CHEMOSPHERE
·
2024
·
IF 8.1
Chengqiang He,Yue Sun,Yingpeng Gu,Hongyu Ji
Generally, the pH of fluorinated groundwater or many industrial wastewater is neutral, while the majority of metal-modified adsorbents can work efficiently only under acidic conditions. In this study, we synthesized a novel hybrid adsorbent, Mg–Zr-D213, by loading nano-Mg/Zr binary metal (hydrogen) oxides in a strong-base anion exchanger, D213, to enhance the adsorption of fluoride from neutral water. Mg–Zr-D213 exhibited a better fluoride-removal capacity in neutral water than monometallic modified resins. Under the interference of competing anions and coexisting organic acids, Mg–Zr-D213 exhibited superior selectivity. The Langmuir model indicated that the fitted maximum sorption capacity of Mg–Zr-D213 was 41.38 mg/g. The results of column experiments showed that the effective treatment volume of Mg–Zr-D213 was 8–16-times higher than that of D213 for both synthetic groundwater and actual industrial wastewater, and that NaOH–NaCl eluent could effectively recover more than 95% of fluoride. Adsorption experiments with Mg/Zr metal (hydrogen) oxide particles and D213 separately demonstrated a synergistic effect between –N + (CH 3 ) 3 and Mg/Zr metal (hydrogen) oxide particles. The ligand exchange or metal-ligand interaction of Mg/Zr metal (hydrogen) oxide particles on fluoride was further demonstrated via X-ray photoelectron spectroscopy. Overall, Mg–Zr-D213 has great potential for enhanced fluoride removal in neutral water.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Fangfang Liu,Mengnan Lu,Xiao Yang,Yuedi Wang,Chunmei Wang,Xiaomin Dou
This work proposed introducing nanoscale Fe-Zr oxides onto the layered-surfaces of MXene carriers to maintain well dispersion and anchoring stabilization. The results indicated that Fe-Zr oxide/MXene has a superior adsorption capacity of 209.1 mg/g at pH 7.0. The mass transfer of antimonite onto Fe-Zr oxide/MXene was investigated by numerical solving the homogeneous surface diffusion model. The external mass transfer coefficient ( k f ) and surface diffusion coefficient ( D S ) were determined to be 6.48 × 10 −4 and 1.86 × 10 −8 cm/min, respectively, and the latter was rate-limited. The 2-D profiles of Sb(III) diffusion within the adsorbents were visualized. Data mining and knowledge discovery using machine learning models indicated that the gradient boosting regression (GBR) model successfully predicted the test datasets. The operational conditions outweigh adsorbent properties in capacity prediction, and equilibrium concentration and adsorbent dose, are the most two important features. Using the trained GBR model, the Sb(III) adsorption capacities of MXene (Ti 3 C 2 ) and Fe-Zr/MXene were well predicted. This work provides insights on understanding the mass transfer mechanisms of Sb(III) in functionalized-MXene adsorbents and employing machine learning models for tuning the treatments for better achievements.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Yijun Chen,Meina Cheng,Long Jin,Hailiang Yang,Sanjian Ma,Zixia Lin,Guoliang Dai,Xin Liu
The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants , such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd–H 2 has been preferred for Fenton-like reactions and the specific H 2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H 2 O 2 . The systematic characterization demonstrated that the nano Pd 0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L −1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min −1 H 2 , 2 g L −1 Pd@UiO-66(Zr) and 25 μM Fe 2+ . The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance . In addition, both reducing Fe(III) and self-generating H 2 O 2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd 0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 42
·18166-18176
·
IF 2.7
Jing Xiao,Linshan Peng,Ailan Ouyang,Xin Mo,Yiping Yao,Chunyan Wang,Chunpei Yan
A phosphonate-functionalized Zr@FMA material was prepared in this work as an adsorbent for the efficient recovery and enrichment of Th(IV) from aqueous solutions. The adsorbent, prepared by functionalizing Zr@FMA with alendronate sodium (ALS), a well-known active bisphosphonate, demonstrates good water stability and a large surface area, making it suitable for the separation and enrichment of Th(IV) in aqueous solutions. A comparison of the adsorption behavior of Th(IV) on Zr@FMA-ALS with the unfunctionalized Zr@FMA reveals that the introduction of phosphonate groups significantly enhances the maximum adsorption capacity and rate of Zr@FMA-ALS. The adsorption data aligns well with the Langmuir isotherm model, suggesting a uniform distribution of Th(IV) on the adsorbent surface in a monolayer coverage. Thermodynamic analysis indicates an endothermic and spontaneous adsorption process. Zr@FMA-ALS also shows excellent selectivity for Th(IV) over other metal ions in mixed solutions. Insights into the adsorption mechanism are provided through SEM, XPS, and FT-IR analyses, indicating that ALS molecules play a crucial role in capturing Th(IV) on the surface of Zr@FMA-ALS.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Yijun Chen,Hailiang Yang,Sanjian Ma,Meina Cheng,Zixia Lin,Long Jin,Xin Liu
As a representative antibiotic, trimethoprim (TMP), the emerging pollutant has been frequently detected in water bodies, and its potential harm has aroused the attention of society. Although the emerging pollutant could be efficiently degraded by the advanced oxidation process (AOP) represented by the Fenton reaction , both the problem of iron sludge disposal and the safe use of H 2 O 2 have plagued the further promotion of this technology. The H 2 (precursor of the active hydrogen [H]) and catalyst Pd/UiO-66(Zr) were introduced into the Fenton reaction in this paper. It was found that the process of reducing Fe(III) and self-generating H 2 O 2 could be facilitated due to the reduction of [H]. Under certain reaction conditions (initial pH 3, trace total iron 25 μM, H 2 30 mL·min −1 , catalyst 2 g·L −1 ) and without H 2 O 2 , a Fenton-like system was constructed, named MHORF-UiO-66(Zr). While achieving zero iron sludge discharge, 100 % of 20 mg·L −1 TMP was rapidly degraded within 1 h. It was found that the degradation of TMP could be attributed to the attack of singlet oxygen and hydroxyl radical . Furthermore, the performance changes of catalyst before and after six rounds of reactions were studied and it was found that Pd/UiO-66(Zr) had excellent and stable catalytic performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qin Wang,Xue Bai,Shiyu Sun,Yan Li,Mingzhe Tan,Yanfeng Wang,Na Wang,Ting Wang,Lina Zhou,Zijian Zhou,Xin Huang,Hongxun Hao
The fluorine chemical industry's rapid growth demands efficient strategies for treating and utilizing the costly and inefficient byproduct, fluoride-containing hydrochloric acid, posing a significant challenge. In this study, a cost-effective method was developed for preparing an acid-resistant and efficient defluorination material. Carbon nitride (C 3 N 4 ) was chosen for its exceptional acid resistance and was modified via template-free doping with different zirconium source. Characterization results through XRD, FTIR, BET, XPS, SEM, and TEM confirm the successful synthesis of CN-Zr using zirconium chloride (ZrCl 4 ) with a specific surface area of 87.77 m 2 /g. Furthermore, the adsorption results indicate outstanding fluoride adsorption performance of CN-Zr in hydrochloric acid, with a maximum adsorption capacity of 145.34 mg/g and minimal zirconium leaching. Moreover, the adsorption mechanism was systematically studied using Zeta potential, FTIR and XPS characterization. The findings indicate that Zr was integrated with C 3 N 4 uniformly by forming a deep eutectic system (DES), utilizing exposed terminal amino groups for effective hydrogen bonding with HF which predominates as the primary fluorine existence in hydrochloric acid. Meanwhile, the enhanced ion exchange, complexation of Zr-F and strong electrostatic attraction all contribute to improving adsorption. Finally, the assessment of recyclability performance and operation cost demonstrate that the material can maintain 80% of its initial adsorption capacity after five cycles. The cost analysis results indicate that the adsorption cost is only 0.3157 CNY/g, making it considerable competitive in the industry.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xiaoxiao Zheng,Xiaoping Chen,Xiaoqing Li,Jide Zhu,Jipeng Chen,Fengcai Lin,Lijuan Shen,Yanlian Xu,Lilong Jiang
The development of stable and effective catalysts to convert toxic H2S into high value-added sulfur is essential for production safety and environmental protection. However, the inherent defects of traditional iron- and zirconium-based catalysts, such as poor activity, high oxygen consumption, and low sulfur selectivity, limit their further developments and applications. Herein, the Fe–Zr bimetallic organic framework FeUIO-66(x) with different cubic morphologies was synthesized via a facile solvothermal method. The results indicate that the introduction of Fe not only increases the specific surface area and weak L-sites of the catalyst without changing its crystal structure, which provides enough reaction space and more active sites for the adsorption and activation of H2S, but also reduces the activation energy of the reaction, significantly promoting the selective oxidation of H2S. As a result, the as-obtained FeUIO-66(1) catalyst exhibits the highest desulfurization activity and superior durability and water resistance stability, and its H2S conversion and sulfur selectivity within 50 h are 100 and 88%, respectively. More importantly, the structure of the catalyst after the desulfurization reaction is consistent with that of the fresh counterpart. The study offers new insights into the development of effective and stable bimetallic catalysts to eliminate H2S and recycle sulfur.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Hua Yan,Yu-hong Luo,Ying Lei,Qing-lin Pan,Jun-chao Zheng
N ickle (Ni)-rich layered oxides as promising candidate of high-capacity cathode materials have aroused extensive concern primarily regarding their higher specific capacity. However, the major hurdle of Ni-rich cathodes (Ni content ≥0.7) is their poor cycling stability, which often suffers from the release of oxygen, structural degradation and increased impedance during cycling, especially at high voltage or high temperature. Herein, we demonstrated a feasible solid phase method for easy industrialization based on the Al 3+ /Zr 4+ co-doping in LiNi 0.72 Co 0.05 Mn 0.23 O 2 (A X Z Y -NCM) single-crystal cathode. The optimized A 0.5 Z 0.5 -NCM single-crystal material exhibited greatly enhanced structural and thermal stability. XRD refinement results indicated that both Al 3+ and Zr 4+ were mainly located in transition metal (TM) sites, strengthening the layered structure through strong M-O bonds and inhibiting cation mixing. In-situ XRD revealed that the synergistic rivet effect of Al/Zr co-doping alleviates anisotropic lattice stress-strain during charge/discharge process. Accordingly, the A 0.5 Z 0.5 -NCM cathode can output a high initial capacity of 177.3 mAh g −1 at 1 C, and captured a more desirable capacity retention of 85.10 % than that of U-NCM (74.33 %) at 1 C over 200 cycles. Even at a high voltage of 4.5 V, its capacity retention can still reach 82.37 %, significantly surpassing the unmodified U-NCM (31.0 %). The above results demonstrated that well-designed dual doping is highly effective for strengthen structure stability and cycling performance of Ni-rich cathodes.
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Journal of the Australian Ceramic Society
·
2024
·
IF 1.8
Lin Jia,Wang Shuai,Yang Yihang,Huang Guimei,Wang Jinhuo
In this study, Zr-modified Si-O-C precursor ceramics were prepared using three-dimensional (3D) printing. Ceramic sintering was completed by printing four precursors containing different zirconium acetylacetone contents. Comparative analysis was conducted on the ceramic yield, size shrinkage, mechanical properties, and microstructure. The results showed that the ceramic yield and size shrinkage of the four samples were increased with the increasing zirconium acetylacetone contents. The sample containing 30 wt% zirconium acetylacetone exhibited good compressive performance, with a compressive strength of 50.2 ± 0.6 MPa. Cracks were observed on the surface of samples containing 40 wt% zirconium acetylacetone, while those containing 10, 20, and 30 wt% zirconium acetylacetone were relatively intact. Therefore, a stable Si-Zr-O-C precursor ceramic with good mechanical properties, which can be used for 3D printing, was obtained.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Yu-Xuan Zheng,Xuwen Wu,Wei-Guang Yang,Bai-Xue Li,Kejing Gao,Jingsheng Zhou,Yunfang Liu,Dongzhi Yang
Radioactive nuclides and highly toxic organophosphates are typical deadly threats. Materials with the function of radioactive substances adsorption and organophosphates degradation provide double protection. Herein, dual-functional polyamide (PA)/polyethyleneimine (PEI)@Zr-MOF fiber composite membranes, fabricated by in-situ solvothermal growth of Zr-MOF on PA/PEI electrospun fiber membranes, are designed for protection against two typical model compounds of iodine and dimethyl 4-nitrophenyl phosphate (DMNP). Benefiting from the unique core-sheath structure composed of inner nitrogen-rich fibers and outer porous Zr-MOF, the composite membranes rapidly enrich iodine through abundant active sites of the outer sheath and form complexes with the amine of inner PEI, exhibiting a highly competitive adsorption capacity of 609 mg g −1 . Moreover, it can adsorb and degrade DMNP with the synergy of PEI component and Zr-MOF, achieving an 80 % removal of DMNP within 7 min without any additional co-catalyst. This work provides a feasible strategy to fabricate dual-functional materials that protect against radioactive and organophosphorus contaminants.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Kai Han,Chen Zhou,Jianlong Wang,Nana Zhao,Jinfeng Yuan,Zhicheng Pan,Mingwang Pan
Robust, self-healing waterborne coatings have become the preferred choice in the field of flexible electronic devices owing to their outstanding compliance, restorability, and environmental friendliness. Nevertheless, most of the existing self-healing waterborne polymers exhibit viscoelasticity, irreversible fatigue damage, and the challenge of reconciling self-healing functions with mechanical properties, all stemming from inherent molecular structure contradictions between flexibility and rigidity. Here, we propose a novel strategy that utilizes a nanofiller with dynamic reversible bonds to overcome the self-healing limitations that theoretically demand flexible chain, for achieving both mechanical robustness and self-healing ability in the waterborne polyurethane (WPU) hybrid coating system. We modified tetrapropyl zirconate (TPOZ) with 3-aminopropyltriethoxysilane (APTES) to enhance compatibility between the matrix and inorganic particles, while the formation of dynamic reversible bonds through both condensation hydrolysis endows the self-healing abilities. The WPU hybrid coating was designed by covalently incorporating amino-modified TPOZ (A-ZrO 2 ) into a glycinamide-functionalized WPU network, conferring excellent fracture energy (50.3 kJ/m 2 ), elastic recovery, along with antistatic capability to the coating. Furthermore, the hybrid coating maintains a robust mechanical performance alongside 92.58 % of healing efficiency, exhibiting a potential for flexible electronics application. The hybridization strategy via incorporation of the nanofillers with hard but reversible covalent bond resolves the inherent robustness-healing trade-off, providing exciting thoughts to expand WPU applications.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
WooYeon Moon,Dong Gyu Park,Younghu Son,Minyoung Yoon,Kyung Min Choi
The removal of bromide ions (Br − ) from water is critical, as these ions can generate bromate and brominated disinfection by-products that are toxic, carcinogenic, and corrosive. Previous research has not focused on the removal of Br − from water with a heavy presence of chloride ions (Cl − ). To address this research gap, we proposed a defective Zr-based metal–organic framework (MOF) to selectively remove trace Br − in environments with high concentrations of Cl − . We demonstrated that the open acidic sites on the secondary building units in a defective Zr-based MOF-808 (MOF-808-Cl) selectively removed the trace Br − in the presence of high concentration of Cl − using varying degrees of electrostatic interactions induced by their own polarizability. The Br − removal was performed with the mixed mechanism of ion-exchange and −adsorption, with contributions of approximately 70% and 30%, respectively. The Br − was successfully removed when the concentration of Cl − was 100 times higher than that of Br − . Our findings demonstrate the potential of MOF-808-Cl for industrial applications requiring trace ion removal and can provide insights for future research on selective ion removal in a competitive environment.
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