CLAY MINERALS
·
2021
·Vol. 56
·期 3
·169-177
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IF 1.478
Xuefen Zhang,Mingxue Xiang,Zhongbang Zhu,Youqin Zou,Ping Zhang
Hierarchical layered double hydroxide (HLDH) was synthesized by using sodium dodecyl sulfate (SDS) as a soft-template agent for the removal of two charged organic dyes (i.e. methylene blue (MB; cationic dye) and methyl orange (MO; anionic dye)). The experimental results based on response surface methodology (RSM) demonstrated distinct removal behaviours of HLDH towards these two dyes: (1) the maximum capacity was 416.7 mg g–1 for MO and 58.7 mg g–1 for MB at 25°C; (2) the increase in temperature could enhance MO removal significantly, whereas it had a negligible effect on the MB treatment process; and (3) rapid removal of MB (5 min) compared to MO (480 min) was observed. In addition, the removal process for both dyes was pH-independent. Multiple characterization techniques further revealed the removal mechanisms, demonstrating that SDS played a significant role in the removal of both dyes; that is, MO replaced SDS to be intercalated into the HLDH interlayer via anion exchange. MB could influence the –SO3 group of SDS, resulting in it modifying the electrodensity of SDS. It could then be further combined with an SDS anion (DS–) via hydrophobic and electrostatic interactions to form DS-MB monolayers. This work not only provides an efficient capture agent for charged dyes, but also offers a deep insight into the underlying removal mechanism.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Yao Li,Le Xin Song,Wei Ping Wang,Yue Teng,Juan Xia,Nan Ning Liu
In this work, we prepared a series of Fe-MOF polyhedra [metal organic framework (MOF)-1 ∼ −13] by introducing β-cyclodextrin (CD) as a morphology modifier using an interaction between ferric chloride and terephthalic acid in dimethylformamide. A novel structural evolution from a hexagonal bipyramid to a bipyramidal hexagonal prism was clearly observed. This evolution was gradual and could be well reflected by the height ratio of the prism and pyramid in these polyhedral structures. It is the relative concentration of β-CD that drives this structural evolution. Although the reaction temperature and time can also affect the height ratio to some extent, their influence can only be realized in the presence of β-CD. In the absence of β-CD, only hexagonal bipyramid structures were obtained. It is worth noting that Fe-MOF-1 with a bipyramidal hexagonal prism structure (prism height, ∼130 nm) showed typical paramagnetic characteristics, and its saturation magnetization was determined to be 23.1 emu·g–1. Furthermore, we found that Fe-MOF-1 exhibited good photocatalytic performance for different types of dyes (crystal violet with positives and methyl orange with negative charges). At the same time, a possible photocatalytic mechanism was proposed to explain the difference of degradation efficiency between the two dyes. Also, we use the combination of specific surface area and zeta potential to explain the differences in the catalytic properties of a series of Fe-MOF materials. In addition, MOF-1 shows the same electrocatalytic oxygen evolution reaction performance as some bimetallic MOFs such as Fe-Co-MOF. For example, the overpotential of MOF-1 is 398 mV at 10 mA·cm–2 current density, while that of Fe-Co-MOF is 410 mV. We believe that the current work can contribute to the adjustment, modification, and application of MOF nanostructures.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Zhihui Li,Aiping Wu,Ying Xie,Ying Gu,Haijing Yan,Dongxu Wang,Siyu Wang,Chengxu Jin,Lei Wang,Chungui Tian
The design of the electrocatalysts with the plentiful heterojuctional interface and large-accessible surface is desired to boost the HER performance, but it remains a challenge. Herein, we showed the design of 2D Ni/Ni 0.2 Mo 0.8 N porous heterojunction nanobelts as effective catalyst for the HER. The intimate combination of Ni and Ni 0.2 Mo 0.8 N can make the formation of the heterojuctional interface with plentiful active sites. The 2D porous structure can provide large accessible surface with less resistance for the transmission of the electrolytes, thus promoting the mass/charge transfer. The ratio of Ni and Ni 0.2 Mo 0.8 N can be easily tuned by regulating the precursor composition, which is important to give catalysts with optimized interface and suitable pores. Density functional theory calculations reveal that the interaction between Ni and Ni 0.2 Mo 0.8 N at the heterointerface can largely improve the intermediate H* adsorption kinetics (ΔG H* = -0.07 eV). Due to the above advantages, the optimized catalysts exhibited excellent HER activity with a low overpotential of 48 mV in 1 M KOH at 10 mA cm −2 (without iR correction), which is superior to the most reported non-noble metal-based catalysts, and the long-term durability with no obvious degradation after continual operation of 48 h Notably, an electrolyzer assembled by the optimized Ni/Ni 0.2 Mo 0.8 N cathode with NiFe-LDH anode only requires a low operating voltage of 1.47 V to deliver 10 mA cm −2 in 1 M KOH, surpassing the corresponding Pt/NF||RuO 2 /NF electrolyzer (1.61 V) and most of reported electrolyzers.
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Advanced Science
·
2021
·Vol. 9
·期 1
·2101527
·
IF 16.806
Min Qian,Ziqiang Cheng,Guanghong Luo,Massimiliano Galluzzi,Yuehong Shen,Zhibin Li,Hongyu Yang,Xue-Feng Yu
Chemodynamic therapy (CDT) is an emerging treatment that usually employs chemical agents to decompose hydrogen peroxide (H 2 O 2 ) into hydroxyl radical (•OH) via Fenton or Fenton-like reactions, inducing cell apoptosis or necrosis by damaging biomacromolecules such as, lipids, proteins, and DNA. Generally, CDT shows high tumor-specificity and minimal-invasiveness in patients, thus it has attracted extensive research interests. However, the catalytic reaction efficiency of CDT is largely limited by the relatively high pH at the tumor sites. Herein, a 808 nm laser-potentiated peroxidase catalytic/mild-photothermal therapy of molybdenum diphosphide nanorods (MoP 2 NRs) is developed to improve CDT performance, and simultaneously achieve effective tumor eradication and anti-infection. In this system, MoP 2 NRs exhibit a favorable cytocompatibility due to their inherent excellent elemental biocompatibility. Upon irradiation with an 808 nm laser, MoP 2 NRs act as photosensitizers to efficiently capture the photo-excited band electrons and valance band holes, exhibiting enhanced peroxidase-like catalytic activity to sustainedly decompose tumor endogenous H 2 O 2 to •OH, which subsequently destroy the cellular biomacromolecules both in tumor cells and bacteria. As demonstrated both in vitro and in vivo, this system exhibits a superior therapeutic efficiency with inappreciable toxicity. Hence, the work may provide a promising therapeutic technique for further clinical applications.
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PubMed
高影响因子
Crystals
·
2023
·Vol. 14
·期 1
·14
·
IF 2.7
Yufei Zu,Zi Wang,Hongliang Tian,Fan Wu,Lianshen Fu,Jixiang Dai,Jianjun Sha
High-entropy diboride-based (MeB2-based) ceramics are promising high-temperature structural materials because of their excellent mechanical properties, high-temperature stability, and oxidation resistance. In order to achieve low-temperature sintering of the high-entropy ceramics, a novel preparation method of high-entropy (Ti,Zr,Nb,Mo,W)B2-SiC ceramics based on reactive sintering of pre-alloyed solid-solution metals and nonmetals of Si, C, B4C was conducted in the current work. Mechanical alloying behavior of the mixed metal powders, as well as the phase composition, microstructure, mechanical properties, and oxidation behavior of the as-sintered MeB2-SiC ceramic were investigated. The XRD, SEM, and EPMA results indicated that the primary MeB2solid-solution and SiC phases could be successfully formed during reactive sintering at a relatively low temperature of 1650 °C. The as-sintered MeB2-SiC ceramics had a high relative density of 97.8% and high mechanical properties (hardness of 19.74 ± 0.8 GPa, flexure strength of 533 ± 38 MPa, and fracture toughness of 6.01 ± 0.77 MPa·m1/2). Combining the oxidation behavior and microstructure evolution of the oxidation layer, a continuous and relatively dense MeOx-SiO2oxidation layer was gradually formed and covered on the external surface, leading to decelerating oxidation behavior after an oxidation exposure time of 10 min.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Henan Zhang,Qi Liu,Alena Novoselova,Valeri Smolenski,Jing Yu,Jingyuan Liu,Yongde Yan,Milin Zhang,Jun Wang
The efficient separation of the rare earth element Sm from spent nuclear fuel is of strategic importance for the nuclear industries. This study explored the feasibility of a novel liquid Ga-Pb hybrid electrode for electrochemical extraction of samarium compounds, and the electrochemical reduction mechanism and dynamic properties of Sm(III) ions were provided in NaCl-2CsCl molten salt. It was established that the reduction mechanisms of Sm(III) to Sm(II) and Pb(II) to Pb(0) on the Mo cathode were a one-step reaction processes, respectively, while Ga(III) to Ga(0) was a two-step reaction process. The co-deposition mechanisms of Sm(III), Ga(III) and Pb(II) ions on the Mo cathode were identified, and the types of intermetallic compounds, formation potentials and reaction processes were analyzed. The deposition potential of Sm on Ga-Pb mixed cathode is determined, and the value of its depolarization was greater than on the liquid Pb electrode. Simultaneously, Sm ions have higher exchange current densities and lower activation energies for electrode reactions on the liquid Ga-Pb mixed electrodes than on the liquid Pb electrodes. Furthermore, the electro-separation of NaCl-2CsCl-SmCl 3 molten salt was executed via potentiostatic electrolysis technique, and the separation efficiency and the effect of cathode product type were analyzed and compared in Ga-Pb hybrid electrode and Pb electrode. It was obtained that the maximum extraction efficiency on the Ga-Pb hybrid electrode and the separation efficiency of Sm could reach 91.3 % after 8 h of electrolysis.
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高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Caifeng Wei,Yanqin Cai,Zujin Yang
The presence of heavy metal ions and organic dyes in aqueous solutions has a significant impact on the ecological environment and human health. Herein, a novel bifunctional imidazolium-based porous organic polymer (IMSPF-Br-C=C) was prepared successfully via quaternization reaction of spirobifluorene and 1,4-dibromo-2-butene. The synthesized material was characterized by scanning electron microscopy (SEM) with energy dispersive spectroscopy (EDS), Fourier transform infra-red spectra (FTIR), Thermogravimetric analysis (TGA), X-ray diffraction (XRD), N 2 adsorption-desorption analysis and solid-state 13 C CP/MAS NMR spectroscopy, confirming its structure and stability. Owing to the conjugated structure of spirobifluorene, IMSPF-Br-C=C showed excellent recognition performance for dichromate anion (Cr 2 O 7 2− ) with the limit of detection (LOD) of 1.58 μmol/L. In addition, IMSPF-Br-C=C with the abundant imidazolium cations showed the outstanding adsorption performance in the removal of Cr 2 O 7 2− and methyl orange (MO). Removal efficiencies and adsorption capacities of IMSPF-Br-C=C were 98.3 % and 99.4 %, 452.8 and 1304.2 mg/g in 6 min, respectively. The results show that the electrostatic interactions and π-π stacking play crucial roles in the fluorescence detection of Cr 2 O 7 2− and adsorptive separation of Cr 2 O 7 2− and MO. Furthermore, physico-chemical techniques, density functional theory (DFT) calculation and frontier molecular orbital theory (FMO) were used to explain action mechanism. This work provides a cost-effective IMSPF-Br-C=C as a bifunctional platform for sensing Cr 2 O 7 2− and adsorptive separation of Cr 2 O 7 2− and MO in aqueous solution.
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高影响因子
Advanced Sustainable Systems
·
2023
·
IF 7.1
Zhiyong Li,Guangshen Chen,Pengfei Cheng,Zhang Zhang,Junming Liu
Positive phototropism enables plants to take advantage of sunlight more efficiently. However, positive phototropism of plant-like photocatalyst has not been reported yet, which cause people's limited understanding on it. Therefore, developing new photocatalysts that can move toward the light source and thus speed up the photocatalytic process, is a great challenge. Herein, a biologically active photocatalyst (graphitic carbon nitride combined with algae microorganisms, g-C 3 N 4 /alga) is reported first that can behave like green plants and move toward light source, leading to a great enhancement in photocatalysis. The photocatalytic degradation efficiency of the phototactic g-C 3 N 4 /alga is improved up to 570% than that of pure g-C 3 N 4 . The phototactic g-C 3 N 4 /alga photocatalyst can effectively utilize the synergy of phototaxis of microalgae and photocatalytic activity of g-C 3 N 4 to promote the pollutant decomposition using sunlight. Imparting photocatalyst with positive phototropism will open a new door in photocatalysis field for clean energy production, pollutant treatment, and biomass conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lufang Fan,Sheng Feng,Kai Wei,Xiaojun Dai,Weijie Zhang,Haihong Wang,Zhaowei Bian,Kaidi Wu,Zhiwen Ge,Jinghao Hua
In this study, we designed and fabricated a Z-scheme Cu 0.5 Cd 0.5 S/MoO 3-x (CMO) heterojunction with localized surface plasmon resonance (LSPR) effect for efficient photocatalytic hydrogen evolution. The oxygen vacancies (OVs) in MoO 3-x induced Schottky-barrier-free LSPR for the generation of hot electrons. The architecture of transition-metal-substituted solid solution (Cu 0.5 Cd 0.5 S, CCS) downshifted the conduction band (CB) of CdS from −0.45 eV to −0.38 eV and upshifted the valence band (VB) from 1.65 eV to 1.54 eV, respectively, weakening the interface barrier of the hot electrons transition from MoO 3-x to CCS and enhancing the Coulomb interaction between the electrons of MoO 3-x and the holes of CCS. Benefiting from the cooperation between Z-scheme heterojunction and LSPR effect, the hydrogen evolution rate (HER) of the optimized CMO was 19.28 mmol·g −1 ·h −1 under visible light with an apparent quantum yield (AQY) of 10.8 % at 420 nm, which was 3.0 and 1.4 times that of the CCS and CCS/MoO 3 . Moreover, the HER of CMO still reached 43.57 μmol·g −1 ·h −1 at 600 nm. This work paved a new path for efficient photocatalysts H 2 evolution by coupling Z-scheme heterojunction and non-noble-metal LSPR effect.
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Journal of Materials Chemistry A
·
2023
·
IF 11.9
Liang Li,Xian-ying Shi,Ting Huang,Nan Zhang,Yong Wang
MXene has great potential to remove contaminants from wastewater due to its abundant active functional groups. However, the application is greatly restricted by the instability of MXene, which is derived from its high oxidization property. In this study, a few-layer MXene was prepared via chemical etching, and then polyethylenimine (PEI) was grafted onto the MXene surface with the aid of glutaraldehyde-assisted crosslinking. The microstructure, storage stability, and adsorption behaviors toward water-soluble pollutants were systematically investigated. The results revealed that grafting PEI could promote MXene exfoliation and enhance adsorption ability. The modified MXene exhibited ultrahigh adsorption capacity toward methyl orange (MO) (909.1 mg g−1) and hexavalent chromium Cr(VI) (1239.5 mg g−1). Furthermore, the storage stability of MXene was greatly improved and almost no oxidization was detected for the modified MXene even after being stored for two months. This study offers a simple method to fabricate MXene-based adsorbents with excellent adsorption capacity and good antioxidant ability, and the application of MXene in wastewater treatment can be advanced.
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高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Huijie Wang,Qi Liu,Mengyang Xu,Chenlong Yan,Xianghai Song,Xin Liu,Huiqin Wang,Weiqiang Zhou,Pengwei Huo
The localized surface plasmon resonance (LSPR) effect has shown significant progress in enhancing the efficiency of light absorption and separating photogenerated carriers. Herein, the dual-plasma enhanced 2D/2D/2D g-C 3 N 4 /Pd/MoO 3-x (CPM) S-scheme heterojunction photocatalysts were synthesized using the method of hydrothermal and electrostatic self-assembly for high-selectivity photocatalytic reduction of CO 2 to produce CO. The dual LSPR effect of MoO 3-x and ultrathin Pd nanosheets synergistically broadened the optical response range of the CPM composites and successfully improved the photocatalytic activity and near-infrared (NIR) performance. The optimized CPM-30 photocatalysts exhibited CO yields of 18.55 μmol g −1 with a selectivity of 96.3%. In addition, the CO yield reached 3.92 μmol g −1 after 4 h of NIR light photoirradiation. The electron spin resonance (ESR) and ultraviolet photoelectron spectroscopy (UPS) tests showed that the S-scheme heterojunctions were constructed by coupling g-C 3 N 4 /Pd nanosheets and MoO 3-x . This work will provide a reference for improving product selectivity through the design of two-dimensional composites and the utilization of plasma materials.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Junli Zheng,Linlin Du,Peng Gao,Kaiwei Chen,LiLi Ma,Yuanli Liu,Shaohong You
The excessive discharge of dye wastewater is a great threat to human health and environment with the development of industry. And it is of great significance to use biomass materials to remove dyes from wastewater with the low cost, renewability and environmental friendliness. In this study, the amine-modified passion fruit peel (ACPFP) was prepared by amination reaction, which exhibited highly efficient removal for anionic dyes (methyl orange (MO) and amaranth (ART)). The adsorption capacities of ACPFP for MO and ART were 1530.81 and 970.87 mg⋅g −1 , respectively. And the adsorption conditions (pH, ionic strength, temperature, initial dye concentration, and contact time) and mechanism (kinetic and isotherm models) were investigated. The results revealed that 99% of MO and ART was removed in the best adsorption conditions: pH=5, an adsorbent dose of 1 g⋅L −1 , 600 mg⋅L −1 of MO and ART initial concentration. The adsorption process correlated well with the pseudo-second-order kinetic model and the Langmuir isotherm. And ACPFP had good adsorption selectivity, stability and recyclability for anionic dyes. In conclusion, ACPFP has broad application prospects in actual water treatment.
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