Cu(II) and Congo red on the AmCs@ZIF-8 composite through density functional theory. Specifically, the adsorption energy values for Cu(II) with AmCs and ZIF-8 were −20.907 and −57.809 kcal·mol −1 , and −26.514 and −16.242 kcal·mol −1 for Congo red, respectively. The efficient adsorption mechanism of Cu(II) and Congo red on the AmCs@ZIF-8 composite can be attributed to the synergistic effects of chelation, electrostatic attraction, ion exchange, and hydrogen bonding through the analysis of experimental characterization and theoretical calculation. Therefore, AmCs@ZIF-8 composites elevate the adsorption capacity of Cu(II) and Congo red in a single-component system and exhibit high removal efficiency (>90 %) in the context of the Cu(II)-Congo red binary system.
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APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Ruiqi Ge,Bingqiao Yang,Bing Deng,Hui Shao,Yimei Xiao,Rudolph Martin,Huihua Luo,Hanquan Zhang
The efficient removal of dolomite from phosphate ores is vital for the subsequent production of phosphate fertilizer. This work investigated the interaction mechanism of poly(sodium styrene sulfonate) (PSS) on apatite and dolomite surface and its implication on flotation through Micro-flotation, adsorption capacity, Zeta potential, SEM-EDS and density functional theory simulation. Flotation results proved that PSS was able to depress dolomite efficiently in broad pH range (8–12). Contact angle, Zeta potential, adsorption capacity and SEM-EDS measurement confirmed that PSS was more prone to adsorb on dolomite rather than that on apatite, which hindered sodium oleate (NaOL) to adsorb on dolomite but almost didn’t influence NaOL to interact with apatite surface. DFT calculations confirmed that the 2p orbital of oxygen atoms within sulfonate groups hybridized with 4s orbital of calcium and 3s orbital of magnesium atoms on dolomite surface to form O Ca, O Ca and O Mg covalent bond, while PSS weakly physisorbed on apatite via electrical interaction, due to the significant difference in steric hindrance and active atom density. PSS exhibited good selectivity and environmental compatibility as dolomite depressant in the beneficiation of phosphate ores for sustainable production of phosphate fertilizer.
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Nanomaterials
·
2019
·Vol. 9
·期 2
·172
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IF 4.034
Xinyue Lao,Xiyu Li,Hans Ågren,Guanying Chen
Although all-inorganic CsPbX3(X = Cl, Br, I) perovskite quantum dots (PQDs) have evoked exciting new opportunities for optoelectronic applications due to their remarkable optical properties, their emission color tunability has not been investigated to any appreciable extent. In this work, double/triple CsPbX3perovskite quantum dots with precise ratios of Cl/Br or Br/I are synthesized and their luminescence (410–700 nm) is explored. A group of down-converted CsPbX3(X = Cl, Br, I) perovskite quantum dot light-emitting diode (LED) devices were constructed to demonstrate the potential use of such double/triple-halide CsPbX3perovskite quantum dots with full-spectrum luminescence. Based on density functional theory, we theoretically explored the properties of CsPbX3with double/triple anion atoms. The calculated band gaps provided strong support that the full-spectrum luminescence (410–700 nm) of double/triple CsPbX3can be realized with the change of the mixed-halide ratios, and hence that such PQDs are of potential use in optoelectronic devices.Keywords:perovskite quantum dots;light-emitting diode;density functional theory;band gap
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Chengyu Zhang,Zhisheng Yu,Xiangyang Wang,Bobo Wang
In this study, a novel γ-Fe 2 O 3 /biochar (BF γ ) composite by a plant in-situ enrichment and one-step pyrolysis strategy was prepared, which was applied as a photocatalyst to activate peroxymonosulfate (PMS) for the degradation of p-chlorophenol (4-CP) under visible light irradiation (BF γ /PMS/Vis) system. The characterization results exhibited that γ-Fe 2 O 3 with localized carbon doping was evenly embedded in biochar during the pyrolysis. BF γ exhibited better photoresponse properties than biochar (BC) and γ-Fe 2 O 3 . The removal efficiency of this system for 4-CP reached 96.41% under optimal conditions. This system showed high removal efficiency with a wide pH range (3.0–13.0) and under conditions of different organic pollutants . It also showed strong resistance to interference with co-existing inorganic ions and humic acid (HA). Electron paramagnetic resonance (EPR) and radical scavenging experiments revealed that the reactive oxygen species (ROS) in this system included SO 4 - ·, ·OH, ·O 2 - and 1 O 2 . The density functional theoretical (DFT) calculations further revealed the promotion of localized carbon doping in γ-Fe 2 O 3 on electron transfer and photoresponse, including C-O bond (d=1.29 Å), C-Fe bond (d=1.80 Å) and band gap value (E gap < 0.72 eV). This study provides new insights into constructing environmentally-friendly catalysts and the possibility of the solid waste recycling for other wetland plants.
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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.
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TRANSITION METAL CHEMISTRY
·
2020
·Vol. 45
·期 4
·279-293
·
IF 1.366
Chang Jian,Zhang Shu-Zhen,Wu Ya,Zhang Hong-Jia,Sun Yin-Xia
Three Ni(II) complexes {[NiL(μ-OAc)(CH 3 CH 2 OH)] 2 Ni} ( 1 ), {[NiL(μ-OAc)(CH 3 OH)] 2 Ni]·2CH 2 Cl 2 ·2CH 3 OH ( 2 ) and {[NiL(μ-OAc)(CH 3 OH)] 2 Ni}·1.5CH 3 OH ( 3 ) based on a Salamo-type bis-oxime ligand (H 2 L = 2,2′-[ethylenedioxybis(nitrilo-methylidyne)]dinaphthol) have been synthesized and characterized by physicochemical and spectroscopic methods. The complexes 1 , 2 and 3 are all trinuclear structures, and the center Ni(II) ions are six-coordinated and show the slightly distorted octahedral coordination. They all consist of three Ni(II) ions, two deprotonated L 2- units, two μ-acetato ligands and two coordinated solvent molecules, as well as the crystallizing solvent molecules. Although the molecular structures of the Ni(II) complexes 1 , 2 and 3 are similar to each other, obtained in different solvents, the supramolecular structures are entirely different. The complexes 1 , 2 and 3 possess the self-assembled infinite 1D, 3D and 2D supramolecular structures via different intermolecular interactions (hydrogen bonds, C–H··· π and π ··· π stacking interaction), respectively. But complex 2 formed a 3D structures by intramolecular hydrogen bonds. It is significant that the solvent molecules have obvious effects on the optical properties and molecular configuration. The Hirshfeld surface analysis showed that the short-range forces of the hydrogen bonds in complexes 1 , 2 and 3 accounted for 67.8%, 44.6% and 52.7%, respectively. The molecular orbital energies for ligand H 2 L and complex 1 were obtained by DFT calculation, and the electron distribution, energy level and energy gap of HOMO and LUMO were given.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Tao Chen,Guangzhu Cao,Yi Qiang,Yanfeng Lu,Ronggao Qin,Wan Xu,Yiming Xie,Ruoyu Mao
The modified walnut shell biochar (WBC) was prepared through zinc-iron bimetallic oxide modification (ZF@WBC) at 600 °C under oxygen-limited conditions in this study. Through adsorption experiments, characterization analyses, and density functional theory (DFT) calculations, the adsorption properties of ZF@WBC to Pb (II) were investigated and the mechanism underlying such adsorption was elucidated. Characterization results showed that the surface area (375.9709 m 2 /g) and total pore volume (0.205319 cm 3 /g) of ZF@WBC were significantly greater than those of walnut shell biochar. The maximum adsorption capacity of ZF@WBC for Pb (II) was found to be 104.26 mg/g, which is 2.57 times higher than that of WBC according to the adsorption experiments conducted. The observed adsorption behavior followed both the pseudo-second-order (PSO) kinetic model and Langmuir isothermal adsorption model, suggesting that chemisorption plays a major role in the absorption process. Based on SEM, XRD, XPS, FTIR characterizations along with DFT calculations performed in this study, it can be concluded that surface complexation, ion exchange, electrostatic attraction, physical absorption are among the main mechanisms responsible for absorption of Pb (II) by ZF@WBC. Furthermore, even in the presence of interfering ions at different concentrations, ZF@WBC exhibited a removal rate above 70% for Pb (II). Therefore, ZF@WBC has great potential as an effective absorbent for removing Pb (II) from wastewater, while also offering opportunities for biomass waste resource utilization.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhengwen Wei,Liuqing Li,Wei Wang,Wankui Ni,Xiang-fei Lü,Giuseppe Mele,Zhen-Yi Jiang
The widespread presence of harmful and stubborn amine organic contaminants in aquatic environments motivated the exploration of efficient technologies for alleviating their serious environmental crisis. Herein, the recyclable magnetic Schiff base polymer (Fe 3 O 4 -TENE) with satisfactory and promising capacity in treating aniline and 3,4-diaminotoluene as representative amine organic contaminants was fabricated via a simple in-situ polymerization method, which combined the magnetic separability advantage of magnetic oxides with the abundant aromatic carbon content properties of Schiff base polymer. Multiple characterization methods verified the effectiveness of the in-situ polycondensation coating reaction and analyzed the physicochemical properties of Fe 3 O 4 -TENE. The Fe 3 O 4 -TENE possessed abundant homogeneous reaction sites and excellent regeneration performance, multiple diffusion driving forces and micro-mechanisms co-participated in the removal reaction. The adsorption pathway, underlying reaction mechanism and the most probable bonding system were identified based on the statistical modelling and DFT quantitative calculations. Especially, the visible electrostatic potential molecular and molecular orbitals verified the π-π interaction and electrostatic forces greatly contributed to the removal reaction. The Driving forces – Challenges – Breakthrough – Application framework was proposed for comprehensively assessing the possible environmental application of Fe 3 O 4 -TENE. Overall, this work not only provides important insights into the utilization of magnetic polymer composite to alleviate ecological and environmental risks caused by amine organic pollutants, but also contributes to an in-depth excavation of the bonding types and removal mechanisms from both micro and macro perspectives.
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