JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Jian Liu,Yingbi Chen,Yuting Hu,Yiting Zhang,Gengwei Zhang,Shixing Wang,Libo Zhang
A metal-organic framework (ZnO@ZIF-8) with great adsorption potential was developed using ZnO nanoparticles as a surface-active center and applied to lead removal from wastewater. The adsorption experiments were carried out and the related adsorption behaviors were investigated. The adsorbent shows excellent adsorption performance between pH 3–5. The maximum adsorption capacity of ZnO@ZIF-8 for Pb (II) was 689.36 mg/g at 303 K. The adsorptive process of Pb (II) onto ZnO@ZIF-8 conforms to the Langmuir isotherm and pseudo-second-order kinetic models. Thermodynamics illustrate that the adsorption process is chemical adsorption on a uniform surface. Selectivity experiments showed that ZnO@ZIF-8 had the strongest affinity with Pb (II). The adsorption-desorption cycle confirmed that ZnO@ZIF-8 was a reliable and recyclable adsorbent. XPS, Zeta potential and FT-IR analysis illustrate that the adsorption of Pb (II) by ZnO@ZIF-8 was concentrated in electrostatic adsorption and chelation. DFT calculation indicated that there are different types of Pb (II) combination mode (Pb-N and Pb-O) and the adsorption mainly depended on the chelation. This study presented herein played important roles in the governance of heavy metal waste-water pollution as a result of ZnO@ZIF-8 can effective selectivity cleanup of Pb (II).
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Hao Wang,Shuai Wang,Shixing Wang,Jiali Tang,Yingbi Chen,Libo Zhang
A new zirconium-based adsorption material (UiO-66-AMP) was prepared by modifying UiO-66-NH 2 with 5-adenosine to effectively remove Pb(II) and Cr(VI) from wastewater. The SEM, EDS, XRS and FT-IR characterization confirmed the successful synthesis of UiO-66-AMP. We conducted a sets of experiments to test the adsorption effectiveness of UiO-66-AMP for Pb(II) and Cr(VI). The maximum adsorption capacity of UiO-66-AMP for Cr(VI) (pH=2) and Pb(II) (pH=4) are 196.60 and 189.69 mg/g, respectively. The adsorption process conforms to the pseudo-second-order and Langmuir models, which indicates that the adsorption is a single-layer chemical process. Gibbs free energy ( ∆G) indicates that the adsorption of Pb(II) is an exothermic reaction , while the adsorption of Cr(VI) is an endothermic reaction . At the same time, the adsorbent maintains excellent adsorption capacity at least after 4 cycles. The good adsorption performance of UiO-66-AMP towards the metal ions was attributed to the surface complexation and electrostatic interactions. Therefore, the new adsorbent has obvious application prospect to remove Pb(II) and Cr(VI) from wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yaoyao Zhang,Shikui Jia,Xinqiang Yuan,Liu Ding,Taotao Ai,Kangze Yuan,Wei Wang,Luca Magagnin,Zhenyi Jiang
In this work, a novel adsorbent was evaluated for eliminating heavy metal ions from water. The cyano-functionalized silica aerogels (ANSA-X) were fabricated by functionalizing silica aerogel with 2-cyanoethyltriethoxysilane, and then further by the reaction with hydroxylamine hydrochloride to obtain amidoxime-functionalized silica aerogels (AOSA-X) with a large specific surface area. The FTIR and NMR analysis indicated that cyano was successfully transformed into amidoxime groups. Adsorption experiments showed the adsorption performed well with the Langmuir isotherm, and AOSA3 exhibited the optimum adsorption property with 598.05 mg/g for Pb (II) and 534.10 mg/g for Cu (II). The thermodynamic results indicated that spontaneous endothermic process was the nature of the adsorption. The adsorption rate of AOSA3 was above 86% after five successive adsorption–desorption cycles. XPS analysis and DFT calculations demonstrated that the N and O atoms participated in the chelating adsorption of Pb (II) and Cu (II), and the N atom on the amidoxime groups played a dominant role. Life Cycle Analysis (LCA) evaluated the environmental effect of the preparation of 1 kg AOSA3 adsorbent, identified the environmental factors with high environmental impact, proposed alternative solutions, proved the feasibility of preparing a novel high-efficiency amidoxime-based adsorbent, and provided a guideline for the sustainable mass production of AOSA3 adsorbent. In conclusion, AOSA3 demonstrated to have promising application perspectives in heavy metal effluent treatment.
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ACS Omega
·
2024
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IF 3.7
Xin Xu,Ze Zhang,Hongwei Yu,Tong Shen,Hongzhi Pan,Dong Chang
Nonsmall cell lung cancer (NSCLC), due to its lack of early symptoms, has become one of the leading causes of cancer-related deaths globally. Exosomes, small membrane vesicles secreted by cells, are widely present in human bodily fluids. In the bodily fluids of NSCLC patients, the quantity of extracellular vesicles is double that of healthy individuals, suggesting their potential as biomarkers for screening NSCLC. This study designed a dual-modal aptasensor that integrated excellent sensitivity in electrochemical detection and portability in fluorescence detection into one device. AuNPs were functionalized with exosome-capturing probes containing thiol-modified CD63 aptamers, which were immobilized on screen-printed gold electrodes. On the other hand, the carboxylated CD63 aptamer was immobilized on the surface of PB-modified g-C3N4 loaded with Co-SANs particles (Co@g-C3N4@PB). By combining these components, a sandwich structure (AuNPs/Apt1/Exo/Apt2- Co@g-C3N4@PB) was constructed, forming a probe for specific exosome recognition. First, the samples were preliminarily assessed for their positive or negative status under a fluorescence inverted microscope. Subsequently, a more in-depth quantitative analysis was conducted on suspected positive samples using electrochemical or fluorescence analysis methods. The detection limits for electrochemical analysis and fluorescence analysis were 66.68 and 33.5particles/mL, respectively. In the analysis of clinical serum exosome samples, the developed dual-modal aptasensor effectively distinguished serum specimens from those of NSCLC patients and healthy volunteers. This highlighted the inspection capability of the dual-modal adapter sensor, especially in point-of-care testing, making it a highly suitable tool for clinical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Xin Li,Tong Wu,Zhiqiang Jia,Tong Hao,Hong Zheng
A widely applicable Zn-DMTD-MOGs was prepared via direct construction strategy. • Zn-DMTD-MOGs shows great potential for trace heavy metals removal from real water. • DFT provides a local coordination cluster model for amorphous MOGs at atomic scale. • Synergistic chelating/monodentate coordination and LMCT enable efficient lead capture. Metal-organic gels (MOGs) have attracted extensive attention in the field of heavy metal removal, owing to their advantages including ease of surface modification, good stability, hierarchical pore structure, tunable functional groups, and mild and facile preparation conditions. However, the existing MOGs still leave considerable room for performance improvement. To produce MOGs with enhanced adsorption sites, high specific surface area, and greater pore volume, this study combined ultrasound-assisted nucleation with a high-concentration reaction strategy and triethylamine-mediated deprotonation, thereby enabling direct coordination between 2,5-Dimercapto-1,3,4-thiadiazole (DMTD) and Zn 2+ . Then, Zn-DMTD-MOGs material with higher-density N and S adsorption sites was successfully synthesized. The material exhibits a disordered particle-stacked amorphous structure with abundant mesopores (3–24 nm). Adsorption experiments demonstrate that the material achieves a trace Pb(II) removal efficiency of 96.98% within 10 s. The material achieves wide applicability over a low concentration range (≤ 42 mg/L) and a broad pH range (3.5–10.5), along with favorable stability, good reusability, and applicability to real water matrices. A local coordination cluster model was obtained through density functional theory (DFT) geometry optimization, and a synergistic chelating/monodentate coordination and ligand-to-metal charge transfer (LMCT) mechanism was established. The analysis reveals that the material adsorbs Pb(II) primarily through chelation at dual N/S sites and monodentate coordination at single S sites. This mechanism endows Zn-DMTD-MOGs with ultrafast adsorption kinetics and excellent cyclic stability, making them promising candidates for heavy metal remediation in drinking water sources. Download: Download high-res image (120KB) Download: Download full-size image
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Xiaocong Zhong,Yahui Ren,Kuifang Zhang,Huai Jiang,Ruixiang Wang,Zhifeng Xu
Incorporating oxygen evolution catalytic particles into the Pb matrix via a powder mixing-pressing-sintering process is an effective strategy to develop efficient lead-dispersed particle (Pb-DP) composite anodes for nonferrous metal electrowinning . Catalytic particles are demonstrated to significantly reduce the anodic potential of Pb-DP anodes. However, the intrinsic contribution of catalytic particles to the electrochemical performance of Pb-DP anodes remains obscure. Herein, Pb-DP anodes with different dispersed particles (chemically inert Si or C, catalytic Co 3 O 4 or MnCo 2 O 4 ) were prepared. The anodic potential, microstructure and phase composition of the oxide layer, and oxygen evolution behavior of these Pb-DP anodes were investigated and compared with those of the Pure-Pb anode (prepared without dispersed particles). The results showed that compared with the Pure-Pb anode, Pb-Si and Pb-C anodes present similar microstructures and phase compositions of the oxide layer. However, they exhibit a larger Tafel slope for the oxygen evolution reaction (OER). Although the incorporation of catalytic particles (Co 3 O 4 and MnCo 2 O 4 ) reduced the thickness and specific surface area of the oxide layer and inhibited PbO 2 growth, the presence of Co 3 O 4 and MnCo 2 O 4 significantly reduced the Tafel slope and charge transfer resistance ( R ct ) of the OER. Consequently, the anodic potentials of Pb-Co 3 O 4 and Pb-MnCo 2 O 4 are approximately 45 mV and 69 mV lower than that of Pure-Pb, respectively. It is demonstrated that the lower anodic potential of the Pb-Co 3 O 4 and Pb-MnCo 2 O 4 composite anodes originates from the catalytic activity of the dispersed particles rather than the physical effect of the dispersed particles.
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Wanlin Qin,Lufang He,Yuchi Zhang,Bohan Li,Le Han,Yan Xu
Construction of heterocompositional hybrid metal–organic frameworks (MOFs) by integration of more than two MOFs is a smart strategy for fine-tuning MOF properties. In this work, a novel yolk-shell MIL-88A@NiFe-PB heterostructure, in which MIL stands for Materials from Institute Lavoisier, and PB represents the coordination network of Prussian Blue, was fabricated through a fast wrapping and then inward-etching growth synthetic strategy under mild stirring condition. The thickness of the outmost layer of NiFe-PB and the internal core structure of MIL-88A can be controlled by tuning the concentration of K 4 [Fe(CN) 6 ]·3H 2 O in the assembly system. A rational growth mechanism for the yolk-shell MIL-88A@NiFe-PB heterostructure was proposed. The as-prepared yolk-shell MIL-88A@Ni 10 Fe PB-50 architectures were then explored for non-enzymatic glucose sensing. The results show that the designed glucose sensor exhibits a high sensitivity of 1963.2 μA mM −1 cm −2 over a wide linear range of 0.005–1.0 mM, a low detection limit (0.12 μM), as well as a fast reaction time (<2 s) and long-term stability for non-enzymatic glucose detection. Also, it shows good applicability in real serum samples. This work provides a “wrapping-inward-etching” synthetic strategy for construction of hybrid MOFs with exceptional outstanding non-enzymatic glucose sensing performance, providing a reasonable guide for construction of other MOF on MOF intriguing structures for electrochemical sensing applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·110417-110430
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IF 5.8
Du Xuan,Rashid Suraya Abdul,Abdullah Luqman Chuah,Rahman Norizah Abdul
Separation materials have received increasing attention given their broad applications in the management of environmental pollution. It is desired to balance the contradiction between high separation efficiency and selectivity of separation materials. The integration of ball-milled bone chars with electrospun membranes might achieve this balance. In this study, electrospun cellulose/chitosan/ball-milled bone char (CL/CS/MB) membranes were by well-dispersing ball-milled bone chars with nanoscale size (98.9–167.5 nm) and developed porosity (40.2–373.1 m 2 /g) in the electrospinning solvent. The synergistic integration of distributed MBs (5.4–31.5 wt.% of loading hydroxyapatite on the membrane matrix) allowed the efficient sorption of Pb(II) with fast kinetics (20.0 min), excellent capacity (219.9 mg/g at pH 5.0, T 298 K), and favorable selectivity coefficients (2.76–6.79). The formation of minerals was dominant for the selective sorption of Pb(II) by combining the spectral analysis and quantitative determination. The surface complexation with O-/reductive N-species, the cation exchange with inorganic Ca 2+ , the electrostatic attraction with deprotonated O − , and the cation-π coordination with the aromatic carbon via the π-electrons should be not ignored for the capture of Pb(II). This work demonstrated the feasibility of electrospun CL/CS/MB membranes as a promising candidate for the remediation of aquatic pollutants.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 28
·期 23
·30312-30322
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IF 4.223
Wang Yingya,Zhang Hanbing,Yaseen Muhammad,Tong Zhangfa,Chen Ninghua,Shi Huazhen
In order to endow alkaline Ca-bentonite (ACB) with magnetic separation ability, simultaneously obtain better magnetic stability and stronger removal capacity of heavy metal cations; magnetic alkaline Ca-bentonite/carboxymethylcellulose-chitosan film (MACB/C-C) was prepared by organic modification of magnetic alkaline Ca-bentonite (MACB) using non-toxic carboxymethylcellulose and chitosan. Textural characterization results revealed that magnetic Fe 3 O 4 nanoparticles were successfully immobilized on ACB and modified with C-C. The functionalized layer of C-C concurrently enhanced the stability of Fe 3 O 4 and removal performances of heavy metal cations. Adsorption results indicated that MACB/C-C exhibited thorough separation from aqueous solution and greater uptake ability for Pb(II) and Cd(II) (483 mg·g −1 and 123 mg·g −1 ) than the nascent MACB (335 mg·g −1 and 76 mg·g −1 ), respectively, at pH 5 and 25 °C temperature. The adsorption of Pb(II) and Cd(II) on MACB/C-C mainly occurred via surface precipitation and complexation when pH > 2. MACB/C-C could be efficiently recycled with marginal decrease in adsorption capacity. The current approach credited to the convenient operation, simplified synthesis, and high efficiency of MACB/C-C could be deemed as a promising alternative for the removal of heavy metal cations from wastewater.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
·
IF 6.789
Jing Nie,Qiming Wang,Shengya Gao,Chi Sun Poon,Yaoyu Zhou,Jiang-shan Li
With rapid economic growth and urbanisation, the reuse and recycling of solid wastes has become a high priority for the sustainable development of modern cities. In this study, two typical solid wastes, incinerated sewage sludge ash (ISSA) and waste bentonite , were co-valorised to produce granular adsorbents through a simple and energy-saving pelletisation/sintering process. A mixture of ISSA and bentonite at a weight ratio of 3:1 was pelletised and sintered at 700 °C. The resultant ceramsite, with good mechanical strength, could effectively remove Pb(Ⅱ) from aqueous solutions. The adsorption kinetics can be described by the pseudo-first-order (PFO) model. The results indicated that the Pb(Ⅱ) adsorption process was dominated by electrostatic attraction , precipitation, and complexation. The isothermal data exhibited a good correlation with the Freundlich model, indicating that the adsorption process was non-ideal and spontaneous. The maximum adsorption capacity was approximately 21.6 ± 0.35 mg/g at 318 K. After 5 cycles of regeneration, the adsorbent maintained good adsorption performance. Moreover, the removal rate was not greatly affected by ionic strength . These findings demonstrate that the granular adsorbent prepared with ISSA and waste bentonite can be recognised as a promising adsorbent for Pb-containing wastewater treatment .
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JOURNAL OF SOILS AND SEDIMENTS
·
2021
·Vol. 21
·期 7
·2540-2550
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IF 3.308
Yang Han,Ye Zhi,Feng Fang,Xu Nan,Yang Jing,Yao Zihan,Li Zuling,Chen Jianping
Purpose Lead (Pb(II)) can be accumulated in soil and transferred to humans via the food chain. Therefore, it is essential to improve Pb(II) immobilization during soil remediation. Materials and methods Nanosized zero-valent iron (nZVI) from green tea extract (tea polyphenols, TPs) was successfully synthesized as an additive reductant. Further, the nZVI was supported on montmorillonite (Mont), resulting in a GT-nZVI@Mont composite characterized by multiple techniques, including Zeta potential, SEM, TEM, XRD, and XPS. Moreover, the transport experiments and the toxicity characteristic leaching procedure (TCLP) were conducted to identify the optimum conditions (i.e., GT-nZVI@Mont dosage, Pb(II) concentration, and pH) for the remediation. Results and discussion The experimental results showed that the enhanced transportability of GT-nZVI@Mont was about 40% more than that of GT-nZVI. Meanwhile, Pb(II) immobilization was increased at various pH values (especially under anoxic conditions). The Pb(II) immobilization capacity of GT-nZVI@Mont was 900.8 mg∙g -1 (per unit of Fe content), which was significantly higher than 530.1 mg∙g -1 per unit of Fe content in GT-nZVI. Such enhancement could be ascribed to the synergistic effects of the wrapped TP around the Fe 0 core and the Mont interlayer support, capable of protecting the Fe 0 surface from further oxidation. When GT-nZVI@Mont reacted with the Pb(II) in soil, TPs’ unwrapped coverage increased the reaction sites of Fe 0 cores for Pb(II) reduction and adsorption. Conclusions GT-nZVI@Mont with sufficient transportability provided efficient in situ remediation of Pb(II) in contaminated soil at a wide pH range.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Xin Zhao,Meng Li,Fuqiang Zhai,Yanling Hou,Rui Hu
Phosphate species can complex with nuclides and heavy metals from aqueous solutions strongly. The introduction of phosphate groups onto the surface of biochar sorbents (mostly <1.0 at.% of P) is highly desired. In this study, phosphate modified hydrochars (HTBs) were prepared through the hydrothermal carbonization of bamboo sawdust with various duration (2, 12, 24 h) in the presence of phytic acid (0–70 wt%). The results showed that the addition of PA with a low concentration of 10 wt% carbonized at 2 h generated hydrogen protons to etch the pristine sawdust, inducing the granulation of surfaces and a 5.5-fold enhancement of surface area. While HTBs carbonized with increasing PA concentrations (30–70 wt%) and longer duration (12 and 24 h) presented more carbonaceous particles with rising sizes from <100 nm to 2.5 μm, which should be due to the cross-linkage of dehydrated phosphate-containing organic carbon components to the matrix, enabling the resultful surface modification (maximum of 2.1 wt% of P). The uptake of U(VI), Pb(II) and Cd(II) on HTBs was investigated given various geochemical conditions including contact time, pH, ionic strength , humic acid and temperature. HTBs could capture U(VI), Pb(II) and Cd(II) efficiently from the ideal and simulated wastewaters, and be reused well after six recycles. This work opened a new strategy for the potential of phosphate-hydrochars in the aqueous remediation.
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