SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Xiaoxue Pan,Junyan Wei,Min Wang,Jie Zhang,Zhiming Xu,Haojie Wei,Nami Lai,Kainan Nian,Rui Zhang,Xuesheng Zhang
Due to wide applications, halophenols (HPs), especially bromophenols, chlorophenols, and fluorophenols, are commonly detected but resistant to biological removal in wastewater treatment plants (WWTPs). This study investigated the overall transformation behaviors of three representative HPs (2,4-dichlorophenol: 24-DCP, 2,4-dibromophenol: 24-DBP, 2,4-difluorophenol: 24-DFP) in six chemical oxidative systems (KMnO 4 , K 2 FeO 4 , NaClO, O 3 , UV, and persulfate (PS)). The results revealed fast removal of selected HPs by O 3 , PS and K 2 FeO 4 , while a large discrepancy in their removal efficiencies occurred under UV irradiation, KMnO 4 oxidation and particularly chlorination. Based on the analysis of the identified intermediates and products, coupling among the five routes was the general route, and dimers were the main intermediates for HP oxidation. The effect of the halogen atom on the transformation pathways of HPs was highly reaction type dependent. Among the six chemical treatments, PS could induce HPs to yield relatively low-molecular-weight polymers and obtain the highest coupling degree. Transition state (TS) calculations showed that the H atom linked to the phenoxy group of HPs was the most easily abstracted by hydroxyl radicals to form the coupling precursor, i.e., phenoxy radicals. This high coupling behavior further resulted in the increased toxicity to green algae. Characterization revealed that HP reaction solutions treated with PS had a severely negative effect on algae growth, photosynthetic pigment synthesis, and the antioxidant enzyme system. These findings can shed light on the reaction mechanisms of advanced oxidation technologies and some risk management and control of PS technique may be considered when treating phenolic pollutants.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jing Tang,Xue Bai,Hongliang Huang,Songlin Xue,Jianming Pan
Simple and green synthesis of oxime or amidoxime functionalized hollow sorbents are critical for meeting the demands of highly efficient uranium extraction. To address this, a facile methodology using air bubbles generated from the “Ouzo-Like” effect as templates to synthesize oxime/amidoxime functionalized hollow PDA nanospheres (H-PDA-SO and H-PDA-AO) with fast and massive uranium extraction performances was reported. When 50 mL of Tris solution (0.6 mg mL −1 ) was mixed with n -propanol (6.25 mL) for 2.0 min, nanobubbles with the mean size of 56.7 nm spilled out, and uniformly sized H-PDA-SO nanospheres with oxime groups (about 250 nm) and H-PDA-AO nanospheres with amidoxime groups (about 150 nm) were simply obtained via self-assembled polydopamine and post-modification around the air/water interface. Owing to the accessible affinity sites and hollow structure, H-PDA-SO and H-PDA-AO displayed high maximum adsorption capacities (103.09 mg g −1 and 331.62 mg g −1 at 298 K) and fast adsorption rate (below 60 min) with high removal efficiency. Under the influence of coexisting ions, H-PDA-SO and H-PDA-AO showed not only a high uranium adsorption capacity but also a more predominant capacity than all the competing ions. Moreover, H-PDA-SO and H-PDA-AO exhibited high stability as well as excellent recyclability toward uranium capture after five regeneration cycles. Surface coordination of oxime/amidoxime sites with uranium was the main binding mechanism, and negative charged O-containing function groups enhance this affinity interactions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Peiwen Zhu,Yi Wang,Xue Bai,Jianming Pan
Highly efficient adsorption of radioactive uranium from seawater is a grand challenge of mounting severity as the energy demand increases. To address this, a salicylaldoxime functionalized raspberry-like microbeads sorbent is created to achieve highly efficient uranium adsorption via the CO 2 -in-Water Pickering emulsion-assisted polymerization-induced self-assembly method. The prepared raspberry-like microbeads sorbent with a high density of accessible functional groups exhibits the maximum uranium adsorption capacity of 41.02 mg g −1 within 30 min, the time required to reach adsorption equilibrium is shorter than most of the reported amine-oxime functionalized microsphere adsorbents. In addition, under the coexistence of high-concentration metals such as Na + , Mg 2+ , K + , Ca 2+ , etc., the raspberry-like microbeads sorbent still showed the best affinity for uranium, which is mainly benefit from the specific binding between amine oxime group and uranium. Our work not only provides a general strategy for the rapid and selective adsorption of uranium from seawater, but also provides a new perspective for the controlled assembly of NSs and the preparation of nano-hybrid materials combining the advantages of micro/nano structures.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Zhili Li,Feng Rao,Shaoxian Song,Alejandro Uribe-Salas,Alejandro López-Valdivieso
Effects of common ions, namely hydroxyl ions and carbonate, on the adsorption and flotation of malachite with salicylaldoxime as a collector was investigated, making use of solubility, micro-flotation, zeta potential , contact angle, FTIR, and XPS measurements. The results suggested that hydroxyl and carbonate ions affect malachite recovery through altering solubility of this mineral. Under conditions of lower solubility, more stable copper atoms acted as adsorption sites for retaining salicylaldoxime on the malachite surface, and the collector consumed by copper species in slurry was reduced. This allowed more collectors to get adsorbed onto malachite surface, resulting in improved malachite recovery. Zeta potential, FTIR, and XPS measurements indicated that salicylaldoxime chemically adsorbs onto malachite by forming copper salicylaldoxime chelates, in which two salicylaldoxime molecules react with one copper atom by N atom and the O atom combined with benzene ring .
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Journal of Central South University
·
2018
·Vol. 25
·期 4
·701-708
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IF 0.761
Kong Qian,Bai Xiu-zhi,Lin Hui-ju,Li Hai-pu,Yang Zhao-guang
For the determination of salicylaldoxime in environmental water samples, a stable and rapid method with low detection was proposed and established, based on the liquid-liquid extraction-high performance liquid chromatography with ultraviolet detector. Parameters including extraction solvent, ionic strength, solution pH, and extraction pattern were discussed for the optimal quantification of salicylaldoxime-spiked water. When the described method was applied to four spiked water samples, the obtained average extraction recovery rate was found between 87%–107% and relative standard deviation was below 6%. At the same time, good linear relationships were observed for spiked water samples from 0.01 to 10 μg/mL ( R 2 =0.9993). In addition, the detection limit of salicylaldoxime was revealed between 0.003–0.008 μg/mL, which is two orders of magnitude lower than previously reported results. Thus, the presented method may be advantageous for the high-efficiency determination of salicylaldoxime in water samples.
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DESALINATION
·
2024
·
IF 8.3
Linzhe Xu,Yingbo Chen,Yuanyuan Zhang,Meng Wang,Siyu Wei,Xinyu Zhao
Uranium, as a radioactive element, is the source of utilizable energy for mankind in the future. Large quantities of uranium resources are contained in seawater, so uranium extraction from seawater is undoubtedly the most feasible method. However, the presence of competitive ions such as vanadium hinders the efficient extraction of uranium, which is currently a challenge that needs to be solved. Here, silane coupling agent (KH550) was grafted onto two-dimensional metal carbide (MXene). Subsequently, salicylaldoxime (SA) was deposited onto MXene particles using self-polymerization of dopamine (DA) to prepare PDA/SA deposited MXene composite grafted with KH550 (PDA/SA/MXene-KH550). The adsorbent exhibited excellent selectivity for uranium ions with a uranium/vanadium selectivity ratio of 4.8. In antibacterial experiments, the PDA/SA/MXene-KH550 composite showed excellent antibacterial performance against Escherichia coli ( E. coli ) and Staphylococcus aureus ( S. aureus ), demonstrating the ability to adapt to complex marine microbial contamination. In addition, the maximum experimental uranium adsorption capacity of the composite was 332.3 mg/g, following the pseudo-second-order kinetic model and the Langmuir isotherm model. After five adsorption-desorption cycles, the elution efficiency of PDA/SA/MXene-KH550 for uranium can still reach 74.7 %, which demonstrated that the adsorbent had superior stability and regeneration ability, providing the possibility for actual enrichment of uranium.
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Minerals
·
2017
·Vol. 7
·期 2
·20
·
IF 2.088
Zhili Li,Feng Rao,Shaoxian Song
To separate one base metal mineral from another by flotation, it is indispensable to identify chemical reagents that specifically interact with the surface metal sites of one mineral or a group of minerals. This work studies the interactions of chelating collectors which offer the best potential for collecting abilities and mineral specificity with a typical refractory oxide mineral (malachite). Zeta potential, adsorption and Fourier transform infrared (FTIR) measurements are applied to differentiate the interactions of salicylaldoxime and salicyl hydroxamate on the malachite surface. Salicylaldoxime and salicyl hydroxamate are of molecular structures that resemble each other, but with different bond distances in the ligand atoms which result in their unusual adsorption behavior and collecting ability. Thus, the flotation of malachite behaves differently with the two chelating collectors. This study might provide useful clues for designing novel collectors in base metal oxide flotations.Keywords:malachite;flotation;chelating collector;adsorption
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DESALINATION
·
2024
·
IF 8.3
Wen Guo,Zixin Lin,Kun Jiang,Hao Li,Xiangfeng Liang,Weizhong An,Huizhou Liu,Haiyan Luo,Haoyu Yao
The extraction of uranium from seawater is not only crucial from a strategic standpoint but also poses significant technical challenges. In this work, a series of novel bifunctionalized mesoporous silicas were prepared through a straightforward method, utilizing the structural characteristics of SBA-15 and synergistic effect of functional groups. The impact of pH value, initial uranium concentration, temperature, and duration on uranium adsorption was investigated through a series of batch experiments. The bifunctional modified SBA-15 demonstrated rapid uranium adsorption, which was a spontaneous endothermic reaction and conformed to the pseudo-second-order model. Thereinto, SBA-15 modified with aldoxime and amino group (SBA-15-SAO-N) exhibited the best uranium adsorption performance, with a maximum adsorption capacity of 701.85 mg·g −1 at 298 K and pH 6, an increase of 146 % compared to SBA-15-SAO. SBA-15-SAO-N exhibits excellent U/V selectivity (selectivity coefficient of 30) in the coexistence of U and V solutions, and it still maintains high adsorption capacity after five adsorption-desorption cycles. In actual seawater conditions, the adsorption capacity of SBA-15-SAO-N was 135.26 μg·g −1 . By combining DFT calculations and characterization, the coordination model and interaction energy between functional groups and uranyl were elucidated, revealing that introducing bifunctional groups can enhance the binding strength of adsorbents to uranium and form more stable complexes, thereby improving adsorption capacity and selectivity. These results indicate that bifunctional modified mesoporous silica offers a promising strategy for recovering uranium resources from seawater.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhibin Chen,Jinke Wang,Lin Lu,Thee Chowwanonthapunya,Weiting Chen,Zongbao Li,Lingwei Ma,Dawei Zhang
A corrosion-oriented self-healing coating system relying on metal–organic framework (MOF) based nanofiller is designed for aluminum alloy protection. The nanofiller is comprise of ZnMg MOF nanoparticle as a framework, salicylaldoxime corrosion inhibitors inside the MOF, and a polydopamine layer on the MOF surface. The Al 3+ ions generated from the aluminum alloy substrate at the damaged coating area can etch the nanofiller, causing the collapse of the nanofiller and releasing the corrosion inhibitors to suppress the corrosion process in time. Subsequently, Zn 2+ and Mg 2+ ions from the nanofiller co-precipitate with Al 3+ to form a dense AlZnMg layered double hydroxide (LDH) film, which provides further protection performance at the exposed alloy surface. Electrochemical impedance spectroscopy results demonstrate that the intact MOF@S/P coating exhibits a remarkable corrosion resistance property. For the damaged coating, the self-healing performance originated from the formation of LDH layer and the release of corrosion inhibitors gradually took effect, with the |Z| 0.01Hz value increasing 2.27 times within 14 days. Moreover, under near-infrared irradiation, the photothermal effect of polydopamine will accelerate the release of corrosion inhibitor, the formation of LDH film, as well as the shape memory effect of coating defect for an efficient recovery of the corrosion resistance property. This novel coating system enables a corrosion-driven and location-specific repair with in-situ deposition of both an inhibitor film and an LDH film. As the first work to fully utilize and consume nanofillers on demand, this approach prevents inadequate use of healing agents, addressing a significant challenge in corrosion-driven self-healing coatings. The self-healing mechanism ensures target-oriented corrosion protection that makes the most efficient use of the healing substances.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Juan Wang,Mingbu Luo,Qipu Lin
Two isomorphic titanium-doped organotin-oxo aromatic aldoxime clusters, SnTi-1 and SnTi-2, have been successfully synthesized via a solvothermal method . Both clusters have an identical undecameric core, consisting of a pentagonal wheel-shaped moiety {Ti 5 } and two alkylate trimers {Sn 3 } fused together, and decorated with unsubstituted and methoxy-substituted aldoxime ligands, respectively. They exhibit excellent solubility, chemical stability, and hydrophobicity owing to the existence of peripheral protective shells of alkyl and aromatic groups. The steric hindrance effect of methoxy induces a rearrangement of clusters, altering weak interactions from C–H···π to π···π between cluster molecules, and ultimately modulating the third-order nonlinear optical from saturation absorption to reverse saturation absorption.
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