APPLIED CLAY SCIENCE
·
2020
·
IF 4.605
Yaowu Cao,Qinghai Guo,Mengsi Liang,Weihao Sun
Antimony enrichment in aquatic environments is of great concern to international community. High-temperature geothermal waters usually contain excessive Sb, which are apt to contaminate the groundwaters or surface waters used as drinking waters in and around a hydrothermal area. However, Sb removal from geothermal water is rarely documented and the effect of high temperature on Sb removal has not received much attention. In this study, batch sorption experiments were conducted to investigate Sb removal from water by a hydroxyl-intercalated, mechanochemically synthesized Mg-Fe-LDH (i.e. Mg-Fe-OH-LDH) capable of avoiding secondary pollutions commonly related to other Mg-Fe-LDH intercalated by undesirable anions, such as Cl − and NO 3 − . The sorption capacities of Mg-Fe-OH-LDH for Sb(III) and Sb(V) were up to 48.7 and 30.0 mg/g, respectively. Notably, Mg-Fe-OH-LDH performed even better in removing aqueous Sb(V) at higher temperatures, superior to sorption of Sb by iron oxides that is generally exothermic and tends to be inhibited by increasing reaction temperature. The removal of Sb(V) existing as Sb(OH) 6 − by Mg-Fe-OH-LDH was attributable to its exchange with interlayer hydroxyl, and therefore could be impaired to some degree by coexisting anions with stronger electronegativity or smaller ionic radii . In contrast, anion exchange didn't contribute so much to Sb(III) sorption, because the main Sb(III) species at pH < 10 is neutral Sb(OH) 3 . XPS analyses confirmed that inner-sphere complexation between sorbed Sb(III) and Fe on Mg-Fe-OH-LDH layers was formed, which was hardly affected by competitive anions. Mg-Fe-OH-LDH is promising to be practically applied in removing both Sb(III) and Sb(V) from contaminated natural waters, wastewaters, or geothermal waters potentially acting as a pollution source .
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xin Wang,Yawen Cai,Tianhao Han,Ming Fang,Kechang Chen,Xiaoli Tan
Elimination of U(VI) from polluted solutions is important for human health and environmental safety. In this work, a relatively low-cost 3D flower-like phosphate-functionalized layered double hydroxides (phos-LDH) was fabricated by a one-pot hydrothermal method. The prepared phos-LDH inherited the structure of 3D flower-like layered double hydroxides (LDH), and had a higher specific surface area (∼203.4 m 2 ⋅g −1 ) than that of LDH. The kinetic process indicated that U(VI) adsorption onto phos-LDH achieved equilibrium within 15 min and obeyed general order model. The adsorption isotherms of phos-LDH illustrated that the U(VI) adsorption obeyed Langmuir model, the adsorption capability of phos-LDH can reach 923.1 mg⋅g −1 at 298 K. The U(VI) adsorption was a spontaneous and endothermic process according to the thermodynamic data. There was the electrostatic attraction between U(VI) and phos-LDH at pH = 5.0. FTIR and XPS analyses educed that the hydroxyl and phosphate groups played a very useful role for the complexation between U(VI) and phos-LDH. In addition, the excellent selective adsorption capability for U(VI) in competitive cation and anion solutions further confirmed the practical application of phos-LDH in real wastewater treatment.
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PubMed
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 23
·4937-4947
·
IF 5.686
Chenglin Miao,Fengyu Zhang,Luoyu Cai,Tianli Hui,Junting Feng,Dianqing Li
Graphical Two kinds of electron-rich interface sites are clearly identified in ultrathin Pt/CoAl-LDH catalyst. A series of technologies found that the Pt−V O −Co δ+ interface site can change the adsorption mode of C=O bond, and the Pt−V Co −OH δ− interface site facilitates the mobility of active hydrogen. Therefore, the ultrathin catalyst exhibits enhanced COL yield under the synergistic effect of the dual interface sites. Focusing on the simultaneous enhancement of activity and selectivity in α, β-unsaturated aldehyde hydrogenation, we designed and prepared an ultrathin CoAl-LDH supported Pt catalyst. A series of technologies revealed the ultrathin CoAl-LDH support possesses the characteristic of dual defects, oxygen vacancy (V O ) and cobalt vacancy (V Co ). Then, two kinds of vacancy related interface sites were identified, namely Pt−V O −Co δ+ and Pt−V Co −OH δ− . Compared with the bulk catalyst, the ultrathin catalyst exhibits both enhanced intrinsic activity and C=O bond selectivity under the synergistic effect of the dual interface sites. Specifically, the Pt−V O −Co δ+ interface site changes the adsorption mode of cinnamaldehyde and promotes the activation of C=O bonds, thus leading to the improved cinnamyl alcohol selectivity. The H atoms of the Pt−V Co −OH δ− interface site participate in the hydrogenation process, which facilitates the mobility of active hydrogen and therefore promotes the intrinsic activity. More importantly, the ultrathin catalyst shows good reusability.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 16
·B1681
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IF 3.12
Dandan Song,Lili Wang,Yuning Qu,Bing Wang,Yanting Li,Xueli Miao,Yuying Yang,Cunpeng Duan
Constructing a reasonable electrode material structure is significant for the sensitivity and selectivity of glucose detection. Herein, in this paper, the three-dimensional (3D) hierarchically layered double hydroxides (CC@CCH MOF LDH) is prepared by using carbon cloth (CC) as the conductive base, cobalt carbonate nanorod (CCH) as the guiding template and metal organic framework (MOF) as the sacrifice template. This unique 3D hierarchical structure facilitates the rapid transfer of ions and the reversible redox reaction. Moreover, the electrochemical tests confirm that the material has excellent electrocatalytic oxidation activity in alkaline solution. The amperometric detection results reveal that CC@CCH MOF LDH electrode material possesses better selectivity, higher sensitivity (4310 μA·mM−1·cm−2), fast amperometric response (<6 s), wide linear range (0.001-2 mM) and low detection limit (110 nM) under the optimal conditions, which is expected to be a high performance enzyme-free glucose sensor.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Qiongguang Li,Yanhong Wang,Bin Lu,Jing Yu,Menglei Yuan,Qiangqiang Tan,Ziyi Zhong,Fabing Su
Vast volume expansion of Si-based materials severely deteriorates the electrochemical performance of lithium-ion batteries (LIBs). To overcome this problem, we designed and synthesized Si@NiAl-LDH (layered double hydroxide) hybrid composites with the unique hollow core-shell structure via a re-precipitation and in situ growth process. In principle, the core of Si nanoparticles (Si NPs) can contribute to a high Li-storage capacity, the void space between the shell of LDH and the Si-core can effectively tolerate the volume expansion of Si NPs, and the shell can maintain the structural integrity and contribute to the electrochemical performance as well. As demonstrated, when used as the anode materials of LIBs, Si@NiAl-LDH exhibited much enhanced electrochemical performance as compared with the LDHs. The Si@NiAl-LDH electrode had a reversible capacity of 534 mAhg −1 after 60 cycles at 50 mAg −1 while that of NiAl-LDH was 343 mAhg −1 only. Regarding the rate performance, the Si@NiAl-LDH electrode could revert to 565 mAhg −1 after a rate test, while that of NiAl-LDH electrode was 353 mAhg −1 only. Obviously, the obtained clear structure-property relationship of the anode materials will be very conducive to the design and synthesis of the high-performance next-generation materials for energy storage and conversion.
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高影响因子
RSC Advances
·
2018
·Vol. 8
·期 23
·12870-12878
·
IF 2.936
Li Tan,Hailong Li,Mengru Liu
In this study, CMC–LDH beads were prepared and characterized using SEM, FTIR and TG analysis. The beads were applied for the removal of Cr(VI) from aqueous solution. The effects of adsorbent dosage, initial pH and initial concentration of Cr(VI) solution on Cr(VI) uptake were investigated in detail. Moreover, adsorption isotherms and adsorption kinetic models were employed to analyze the adsorption process, and a preliminary study of the reusability of the adsorbent was performed. The experimental results showed that the CMC–LDH beads could remove Cr(VI) from aqueous solution efficiently. When the initial concentration of the Cr(VI) solution was 100 mg L−1 and the adsorbent dosage was 12 g L−1, the removal efficiency of Cr(VI) reached 96.2%. After the CMC–LDH beads were reused 10 times, the removal efficiency of Cr(VI) still remained at 89.6%.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2018
·
IF 6.578
Jiuyun Cui,Zhiping Zhou,Atian Xie,Qianqian Wang,Siwei Liu,Jihui Lang,Chunxiang Li,Yongsheng Yan,Jiangdong Dai
Development of antifouling membrane to separate oil–water emulsions by low energy consumption approach is an urgent demand. Herein, we report for the first time a grass-like structured composite membrane from array growth of nickel cobalt layered double hydroxide (NiCo-LDH) onto the polydopamine modified polyvinylidene fluoride (PVDF) membrane surface via simple hydrothermal strategy. The surface morphology of as-prepared membrane has controlled by hydrothermal time. The obtained NiCo-LDH/PVDF composite membrane exhibits superhydrophilicity/underwater superoleophobicity for separating both surfactant-free and surfactant-stabilized oil–water emulsions by capillary effect under the driving of gravity. Moreover, with the advantages of antifouling performance, the membrane displays outstanding cyclic performance for long-term application, which is promising for practical oily wastewater treatment .
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Kiran Gupta,Jiang-Bo Huo,Jia-Cheng E. Yang,Ming-Lai Fu,Baoling Yuan,Zhangxu Chen
We introduced (MoS 4 ) 2− moiety into the lamellar layers of Ca 0.66 Al 0.34 (OH) 2 (NO 3 ) 0.34 ⋅yH 2 O to fabricate Ca 0.66 Al 0.34 (OH) 2 (MoS 4 ) 0.17 ⋅yH 2 O (CA-MoS 4 ⋅LDH), a stable and efficient adsorbent for removal of two envoy Fluoroquinolones (FQs), Ciprofloxacin (CIP) and Ofloxacin (OFL), from contaminated aquatic sources. Various characterization tools, such as X-ray diffraction (XRD), Scanning electron microscopy, Energy dispersive X-ray spectrometer, transmission electron microscopy , X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy and Thermogravimetric analyses etc. were applied to confirm structural and compositional changes during the synthesis and adsorption properties of CA-MoS 4 ⋅LDH. The efficiency of adsorbent was investigated by evaluating different parameters including contact time, pH of solution, initial concentration of pollutant, and effect of temperature. By using CA-MoS 4 ⋅LDH as adsorbent, we found more efficient removal of CIP than that of OFL due to the steric hindrance. The highest uptake of 707.20 mg/g and 476.74 mg/g of CIP and OFL, respectively, was found at pH of 6 with improved kinetics and easily reusability for these representative antibiotics models so far. Removal kinetics of both FQs were found to better follow the pseudo-second-order kinetic model than the pseudo-first-order. The Langmuir adsorption isotherm was employed to understand the removal process, suggesting monolayer chemisorption mechanism. The adsorbate-adsorbent interaction revealed remarkable features originate from the combination of weak hydrogen bond interaction between thio group and NH 2 + group of antibiotic and electrostatic interaction between positive LDH layer and COO − group of antibiotic as well, and anion exchange mechanisms, which were also confirmed by XRD, FTIR, XPS and Raman spectrum etc. obtained after adsorption. It is proposed that all (MoS 4 ) 2− moiety offers stability to the CA-MoS 4 ⋅LDH structure to avoid its solubility under ambient environments.
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GREEN CHEMISTRY
·
2016
·Vol. 18
·期 21
·5900-5914
·
IF 8.506
Shuangtao Yin,Jin Li,Hui Zhang
A series of honeycomb-like hierarchical hollow nanostructured magnetic catalysts, γ-Fe2O3@M3Al-LDH@Au25-x (x represents determined mass of gold in wt%), have been successfully fabricated by modified electrostatic adsorption of water-soluble captopril-capped Au25 nanoclusters (Au25Capt18) on pre-prepared magnetic supports, Fe3O4@M3Al-LDH (M = Ni, Mg, or Cu/Mg (0.5/2.5), LDH: layered double hydroxide) followed by proper calcination. The characterization results show that the low Au-loading samples, γ-Fe2O3@Ni3Al-LDH@Au25-x (x = 0.053, 0.11), show nearly atomically precise Au25 nanoclusters (Au25NCs) (∼1.4 ± 0.3–1.9 ± 0.6 nm) dispersed on the surface of the Ni3Al-LDH shell, while the catalysts, γ-Fe2O3@M3Al-LDH@Au25-x (x ∼ 0.2), display slightly aggregated Au25NCs on the LDH shell with sizes of ∼3.0 ± 1.3, 3.3 ± 1.2, and 4.2 ± 1.5 nm for Ni-, Mg-, and CuMg-based catalysts, respectively, related to varied synergy between Au25NCs and magnetic LDH supports at slightly higher Au loadings. All the γ-Fe2O3@M3Al-LDH@Au25-x catalysts exhibit much higher catalytic activity for the oxidation of 1-phenylethanol under atmospheric O2, without basic additives, in toluene than Fe3O4@Mg3Al-LDH@Au prepared by a traditional deposition–precipitation method. The catalyst, γ-Fe2O3@Ni3Al-LDH@Au25-x, presents even higher alcohol oxidation activity than γ-Fe2O3@Mg3Al-LDH@Au25-0.21 and γ-Fe2O3@Cu0.5Mg2.5Al-LDH@Au25-0.2 and, particularly, γ-Fe2O3@Ni3Al-LDH@Au25-0.053 exhibits the highest activity (TOF: 112 498 h−1) for the aerobic oxidation of 1-phenylethanol under solvent-free conditions and can be applied for a variety of alcohols, this being mainly attributed to its nearly atomically precise Au25NCs and remarkable Au25NCs–LDH–magnetic core three-phase synergistic interaction, along with its abundant Ni-OH sites. Moreover, γ-Fe2O3@Ni3Al-LDH@Au25-0.053 can be easily separated, by simply applying an external magnetic field, and reused for more than ten runs without significant loss of activity, giving the magnetic catalysts long-term stability. These observations make Fe3O4@LDH a universal green platform to support other noble or non-precious metal nanoparticles by using a metal nanocluster precursor method to construct desired metal-loaded ecofriendly catalysts that can be applied in a broad range of heterogeneous catalysis processes.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yan-Mei Zhang,Li-Hao Xu,Xiao-Xue Hu,Bing-Hong Chen,Xin-Ru Chen,Qian-Qian Li,Heng Mao,Zhi-Ping Zhao
Metal-organic framework (MOF) membranes, by virtue of their high selectivity and low diffusion resistance, make a significant contribution to energy conservation and CO 2 emission reduction via separation technology. Despite possessing substantial potential for propelling the production of high-performance membranes, hurdles persist in the process of constructing MOF membranes that are both highly integrated and structurally sound on flexible polymer substrates. We propose a strategy for constructing highly stable cobalt zeolitic imidazolate framework (ZIF-67) composite membranes on seeded polyacrylonitrile (PAN) substrate. Through a timed-interrupted in-situ growth process, the amino-modified polycrystalline ZIF-67 as a CO 2 affinity layer is precisely and completely confined within the “top sites” and partial “face sites” of the vertical layered double hydroxide (LDH) precursor layer, creating a barrier-low passage for CO 2 as a fast diffusion layer. The substrate and the hybrid ZIF-67@LDH layer were robustly anchored together by the pre-embedded LDH seeds, thereby producing an appealing membrane-multilayer interlocked-support (MMIS) composite architecture. This fast diffusion-CO 2 affinity Pebax/ZIF-67@LDH/PAN membranes with MMIS architecture show average CO 2 permeability of 1487 Barrer and CO 2 /N 2 selectivity of above 55.1 after the surface repair coating of polyether-block-amide (Pebax), maintaining stable performance over 150 h, surpassing the Robeson upper bound. The Pebax/ZIF-67@LDH/PAN membranes also exhibit the durability and mechanical robustness, because of the highly inducible activity of LDH precursor layer serving as a linker between the membrane and substrate. These results promote the development of MOF-based membranes in practical separation applications.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·
IF 1.5
Lu Sen,Yin Yuqiang,Bao Jiacheng,Wang Hongqiang,Lei Zhiwu,Hu Eming,Xin Qi,Quan Yihao,Wang Qingliang
In this study, tin sulphide (SnS 2 ) and nickel–chromium hydrotalcite (NiCr-LDH) complexes (SnS 2 /NiCr-LDH) were used for the simultaneous removal of U(VI) and humic acid (HA) from U(VI)-containing wastewater. The results showed that the adsorption of HA by the SnS 2 /NiCr-LDH was greatly enhanced, which was 4.07 and 2.94 times higher than that of pure SnS 2 and NiCr-LDH, respectively, and the highest U(VI) adsorption quantity over SnS 2 /NiCr-LDH increased from 127.81 to 446.68 mg g −1 when HA was present. Density functional theory (DFT) calculations revealed that the enhanced U(VI) adsorption on SnS 2 /NiCr-LDH was facilitated by the formation of a robust inner-sphere surface complex between U(VI) and HA.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2024
·
IF 2.6
Yan Yue,Wu Wenrui,Tian Xinyu,Wei Chengzhi,Xu Tao,Li Xianfu
Optimizing the performance of layered double hydroxide (LDH) electrodes by MXene is of significant importance for high-performance asymmetric supercapacitors. In this paper, CoAl-LDH nanosheet-doped s-MXene composites were prepared by a facile hydrothermal method, and two-dimensional layered microstructured CoAl-LDH/s-MXene electrode materials with excellent performance were prepared. The homogeneous growth of CoAl-LDH on s-MXene successfully hinders the agglomeration of CoAl-LDH and provides more layered channels for electron and ion transfer across the electrode material. In addition, CoAl-LDH can effectively suppress the stacking of s-MXene, which increases the electrochemical active site of the material, resulting in an increase in specific capacity. The CoAl-LDH/s-MXene electrode material has a high specific capacity of 1259.9 C g −1 at 1 A g −1 , which has outstanding specific capacity and rate capability. The assembled asymmetric CoAl-LDH/s-MXene//AC supercapacitor achieves the desired energy density of 104 and 88 Wh kg −1 at 1500 and 6000 W kg −1 . After 5000 laps at 10 A g −1 , CoAl-LDH/s-MXene//AC has a capacitance retention rate of 86.6% and a coulomb efficiency of nearly 100%, demonstrating its splendid cycling stability. Therefore, this paper adopts a simple hydrothermal method to prepare CoAl-LDH/s-MXene active material, which provides an effective strategy for constructing supercapacitors with excellent performance. Graphical abstract
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