Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Guihong Han,Lulu Kou,Zhan Chu,Wenjuan Wang,Hongfei Ma,Bingbing Liu,Hu Sun,Shuzhen Yang,Yanfang Huang
Treatment of molybdenum-containing wastewater is crucial for mitigating the environmental threat of Mo(VI) ions and recovering valuable metals. Compared to conventional separation methods, adsorbing colloid flotation emerges as a viable way to efficiently remove Mo(VI) ions. However, the current colloidal adsorption reagents have constrained the development of adsorbing colloid flotation due to their poor removal efficiency and narrow solution pH range. To overcome these challenges, Zr(IV) salts and La(III) salts were employed as colloidal adsorption reagents for the first time to remove Mo(VI) ions from wastewater in this work. In particular, the differences in removal efficiency of Mo(VI) ions between Zr(IV) salts, La(III) salts and traditional Fe(III) salts were systematically evaluated over a wide solution pH range. Zr(IV) salts demonstrated robust pH stability, displaying a significant removal efficiency of over 70.00% for Mo(VI) ions during the colloidal adsorption stage across a broad solution pH range from 3 to 11. Even more astonishingly, the removal efficiency of Mo(VI) ions was further enhanced through the synergistic effect of cetyltrimethylammonium bromide (CTAB) during the flotation separation stage. Under the optimal conditions of bubble flotation, the solution turbidity decreased rapidly from 164.50 NTU to 3.33 NTU, and the removal efficiency of Mo(VI) ions reached an impressive 99.10% which was enhanced by 23.73% compared to the colloidal adsorption stage. In conclusion, Zr(IV) salts, serving as colloidal adsorption reagents, have overcome the limitations of traditional colloidal adsorption reagents and exhibit significant potential for the removal of Mo(VI) ions from wastewater.
研究领域:
环境科学
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化学工程
·
废水处理
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DOI
高影响因子
Molecular Catalysis
·
2017
·
IF 0
Ruiying Wang,Jianjia Wang,Huimin Zi,Yongmei Xia,Haijun Wang,Xiang Liu
Zr(IV)-salphen-MCM-41 was prepared by immobilizing a zirconium(IV) Schiff base complex onto the surface of MCM-41. The structural properties of the heterogeneous catalysts were characterized by FT-IR, UV, TG, XRD, SEM, TEM, BET, EDX, CO 2 -TPD, NH 3 -TPD and ICP-OES. Studies on the catalytic properties of the immobilized Zr(IV)-Schiff base complexes were performed using the reduction and cyclization of ethyl levulinate (EL) to γ-valerolactone (GVL) with isopropanol as the hydrogen source. Various reaction parameters, such as temperature, reaction time, solvent and catalyst loading were carefully investigated. The optimal conditions (GVL yield up to 90%) involved the utilization of Zr(Salphen)-MCM-41 as the catalyst in isopropanol. The key to heightened reaction performance was the incorporation of the phenolate and aniline groups in the ligands of bound to Zr. This increased the basicity of the catalyst, which subsequently enhances the efficiency of the transfer hydrogenation reported herein. Meanwhile, the immobilized catalyst can be easily separated and efficiently recycled at least five times without significant loss of activity. Finally, we proposed a plausible reaction mechanism based on experimental and characterization data.
研究领域:
化学工程
·
催化材料科学
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DOI
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shi-Qing Wang,Xu Gu,Xinzhu Wang,Xiao-Yu Zhang,Xiao-Yao Dao,Xiao-Mei Cheng,Jing Ma,Wei-Yin Sun
Defects in MOFs can benefit light absorption and charge transfer for photocatalytic application, nevertheless, studies on interplay between structural defects and photocatalytic properties of MOFs are in infancy. Herein, a series of UiO-66-NH 2 with different kinds of defects were created for regulating CO 2 photocatalytic reduction. Theoretical calculations in combination with experimental data verified that the sample with ligand-vacant (UiO-66-NH 2 -LV) defect performed better than non-defect, missing-cluster and monocarboxylate compensated ones in the photocatalytic CO 2 reduction reactions. UiO-66-NH 2 -LV shows superior photocatalytic activity with the highest CO yield of 30.5 μmol g −1 h −1 , which is 9.2 times higher than that of the sample with missing-cluster (UiO-66-NH 2 -MC), as well as the highest quantum yield (QY) of 0.90%. DFT calculations further demonstrate the correlation between discriminative photocatalytic activities in defect structures and tunable electronic properties characterized by absorption energy, E abs , and charge transfer energy, E LMCT , in the photocatalytic process. The ligand-vacant defect with the lowest sum of E abs and E LMCT will lower photocatalytic reaction energy barrier in the rate-limiting step among the elementary reaction step during CO 2 photoreduction. The insights gained from this study will guide the MOFs defect-engineering for enhancing CO 2 photocatalytic capacity.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Leyi He,Xiuli Wang,Yaoxia Li,Lulu Chen,Jia Guo,Changchun Wang
The efficient separation of adenosine analogues (e.g., Ado, AMP and dA) is crucial for clinical diagnosis, drug discovery and basic research. However, their structural similarities pose significant challenges to the separation and purification. PS@PGMA-IDA-Zr 4+ (PPIZ) microspheres were synthesized as IMAC stationary phases in this study. Efficient separation of Ado, AMP and dA was achieved by leveraging differential interactions including Zr 4+ -phosphate coordination, Zr 4+ -diol coordination and hydrogen bonding. Static adsorption experiments identified the PPIZ40–0.7 microspheres at pH 6 with optimal selectivity for the adenosine analogues (α (Ado/dA) = 4.46, α (AMP/Ado) = 41.40), while material characterization and adsorption kinetics elucidated the separation mechanism. Elution experiments demonstrated that Ado and AMP could be eluted utilizing PBS solutions with phosphate concentrations of 0.1 mM and 10 mM, respectively. Moreover, in chromatographic separation tests, PPIZ40–0.7 microspheres as packing material achieved excellent resolution for the adenosine analogues (Rs (Ado/dA) = 5.39, Rs (AMP/Ado) = 3.91), along with robust mechanical stability and reusability. Therefore, the PS@PGMA-IDA-Zr 4+ microspheres demonstrate significant promise for high-efficiency chromatographic separation of adenosine analogues.
研究领域:
分析化学
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分离科学
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生物无机化学
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药物分析
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DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 55
·34754-34765
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IF 3.361
Wei Qin,Kaixuan Xu,Junwei Wang,Xiaofeng Cui,Jianli Zhang,Yaqing Weng
To overcome the urgency of zirconium and hafnium separation, a novel mesoporous silica sorbent (PS-G1.0-MSNs) modified with phosphorous-functionalized G1.0 PAMAM dendrimers was prepared. The adsorption and separation behaviors of PS-G1.0-MSNs adsorbent on Zr(IV) and Hf(IV) were perfromed as a function of acidity, contact time, temperature, and ion concentrations by batch sorption methods. The maximum adsorption capacities for Zr(IV) and Hf(IV) were 25.7 mg g−1 and 5.36 mg g−1 under optimal experimental conditions, respectively, and the separation factor βHf/Zr = 2.0 > 1 demonstrated that the prepared sorbent had preferential selectivity for Hf(IV) in rich Zr(IV) solution. Moreover, kinetic data indicated that the sorption process on Zr(IV) and Hf(IV) achieved equilibrium within 120 min, and followed the pseudo-first-order model with a rate-determining step. The adsorption amount increased as temperature raised from 283 K to 303 K and the isothermal data plotted with the Langmuir model was better than the Freundlich model with monolayer behavior. Thermodynamic data analysis indicated that the sorption process was spontaneous and endothermic. Furthermore, XPS analysis revealed that the metal ion adsorption was mainly induced by the chemical coordination of Zr(IV) and Hf(IV) ions with N, O, P atoms of amide and phosphate groups. The present work provides good guidelines on the design of high efficient sorbent for the separation of Hf(IV) from Zr(IV) solutions.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
AICHE JOURNAL
·
2019
·Vol. 65
·期 8
·e16616
·
IF 3.463
Daofei Lv,Jiayu Chen,Yongwei Chen,Zewei Liu,Yuzhi Xu,Chongxiong Duan,Houxiao Wu,Ying Wu,Jing Xiao,Hongxia Xi,Zhong Li,Qibin Xia
Metal–organic frameworks (MOFs) combined with selective adsorption capacity of ethane over ethylene and good moisture stability are highly urged by adsorption industrial community. Here, the moisture stability mechanism of Zr-bptc, UiO-66, PCN-245, and Ni(bdc)(ted) 0.5 were investigated by moisture stability experiments, and computational simulation of metal node-linker breaking energy caused by water. Results show that the moisture stability follows the order of Zr-bptc > UiO-66 > PCN-245 > Ni(bdc)(ted) 0.5 . The different moisture stability for these MOFs is likely attributed to the bond strength between metal center and ligands, the coordination number of metal center, the hydrophobicity of framework, as well as the degree of interpenetrated framework. Additionally, comparing with ethylene-selective MOFs, ethane-selective MOFs have fewer coordinatively unsaturated metal sites. Breakthrough experiments indicated that Zr-bptc is the promising material for ethane/ethylene separation.
研究领域:
材料化学
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配位化学
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气体分离
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多孔材料
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工业吸附
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Siqi Liu,Jiawei Wang,Jiangwei Ren,Meng Zhang,Hui Mao
The contamination of fluoride is a concerned issue from the perspective of drinking water safety. Herein, we reported the controlled synthesis of novel chitosan aerogel functionalized by tannin-chelated Zr(IV), which was capable of accomplishing the high-performance adsorption of fluoride from water. The as-prepared functional chitosan aerogel (BTCA-Zr) featured fast adsorption kinetics and exceptional adsorption capability to fluoride. In static adsorption experiments, the superiority of the functional chitosan aerogels was demonstrated with the removal efficiency higher than 95% in the wide pH range of 3–10. The high porosity (79.08%) combined with surface decoration of amphiphilic tannin provided the functional aerogel with fast adsorption equilibrium in 40 min. Adsorption capacity of 86.0 mg g −1 for fluoride was achieved by the functional aerogel with the low fluoride concentration of 2.0 mg L −1 . The fluoride adsorption on BTCA-Zr exhibits pseudo-second-order (PSO) kinetics and fits the Langmuir isotherm, and the adsorption process is exothermic and spontaneous. The adsorption mechanism was revealed by adsorption experiments combined with the density functional theory (DFT) calculations, which confirmed the critical role to form the species of Zr-oxyfluoride with low binding energy for accomplishing the high-performance adsorption of fluoride. Notably, the functional aerogel achieved 85.59% of fluoride removal by column adsorption of the simulated underground water. The functional aerogel was recycled 5 times in column adsorption of the simulated underground water by retaining 78.38% of its initial adsorption capacity.
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 45
·68320-68331
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IF 5.19
Luo Qie,Cui Wenzheng,Wang Huan,Xiao Bo,Chen Lei,Wang Youqun,Zhang Zhibin,Liu Yunhai,Cao Xiaohong
The separation of magnetic adsorbents from aqueous solutions is made simple by using an external magnetic field. Herein, magnetic Zr(IV)-ethylenediamine tetramethylene phosphonic acid (EDTMPA) hybrids (MZrOP- x -T, x , and T were the different quality of Fe 3 O 4 @C and temperature in the synthesis process, respectively). A study was conducted on the uses of MZrOP- x -T in the capture of U(VI). The influences of pH, adsorption period, initial concentration, and temperature were all investigated. Furthermore, the desorption and reusability of the materials were explored. The optimal values of x and T were 0.2 g and 100 °C, respectively. At 298.15 K, the maximum adsorption capacity of MZrOP-0.2-100 was 330.30 mg·g −1 . The current research demonstrates that MZrOP-0.2-100 is a potentially effective material in removing U(VI) from radioactive solution.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2026
·
IF 1.7
Liu Xiaotong,Li Hui,Xu Chengjin,Peng Xiujing,Sun Guoxin,Cui Yu,Lu Ping
Efficient separation of nuclear-grade zirconium (Zr) and hafnium (Hf) remains a significant challenge in the nuclear industry. In this study, a novel extractant, di(p-tert-octylphenyl) phosphate (DTOPPA), was designed and synthesized. DTOPPA demonstrated preferential extraction of Hf over Zr in sulfuric acid media, surpassing the performance of conventional extractants such as D2EHPA and PC88A. Under optimized conditions, Hf(IV) extraction achieved 90.7% with a separation factor SF (Hf/Zr) of 13.4. Density functional theory (DFT) calculations and acid–base titration indicated enhanced dissociation of DTOPPA, attributed to the electron-withdrawing phenoxy group, which facilitates cation exchange. Slope analysis, saturation capacity measurements, and Fourier-transform infrared spectroscopy (FTIR) identified the extracted species as Zr(Hf)OA 2 ·2DTOPPA, involving cation exchange and P=O coordination. Selective stripping of Zr was accomplished using dilute sulfuric acid, while oxalic acid efficiently stripped Hf. A two-stage countercurrent extraction process yielded nuclear-grade Zr with stable organic phase recycling. This novel extractant provides an environmentally friendly and efficient method for Zr/Hf separation with significant potential for industrial application.
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 4
·B193
·
IF 3.12
Sheying Dong,Hao Cui,Dandan Zhang,Mengmeng Tong
Several reports reveal that high level of C-reactive protein (CRP) in serum enhances venture of diabetes. In this article, we presented a platform which blended Zr(IV)-organic framework with 2,5-thiophenedicarboxylate ligand (Zr-tdc) and ionic liquid (IL) to form a steady composite membrane on the carbon paste electrode (CPE). The platform was applied to CRP and glucose biosensors which were connected with diabetes and displayed well performances. Firstly, a sensitive immunosensor for label-free and direct detection of CRP was developed at Zr-tdc/IL modified electrode. Under optimal conditions, differential pulse voltammetry (DPV) response showed the low detection limit of CRP was 0.2 ng/mL. Secondly, the glucose biosensor immobilized glucose oxidase (GOX) was constructed and studied by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and amperometric response. The Michaelis–Menten constant (KM) of immobilized GOX was 0.16 mM, and the detection limit was 2.7 μM for glucose. Two novel biosensors displayed well selectivity, stability and lower detection limit. This work improved the performance of electrochemical sensing and expand the utilization of the material by carrying on the effective immobilization of enzyme and antibody.
研究领域:
生物医学工程
·
分析化学
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
He Huang,Zhao-Yang Liu,Shuang-Bao Li,Juan Zhu,Bao-Xu Jiang,Yu-Teng Zhang
In this work, an amino-functionalized Zr-based metal-organic polyhedron (denoted ZrT-1-NH 2 ), synthesised under the solvothermal method , has been selected as the photocatalyst for the removal of tetracycline (TC). The effects of adding dosages, pH values of TC degradation efficiency were investigated, and the results showed that this material was better effective in photocatalysis degradation of tetracycline antibiotic. In addition, the trapping experiments reveal that hydroxyl radical (•OH) and superoxide radical (•O 2 − ), serving as active species, play major roles in the photocatalytic process. Furthermore, a possible mechanism for the photocatalytic process is proposed. This work presents that zirconium-based metal-organic polyhedra (Zr-MOPs) may be promising photocatalysts for the removal of antibiotics in wastewater.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Rui Ma,Xinjie Cui,Youyi Liu,Qianhui Xu,Weiwei Wang,Guangze Nie
Nanocomposites fabricated through the encapsulation of hydrated Zr(IV) oxide (HZO) nanoparticles within millimeter-scale hosts have emerged as promising candidates for phosphate sequestration from water. However, achieving ultrasmall nanoparticles within these hosts that maintain high decontamination reactivity is still a significant challenge. Herein, a novel nanocomposite (denoted HZO@CS-PEI) was obtained by confining the growth of HZO in dual crosslinked network hydrogels composed of interpenetrating chitosan (CS) and polyethyleneimine (PEI). Benefiting from the confinement effect of the dual cross-linked structure, the HZO within HZO@CS-PEI exhibited an ultrasmall size of approximately 2.16 nm. The incorporation of PEI enhanced both phosphate sequestration efficiency and mechanical stability of the nanocomposite, improving its practical applicability. Ultrafine dispersion of HZO nanoparticles within the composite matrix achieved a saturable phosphate adsorption capacity exceeding 64.41 mg/g at 298 K. Crucially, selective phosphate adsorption by HZO@CS-PEI remained effective in water containing high concentrations of coexisting anions and organic matter. The synergistic application of spectroscopic analyses and density functional theory (DFT) calculations revealed three distinct interaction mechanisms between HZO@CS-PEI and phosphate: inner-sphere complexation, hydrogen bonding, and electrostatic interactions. Furthermore, the used HZO@CS-PEI could be effectively regenerated with 0.1 mol/L NaOH for repeat use. In the column adsorption tests, phosphate-contaminated water was successfully treated by HZO@CS-PEI columns over 2750 bed volumes (BV), confirming operational stability under dynamic flow conditions.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）