ACS Nano
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2020
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IF 14.588
Jiani Zhu,Lei Wang,Jin Wang,Fudi Wang,Mengtao Tian,Shuchang Zheng,Ning Shao,Lele Wang,Miaolu He
Two-dimensional (2D) membranes exhibit exceptional properties in molecular separation and transport, which reveals their potential use in various applications. However, ion sieving with 2D membranes is severely restrained due to intercalation-induced swelling. Here, we describe how to efficiently stabilize the lamellar architecture using Keggin Al13 polycations as pillars in a Ti3C2Tx membrane. More importantly, interlayer spacing can be easily adjusted with angstrom precision over a wide range (2.7–11.2 Å) to achieve selective and tunable ion sieving. A membrane with narrow d-spacing demonstrated enhanced selectivity for monovalent ions. When applied in a forward osmosis desalination process, this membrane exhibited high NaCl exclusion (99%) with a fast water flux (0.30 L m–2 h–1 bar–1). A membrane with wide d-spacing showed notable selectivity, which was dependent on the cation valence. When it was applied to acid recovery from iron-based industrial wastewater, the membrane showed good H+/Fe2+ selectivity, which makes it a promising substitute for traditional polymeric membranes. Thus, we introduce a possible route to construct 2D membranes with appropriate structures to satisfy different ion-sieving requirements in diverse environment-, resource-, and energy-related applications.
研究领域:
材料科学
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环境工程
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分离技术
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DOI
PubMed
高影响因子
DALTON TRANSACTIONS
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2020
·Vol. 49
·期 8
·2559-2569
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IF 4.174
Shuang Wang,Shuying Li,Rui Shi,Xinyu Zou,Zhijuan Zhang,Guoyuan Fu,Lei Li,Fang Luo
A nanoscale hybrid material (V2O5–Al13) for highly efficient alcohol oxidation is synthesized through electrostatic self-assembly between oppositely charged Keggin Al13 polyoxocations and exfoliated V2O5 nanosheets. The analyses by X-ray diffraction, electron microscopy, X-ray photoelectron spectroscopy and structural consideration based on charge balance indicate that the Keggin Al13 ions could be sparsely distributed in the nanosheet galleries. The as-prepared catalyst successfully achieved high catalytic activity toward alcohols (96.8% sel.) with the oxygen molecule as an ideal oxidant under mild conditions. Also, the nanohybrid showed an outstanding adsorption capability for benzyl alcohol (773 mg g−1). In comparison to individual exfoliated V2O5 nanosheets and bulk V2O5, the V2O5–Al13 nanohybrid catalyst exhibited superior catalytic activity and selectivity under the same experimental conditions. The results highlight the outstanding functionality of the V2O5–Al13 nanohybrid as an efficient oxidation catalyst. A detailed study of its structure–activity relationship showed that the high performance of the V2O5–Al13 nanohybrid is attributed to the adsorption–catalysis synergistic effect between V2O5 and Al13.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Ruyuan Jiao,Lijuan Huo,Xin Xin,Dongsheng Wang,Weijun Zhang
In this study, a multi-functional coagulant with both coagulation and oxidation function was obtained by pre-doped nano zero-valent iron (nZVI) with Al 13 for the removal of the typical emerging contaminants Carbamazepine (CBZ). At the optimal doped dosage of nZVI, the pre-doped agent (Al 13 @nZVI) showed 23% improvement of the maximum removal rate of Carbamazepine compared with Al 13 under pH 7. It was found that Al 13 @nZVI could produce H 2 O 2 in situ at pH 2 to pH 8, especially under acid conditions. By the analysis of FT-IR, it could be found that the groups of C-N, benzene, and C O were disappeared after treatment. Instead, -NO 2 was found in treated water which indicated the breakage and oxidation of amine group. Thus, the effects of pH on Al 13 and Al 13 @nZVI were different. Al 13 will undergo depolymerization and decompose into small polymers with low positive charge density with the increasing of pH, while, because of Al 13 @nZVI having oxidation ability, effect of pH on Al 13 @nZVI was not that significant. The influence of Humic acid (HA) with different concentration on CBZ removal were analyzed. The system with 2 mg/L HA showed better removal performance of both CBZ and total dissolved organic carbon (DOC) compared to the system with 1 mg/L HA, which may because of the increase of the necessary nuclei for the flocs formation, as well as the bridging function by the long chain structure of HA. Moreover, Al 13 @nZVI was found improved the removal efficiency of organic matters with molecular weight about 1500–2000 Da compared to Al 13 .
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DOI
高影响因子
WATER RESEARCH
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2021
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IF 11.236
Guangyu An,Ye Yue,Pin Wang,Libing Liu,Hailu Demissie,Ruyuan Jiao,Dongsheng Wang
Unraveling the transformation of coagulants and their interaction with contaminants at the micro-level is vital to advancing our understanding of the coagulation mechanism. To the best of our knowledge, the coagulation effectiveness of [AlO 4 Al 12 (OH) 24 (H 2 O) 12 ] 7+ (Al 13 ), regarded as the dominant species in polyaluminum chloride (PACl), is highly related to its aggregation characteristic, but the detailed process of Al 13 aggregation in coagulation time scale was not well studies. Here we systematically studied the deprotonation and aggregation processes of Al 13 by alkaline titration to simulate the reaction in coagulation case. By reacting with OH − , Al 13 can continuously lose protons regardless of pH until its positive charge was well neutralized. The initial Al 13 aggregates (Al 13 agg) appeared at B of 2.70 and large Al 13 agg was generated by coalescence of small initial Al 13 agg. Most Al 13 polycations kept their main structure unchanged during aggregation and part was decomposed into monomers or oligomers. Density functional theory (DFT) results reveal that Al 13 becomes unstable after deprotonation, but the aggregation of Al 13 bridged by Al monomers can stabilize the polycations. Al 13 needs to be hydrolyzed before interacting with colloidal particles, but particles can promote the aggregation of Al 13 by weakening the repulsion force between the polymers. Strong and compact flocs can be generated induced by in-situ aggregation of Al 13 in neutral and alkaline conditions. This study can provide a deep understanding about the role of Al 13 agg in removing particles and instruct the development of new efficient coagulants against the various water qualities.
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
DESALINATION
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2024
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IF 8.3
Jinjin Jia,Jinlong Wang,Dachao Lin,Jing Zhao,Hesong Wang,Longfeng Hu,Jiaxuan Yang,Han Zhang,Guibai Li,Heng Liang
Membrane scaling severely hinders practical application of nanofiltration (NF) for brackish water treatment. However, the contributions of residual aluminum ( Al ), especially various species with differing polymerization degrees and sizes, to gypsum scaling remain unclear. Herein, the complex interactions between three Al species (AlCl 3 , Al 13 and Al 30 ) and gypsum scaling were investigated, including surface and bulk crystallization processes. Results demonstrated that Al species adhering to the membrane surface promoted surface crystallization and altered crystal morphology. Notably, the Al 13 species induced the formation of dense, complete rosette crystals causing the most severe flux decline. For bulk crystallization, Al 30 was the primary species to promote nucleation. This promotion resulted from two factors: a lower nucleation energy barrier and the promoted aggregation of small crystals. Furthermore, molecular dynamics (MD) simulations revealed that the inhibition of nucleation due to the competition between Al species and calcium ions at nucleation sites was negligible compared to the strong promotion effect. These findings demonstrated that PACl exhibit higher scaling potential during NF than monomeric Al coagulants. Ultimately, the competition between surface and bulk crystallization determined the final membrane flux decline. This study offers valuable insights into the mechanisms of NF scaling caused by residual Al and guides mitigation strategies.
研究领域:
环境科学
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水处理
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膜技术
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shanshan Qu,Jin Zhang,Yu Xiang,Jie Luo,Yan Zhang,Wenbo Wang,Hui Xu
Disinfection by-products (DBPs), which formed in the process of chlorination disinfection of water, has a potential threat to human health. To date, Natural organic matter (NOM) is the precursor of DBPs so that it is important to remove the NOM to reduce the generation of DBPs. Coagulation is a key process to remove the NOM from water. However, the traditional coagulants have poor removal ability for hydrophilic(HPI) NOM. In this study, multi walled carbon nanotubes was modified with Mg, Ca and Fe to produce modified multi walled carbon nanotubes and then reacted with Al 13 to produce composite coagulant. Al 13 and composited coagulants were utilized to treat water with bovine serum albumin to compare the removal efficiency for HPI NOM. The results showed that the composited coagulant had a relatively high removal efficiency for organic matter, and among them, the effect of Al 13 -MgMW is best. The DOM removal rates of Al 13 and Al 13 -MgMW at doses of 0.12 mmol/L were 64.8 % and 75 %, respectively. Meanwhile, Al 13 -MgMW had an 89.2 % removal rate for HPI NOM. The XPS and FTIR of flocs showed that the Al 13 -MgMW had a significant removal ability for O C substances such as proteins. MgMW has a larger specific surface area and pore volume. ESI-TOF-MS results showed the composited coagulants retain the original structure of Al 13 , and thus preserve and improve the advantages of Al 13 .
研究领域:
环境科学
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水处理工程
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材料科学
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产品关联
DOI
高影响因子
Desalination and Water Treatment
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2016
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IF 1.272
Xiang Li,Qian Deng,Zaili Zhang,Xiaoshan Jia
In this study, remediation of tetrabromobisphenol-A (TBBPA) from aqueous solution by sorption using transition metals-modified inorganic–organic montmorillonite (IOMt) was demonstrated. The adsorbents were prepared in two steps: (1) intercalation of surfactants into Al13-pillared montmorillonite for synthesizing two types of IOMt; (2) incorporation of transition metals (Cu2+, Ni2+, or Co2+) onto those IOMts. Firstly, these materials were characterized by XRD, FTIR, TGA, SEM-EDS, and BET analyses. Then, experiments were conducted on the sorption isotherms, kinetics, and thermodynamics of TBBPA. In general, sorption process with Cu- and Ni-modified IOMt achieved higher TBBPA removal efficiency than sorption process with original IOMt. The modified IOMt displayed the sorption capacity that varied depending on TBBPA initial concentration, pH, and metals loading. However, the type of surfactants did not influence TBBPA sorption on metals-modified IOMt. This probably indicated that complex interaction between TBBPA and metals rather than hydrophobicity plays a key factor in TBBPA sorption process. Equilibrium data could be well interpreted by the Freundlich model, and the rate of sorption was adjusted to a pseudo-second-order kinetic model. The negative values of Gibbs energy change (∆G) and positive values of enthalpy change (∆H) indicated the spontaneous and endothermic nature of process.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Shiyi Hu,Yadong Wang,Mengwen Liu,Yabo Shang,Keqian Li,Lu Xu,Xue Bai,Xuan Shi,Xin Jin,Pengkang Jin
The removal of low-coagulability organic matter remains a major challenge for conventional coagulation (CC) process. Enhancing the formation of highly active polymeric coagulant species such as Al 13 is a possible strategy for improving the removal efficiency of low-coagulability organic matter. In this work, it was found that synchronous ozonation promoted the generation of freshly-formed polymeric hydrolyzed Al species during coagulation process at pH 5 and 7 through hydroxyl bridges (μ-OH) derived from surface hydroxyl groups and surface protonated hydroxyl groups. The freshly-formed polymeric hydrolyzed Al species generation during synchronous ozonation was unveiled through density functional theory (DFT) calculation. Therefore, the hybrid ozonation-coagulation (HOC) process was established, in which ozonation and coagulation occurred synchronously in a single reactor. Using 2,4-dichlorophenoxyaceticacid (2,4-D) as a typical low-coagulability organic, the HOC process achieved nearly 60 % dissolved organic carbon (DOC) removal efficiency, which significantly outperformed both the pre-ozonation coagulation (POC) and CC processes. Surface hydroxyl groups and surface protonated hydroxyl groups formed during Al hydrolysis can also serve as active sites to catalyze ozone to enhance •OH generation, which can improve the transformation of 2,4-D to oxidized intermediates. Freshly-formed polymeric hydrolyzed Al species exhibited a stronger ability to capture oxidized 2,4-D intermediates such as 2,4-dichlorophenol, 4,6-dichlororesorcin, 2-chlorohydroquinone, facilitating the separation performance due to enhanced floc formation. Stronger binding ability of freshly-formed hydrolyzed Al species with 2,4-D intermediates via hydrogen bonding and complexation was also proved by DFT calculation in molecular scale. As consequence, freshly-formed polymeric hydrolyzed Al species generated during the HOC process enhanced the capture of low-coagulability organic intermediates, which finally improved the low-coagulability organic matter removal.
研究领域:
环境科学
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化学工程
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水处理技术
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材料科学
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物理化学
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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）