SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yufeng Da,Yong Liu,Yong Chen,Rui Han,Jianlong Wang
Recently, the activation of molecular oxygen (O 2 ) by graphite (Gr) supported aluminum (Al) composite for the in-situ generation of H 2 O 2 / OH gains increasing attention. However, the limited O 2 mass transfer and low catalytic activity of decomposition H 2 O 2 at neutral pH restrict its further application in the wastewater treatment. In this work, a novel N-rich graphite supported aluminum (Al-Gr-NPC) composite was fabricated by introducing the nitrogen-rich porous carbon (NPC) obtained from ZIF-8 derivative as precursor, and by a ball-milling and sintering process. The results showed that the NPC introduction not only improved the physiochemical property of Al-Gr, such as specific surface area, pore structure and hydrophobicity, facilitating the mass transfer of O 2 , but also made Al-Gr contain plentiful N species, serving as active sites for the two-electron ORR process and catalytic decomposition of H 2 O 2 . These excellent performances of Al-Gr-NPC favored the production and utilization of H 2 O 2 by the activation of O 2 at neutral pH and air aeration. The carbonization temperature of ZIF-8 determined the type of N species, surface area and the hydrophobicity of NPC. 1 O 2 was the main oxidant for tetracycline hydrochloride (TC) degradation. 100 % TC degradation and 60.57 % of TOC removal were achieved within 60 min at neutral pH, Al-Gr-NPC dosage of 0.5 g/L and initial TC concentration of 20 mg/L. The toxicity of the final products of TC degradation were much lower than TC by ECOSAR software analysis. Al-Gr-NPC could be used for the removal of antibiotic contaminants from wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jinxiang Zuo,Donglei Fu,Pengwei Yan,Shuyu Wang,Yabin Li,Linlu Shen,Yizhen Cheng,Jimin Shen,Jing Kang,Zhonglin Chen
In this study, Al-doped NiFe 2 O 4 (NiAl x Fe 2-x O 4 ) was synthesized by the isomorphic substitution strategy, which was further employed for peroxymonosulfate (PMS) activation to remove 2,4-dichlorophenoxyacetic acid (2,4-D) in water. Doping of Al could construct oxygen vacancies (OVs) in the structure of NiAl x Fe 2-x O 4 , which further facilitates the exposure of metal sites for PMS activation. The removal rate of 2,4-D increased greatly compared to the NiFe 2 O 4 -activated process. By the density functional theory (DFT) process, it was verified that Al was more likely to replace Fe rather than Ni. OVs sites have the lowest adsorption energy of H 2 O ( E ads = -0.95 eV), and easily formed surface hydroxyl groups (–OH), which were further replaced by PMS (HSO 5 - ). The formed surface complex Me-O-O-SO 3 - was readily activated via electron transfer between O-O bond, thus promoting the cleavage of it and inducing SO 4 · - generation. This process induced the high performance of the NiAl x Fe 2-x O 4 /PMS system for effective 2,4-D degradation. Furthermore, the purified water showed relatively low toxicity. The present study proposed new insights into the interface mechanism of PMS triggering.
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ACS Omega
·
2023
·
IF 4.1
Jing Wang,Yong Zhang,Fubin Liu,Ying Liu,Litao Wang,Guihua Gao
A multifunctional cylindrical hybrid foam column, referred to as the chitosan/cyclodextrin/MIL-68(Al) (CS/CD/MIL-68(Al)) foam column, was prepared for the first time. The prepared foam column could be used for the adsorption/removal of hydrophilic and hydrophobic contaminants by different forms. Here, it was placed in hydrophilic dye solutions to investigate the adsorption behavior of methylene blue and trypan blue. The adsorption process followed the pseudo-second-order kinetic model with R2 ranging from 0.9983 to 0.9998 for methylene blue and from 0.9993 to 1.0000 for trypan blue, and the adsorption process was consistent with the Langmuir isothermal model with R2 greater than 0.96. The RL values for methylene blue and trypan blue were 0.8871 and 0.5366, respectively, which were present between 0 and 1, indicating that the adsorption behaviors of the two dyes onto the CS/CD/MIL-68(Al) foam column were favorable. The maximum adsorption capacities (Qm) of methylene blue and trypan blue were 60.61 and 454.55 mg/g at 298 K, respectively. Also, the CS/CD/MIL-68(Al) foam column was spun into a syringe and used to adsorb trace hydrophobic sulfonamides from water in the form of filtration. The porous structure impeded the need for any external force and equipment, allowing the water sample to pass through the foam column smoothly. The conditions of the CS/CD/MIL-68(Al) foam column were optimized. The adsorption was carried out under the condition of pH = 4, the amount of the adsorbent was two foam columns, and no salt was added. It was found that the removal rate of the CS/CD/MIL-68(Al) foam column for six sulfonamides was 100%, and it could be reused at least five times. Therefore, this CS/CD/MIL-68(Al) foam column had a simple preparation method, offered a flexible and diverse form of use, was nonpolluting, biodegradable, and reusable, and could have a wider application in the field of environmental pollutant removal and adsorption.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Weiquan Yuan,Jingzhong Kuang,Haixiang Hu,Dan Ding,Mingming Yu
The removal of impurity Al(III) from rare earth ion solution by selective adsorption method was one of the challenging tasks. Herein, calcination and acid dissolution treatment were used to construct the pore structure for the halloysite substrate (Hal-650-H) and provide conditions for the formation of the chitosan mesoporous membrane to prepare composite (Hal-H-2CS). The selective adsorption properties and mechanism of the Hal-H-2CS for Al(III) in the rare earth ion solution were studied. The results showed that the formation of mesoporous structures for chitosan provided abundant sites for the adsorption of Al(III). Hal-H-2CS showed remarkable selective adsorption properties for Al(III) in a wide pH range and the binary mixtures with high content of Al(III) or La(III). The maximum adsorption capacity of Al(III) was 106 mg/g, while the adsorption capacity of La(III) was only 1.41 mg/g at pH 4.0. In addition, the Hal-H-2CS exhibited excellent regeneration and structural stability. The remarkable selective properties of Hal-H-2CS was achieved by the synergistic effect between chitosan mesoporous membrane and Hal-650-H, the main adsorption sites were the OH, NH 2 , CONH 2 of chitosan and the oxygen sites of the Hal-650-H. This work provides a new strategy for the design and preparation of outstanding selective adsorbent for Al(III).
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 36
·14299-14314
·
IF 4.5
Xu Chenzhe,Qiu Yue,Wang Zheng,Gao Zifei,Liu Cai,Sun Yanran,Zhang Haitao,Ma Juanjuan,Liu Lin,Liu Chao,Tong Zhiwei
A facile one-step hydrothermal approach was proposed to fabricate Pd nanoparticles decorated Mg–Al layered double hydroxide nanosheets (denoted as Pd NPs/Mg–Al LDH composite), wherein polyvinylpyrrolidone (PVP) functioned as both a reductant and stabilizer. The resulting samples were characterized by XRD, SEM, TEM, XPS and BET techniques. The effect of synthetic parameters during the hydrothermal reaction including PVP dosage and temperature on the size and distribution of Pd NPs was investigated in details. Pd nanoparticles with an average particle size of 3.6 nm were uniformly supported onto Mg–Al LDH nanosheets under the optimal conditions. The obtained Pd NPs/Mg–Al LDH composite could serve as an efficient heterogeneous catalyst for the Heck reaction between iodobenzene and methyl acrylate, achieving a high yield of 95.8% within 60 min at 100 °C. Furthermore, Pd NPs/Mg–Al LDH was highly stable and reused 6 times without significant loss of its catalytic activity.
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Molecular Catalysis
·
2020
·
IF 3.687
Yi Yu,Fanfan Li,Zhouxuan Zang,Li Xu,Guoji Liu
Catalytic oxidation of 2-methylnaphthalene to 2-methyl-1,4-naphthoquinone (vitamin K 3 ) is a significant pathway to produce vitamin groups K. High pollution and low-productivity of the traditional method require a greener catalyst and process. In this work, Al/Ti-SBA-15 with different n Si /n Al and n Si /n Ti ratios were hydrothermally prepared in mild acidic condition and tested in partial oxidation of 2-methylnaphthalene. Commercial zeolites NaY, β and ZSM-5 were applied to investigate the influence of mass transfer resistance and acidity on catalytic performance. Catalysts were characterized by XRD, N 2 adsorption-desorption, TEM, NH 3 -TPD, FTIR and Py -FTIR. We have found that the 2-methylnaphthalene conversion and vitamin K 3 selectivity depend strongly on the mesoporous structure as well as Brönsted acid concentration and strength. Irregular micropores and strong acidity will accelerate the cleavage of C = C in aromatic rings, leading to the production of phthalic anhydride. DFT calculation reveals that incorporation of aluminum in SBA-15 can reduce the energy gap, facilitating the electron transfer. And as a consequence of the substitution of Al in tetrahedral positions in SBA-15, Al-SBA-15 (10) gives the best result with 72% yield to vitamin K 3 . This catalyst markedly reduces the activation energy due to the modified activated center. Repeated experiments recommend that Al-SBA-15 is a steady and high-efficiency catalyst for the production of vitamin K 3 .
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Nanoscale
·
2020
·Vol. 12
·期 26
·14180-14187
·
IF 6.895
Luyan Wu,Jie Hu,Qilin Zou,Yaling Lin,Decai Huang,Dejian Chen,Hongyu Lu,Haomiao Zhu
Persistent luminescence nanophosphors (PLNPs) emitting in the second near-infrared window (1000–1700 nm, NIR-II) are emerging as one promising class of in vivo bio-imaging agents due to their unique advantages including non-autofluorescence and low optical scattering in tissues. Currently, it remains a great challenge to synthesize nanosized lanthanide-doped inorganic NIR-II phosphors with a good persistent luminescence performance. Herein, we present a salt microemulsion method for synthesizing Ce3+, Cr3+, Nd3+ codoped Y3(Al/Ga)5O12 nanocrystals, which generate multi-wavelength persistent luminescence in the visible (∼508 nm, 5d1 → 4f of Ce3+), the first near-infrared window (∼890 nm, 4F3/2 → 4I9/2 of Nd3+) and NIR-II (∼1063 nm, 4F3/2 → 4I11/2 of Nd3+) regions. Under illumination of a 410 nm diode (3 W) for 10 min, the observed duration time of NIR-II persistent luminescence is as long as 60 min at room temperature. Moreover, the persistent luminescence can be excited efficiently by multiple excitation sources including a blue diode, white LEDs and an X-ray generator, which is crucial for deep tissue imaging applications. By comparing the penetration depth between NIR-I and NIR-II persistent luminescence through chicken breast, we prove that NIR-II photons exhibit a deeper optical penetration length (3.9 mm) than that of the NIR-I ones (2.5 mm). In addition, the NIR signals can still be detected 3 min after ceasing the excitation source by a small animal imaging system (InGaAs detector) when the thickness of the covering chicken breast is 20 mm. These results show great promise for Y3(Al/Ga)5O12:Ce3+,Cr3+,Nd3+ nanocrystals as a PLNP for bio-imaging applications with deep penetration depth and a high signal-to-noise ratio.
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 48
·17741-17751
·
IF 4.052
Jin Li,Ying Song,Yajuan Wang,Hui Zhang
A series of PdCo alloy nanocluster (NC) catalysts x-PdCor/Co(Mg or Ni)Al-LDH (x: Pd loading, r: Co/Pd molar ratio) were synthesized by immobilizing ultrafine PdCor-PVP NCs on flower-like layered double hydroxide (LDH) supports. The sizes of PdCo alloy NCs of the catalysts can be elaborately tuned in ∼1.6–3.2 nm by both Co/Pd ratios and Pd loadings, and the PdCo NCs are mainly dispersed on the edge sites of LDH nanosheets upon a flower-like morphology. The PdCo bimetallic catalysts 0.81-PdCo0.10/MgAl-LDH (2.6 ± 0.6 nm), 0.86-PdCo0.28/MgAl-LDH (2.3 ± 0.7 nm) and 0.79-PdCo0.54/MgAl-LDH (3.2 ± 0.9 nm) exhibit enhanced activity compared with the monometallic Pd catalyst for Heck coupling of iodobenzene with styrene. Particularly, 0.86-PdCo0.28/MgAl-LDH shows the highest activity, which can be attributed to its smallest PdCo0.28 alloy NCs, and the maximum electron density of the Pd0 center resulted from the electron transfer from Co and the strongest PdCo0.28 NCs – LDH synergistic effect. 0.67-PdCo0.28/CoAl-LDH shows much better activity than those of 0.64-PdCo0.28/NiAl-LDH and 0.86-PdCo0.28/MgAl-LDH. The lowest Pd loading sample 0.01-PdCo0.28/CoAl-LDH (1.6 ± 0.4 nm) shows an ultrahigh turnover frequency of 163 000 h−1 (Pd: 1.9 × 10−5 mol%), which is the highest value obtained so far. Meanwhile, the catalyst shows excellent adaptability for the substrates and can be reused for 12 runs without significant loss of activity. The present work may provide a new idea for the simple and green synthesis of ultrafine Pd-based non-noble bimetallic catalysts for varied catalytic processes.
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International Journal of Minerals Metallurgy and Materials
·
2016
·Vol. 23
·期 11
·1346-1351
·
IF 0.882
Jiang Peng,Yang Wen-hui,Zhou Yun-cheng,Kuang Jian-lei,Li Yong,Xiao Ting
Brownmillerite-type oxides Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
(0 ≤ x ≤ 0.6, 0 ≤ y ≤ 0.5) were prepared at 1300°C through solid-state reaction. X-ray diffraction (XRD) analysis showed that the structure symmetry evolved from orthorhombic to cubic with increasing Mn and Al contents. When y was greater than 0.3, peaks associated with small amounts of BaAl 2 O 4 and Ba 2 InAlO 5 impurities were observed in the XRD patterns. When substituted with a small amount of Mn ( x ≤ 0.3), the Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
samples exhibited an intense turquoise color. The color changed to green and dark-green with increasing Mn concentration. UV–vis absorbance spectra revealed that the color changed only slightly upon Al doping. The valence state of Mn ions in Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
was confirmed to be +5 on the basis of X-ray photoelectron spectroscopic analysis. According to this analysis, the intense turquoise color of the Ba 2 In 2− x − y
Mn
x
Al
y
O 5+ x
samples is rooted in the existence of Mn 5+ ; thus, the introduction of Al does not affect the optical properties of the compounds.
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COMBUSTION AND FLAME
·
2024
·
IF 5.8
Ruixuan Xu,Zhihua Xue,Haorui Zhang,Hongqi Nie,Qi-Long Yan
The control of burning rate pressure sensitivity is essential for stable and reliable combustion of solid propellants. It has been proved that the combustion behavior of propellants can be effectively tuned by interfacial control of Al/oxidizers. In this work, core-shell Al-based composites, using oxidizers such as ammonium perchlorate (AP) and cyclotetramethylene tetranitramine (HMX) as the shell layer, have been prepared with a well-controlled location of graphene-based carbohydrazide complexes (GO-CHZ-M, M = Co 2+ or Ni 2+ ) as the catalysts. The catalysts can be located inside HMX or embedded on the surface of AP particles. The decomposition of AP and HMX could be greatly promoted with a trace amount of catalyst. Under the synergistic effects of Al/oxidizer interfacial control and GO-CHZ-M, the ignition delay time is shortened by >48 % with increased in flame radiation. More importantly, the burning rate ( r ) and pressure exponent ( n ) of the solid propellants are effectively regulated in a wide range. In particular, the use of Al@HMX/Co results in a lowered n of 0.29 within 1∼20 MPa compared to 0.79 for the blank reference sample. The agglomeration of Al particles during combustion was also inhibited due to the micro-explosion effect of Al@HMX composites. Novelty and Significance statement The innovative approaches of integrating Al/HMX/AP composites and precise catalysis of graphene-based energetic catalysts in solid propellants have successfully achieved, regarding the modulation of the burning rates and pressure sensitivity. Moreover, the effect of catalyst location on the ignition delay and burning rates has also been studied thoroughly and clarified. This paper provides new insight into the regulation of combustion performance of solid propellants, with improved reaction efficiency and maintained energy density.
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Journal of Building Engineering
·
2024
·
IF 6.7
Wenjie Liu,Biqin Dong,Peiyu Chen,Lei Zeng,Ming Peng,Xiang Wang,Yanshuai Wang,Shuxian Hong
In situ growth of different anion-intercalated layered double hydroxide (LDH) films on steel substrates for corrosion resistance has been achieved via the electrodeposition-hydrothermal method, but its growth process remains unclear. In this study, the effects of electrodeposition potential (−1.1 to −1.4 V) on the formation and growth mechanism of Zn/Al-NO 3 − -LDH films were investigated using XRD, FTIR, and SEM techniques. The results demonstrated that weak potentials either failed to form the LDH film or caused cracks, while excessive potentials resulted in hydrogen evolution and the formation of heterogeneous ZnO. The LDH films prepared at the optimal potential of −1.3 V were dense and uniform, with an adhesion grade of 4B, exhibiting a corrosion inhibition efficiency of 80.6 % in a 3.5 wt% NaCl solution.
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LUMINESCENCE
·
2024
·Vol. 39
·期 11
·1-8
·
IF 3.2
Zhigang Wang,Jiayu Wang,Dangli Gao,Wenqian Xu,Wenna Gao,Xiangyu Zhang,Sining Yun,Xiaojun Wang
Double wavelength emitting phosphors with hypersensitive thermal response are important for optical/thermal sensors and multiplexing optical data storage technology. However, it is a daunting challenge to develop multicolor electron-trapping materials with superheat sensitivity and anomalous quenching luminescence characteristics for information storage. Here, based on the selection of host lattice and the control of doping ion types, we have designed Mn 2+ - and/or Cr 3+ -activated persistent materials with excellent fluorescence properties. Among these phosphors, Mn,Cr co-activated biphasic mixture exhibits not only sensitive anomalous thermosensitive fluorescence properties but also multicolor and multimode fluorescence emission characteristics derived from Mn and Cr simultaneously. The corresponding multimode fluorescence mechanism is proposed based on afterglow energy transfer and deepening trap effect. Especially, based on the excellent fluorescence performances, these phosphors as information storage medium demonstrate multilevel information storage by a combination of the trap multiplexing and wavelength multiplexing technologies. The study here provides not only the ideas for designing and synthesizing new electronic materials but also a material foundation for the fourth generation of optical information storage and encryption.
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