MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yanghuan Huang,Haocheng Zhang,Lou Gao,Tianlan Yan,Yueer Yan,Yahong Zhang,Yi Tang
A series of Zr–Al-MWW zeolites with different Zr state and layer-stacking structure are successfully synthesized via direct grafting zirconocene dichloride onto the external silanols of three kinds of MWW zeolites, i.e. MCM-22 with multilayered structure, ITQ-2 (through layer delaminated route) and OL-MWW (by direct hydrothermal synthesis) with oligolayered structure. The structure, porosity and state of grafted Zr species are distinctly different among the three Zr–Al-MWW zeolites. Zr-OL-MWW possesses the highest content of single Zr atoms with an ideal micro-meso-macro pore system, while Zr-MCM-22 and Zr-ITQ-2 contain two kinds of Zr species (ZrO 2 clusters and single Zr atoms) coexisting in various proportions. The high dispersion of single Zr atoms on OL-MWW can be assigned to the large amount of external silanols of OL-MWW. The as-prepared three bi-functional Zr–Al-MWW zeolites are used for the cascade Meerwein-Ponndorf-Verley (MPV) reduction and etherification (ETH) reaction. Among them, Zr-OL-MWW shows dramatically higher conversion of cinnamaldehyde and yield of 1-cinnamyl 2-propyl ether than Zr-MCM-22 and Zr-ITQ-2, owing to the higher catalytic activity of Lewis acid centers from single Zr atoms, as well as more integrated framework Al sites as Brønsted acid centers with good accessibility. This study offers a simple and efficient strategy to construct Lewis-Brønsted acidic zeolites with exposed heteroatom sites and integrated framework structure, which will provide especial potential in the catalytic conversion of macromolecules.
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Nanomaterials
·
2021
·Vol. 11
·期 9
·2332
·
IF 5.076
Qiangqiang Feng,Yanyan Liu,Jitong Yan,Wei Feng,Shaozheng Ji,Yongfu Tang
A promising aqueous aluminum ion battery (AIB) was assembled using a novel layered K2Ti8O17anode against an activated carbon coated on a Ti mesh cathode in an AlCl3-based aqueous electrolyte. The intercalation/deintercalation mechanism endowed the layered K2Ti8O17as a promising anode for rechargeable aqueous AIBs. NaAc was introduced into the AlCl3aqueous electrolyte to enhance the cycling stability of the assembled aqueous AIB. The as-designed AIB displayed a high discharge voltage near 1.6 V, and a discharge capacity of up to 189.6 mAh g−1. The assembled AIB lit up a commercial light-emitting diode (LED) lasting more than one hour. Inductively coupled plasma–optical emission spectroscopy (ICP-OES), high-resolution transmission electron microscopy (HRTEM), and X-ray absorption near-edge spectroscopy (XANES) were employed to investigate the intercalation/deintercalation mechanism of Na+/Al3+ions in the aqueous AIB. The results indicated that the layered structure facilitated the intercalation/deintercalation of Na+/Al3+ions, thus providing a high-rate performance of the K2Ti8O17anode. The diffusion-controlled electrochemical characteristics and the reduction of Ti4+species during the discharge process illustrated the intercalation/deintercalation mechanism of the K2Ti8O17anode. This study provides not only insight into the charge–discharge mechanism of the K2Ti8O17anode but also a novel strategy to design rechargeable aqueous AIBs.Keywords:aluminum ion battery;K2Ti8O17anode;discharge–charge mechanism
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 42
·15057-15061
·
IF 4.39
Ming-Yang Cao,Chun-Li Hu,Fang Kong,Zhe-Yao Xiong,Jiang-Gao Mao
Exploration of new types of borates is important because of their promising applications in diverse fields. Two new boroselenites, namely, M(B(SeO3)3)H2O (M = Al, Ga), which represent the first IIIA metal boroselenite, were synthesized by hydrothermal reactions. M(B(SeO3)3)H2O (M = Al, Ga) possesses a unique sandwich like double-layer structure formed by two 2D [MSe2O8]5− layers interconnected by 1D [BSeO5]3− chains. More interestingly, both compounds display large band gaps (4.86/4.79 eV) and moderate birefringences (Δn = 0.063/0.064 at 1064 nm) based on density functional theory (DFT) calculations.
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JOURNAL OF PHYSICAL CHEMISTRY B
·
2021
·
IF 2.991
Jinxia Wang,Xiangyue Liu,Hongwei Xie,Huayi Yin,Qiushi Song,Zhiqiang Ning
The magnetohydrodynamic (MHD) effect was usually used to improve the mass transport during electrodeposition in a solution electrolyte. Herein, we reported the effect of a magnetic field on the electrode process of Al electrodeposition in a [Emim]Cl-AlCl3 ionic liquid composed of pure ions. Under a uniform and perpendicular magnetic field to the Cu electrode plane, electrochemical impedance spectroscopy (EIS) of the circuit, the cyclic voltammetry (CV) curves, and the different capacitances at the potential of zero charge (PZC) were measured, and the electrodeposition of aluminum was carried out at a constant current density. The results indicated that a vertical magnetic field significantly reduced the resistance (activation energy) for charge transfer of electrochemical reduction of Al2Cl7–; meanwhile, the capacitance of an electric double layer (EDL) and the density of the electrodeposited aluminum layer were increased.
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Journal of Materials Research and Technology-JMR&T
·
2021
·
IF 5.039
Yuyu Liu,Zheng Chen,Xiaoqin Yang,Jinyong Zhang,Zhonggang Sun,Yuzeng Chen,Feng Liu
Different from the reported catalysts such as metallic glasses ribbons and ball-milled high entropy alloy powder, high entropy alloy nanoparticles (HEA NPs) have attracted wide attention for compelling and functional catalytic properties to degrade methylene blue (MB) dye. CoCrXFeNi (X = Al, Cu, Mn) HEA NPs with different loadings were synthesized by impregnation-adsorption method on activated carbon (AC). Nanoscale HEA NPs with maximized configuration mixing entropy are composed of a single solid-solution face-centered cubic (FCC) phase and the nanocomposites show distinctive porous architectures and large specific surface area (average S BET = 632.7 m 2 /g) for 10 wt.% loadings. The reaction rates ( k o b s ) of 10 wt.% CoCrAlFeNi and CoCrMnFeNi HEA NPs-AC for MB degradation are 0.1998 and 0.1830 min −1 and show comparable intrinsic catalytic performance to amorphous ribbons and HEA powders. The HEA NPs can effectively decompose MB molecule via nanoscale galvanic cell effect which provides a promising material in dye decomposition and mineralization.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Lijia Dong,Shengbo Li,Yefei Jin,Baowei Hu,Guodong Sheng
In this paper, CaAl hydrotalcite or hydroxyapatite decorated invasive plant ( Solidago canadensis )-derived biochar were synthesized by co-precipitation and high temperature pyrolysis method. The three composites and bare biochar were characterized by Scanning electron microscopy (SEM), X-ray spectroscopy (EDX), the Fourier transform infrared spectroscopy (FT-IR), X-ray diffractometer (XRD), and X-ray photoelectron spectroscopy (XPS) techniques, and employed to remove Eu(III) from wastewater under a series of environmental conditions. The results indicated that the Eu(III) adsorption on BC@LDH@HAP was higher than that on BC, BC@LDH, and BC@HAP, and belonged to multi-layer adsorption, which was different from the monolayer adsorption of biochar. The adsorption could be fitted best by Langmuir model and the maximum adsorption capacity of Eu(III) on BC@LDH@HAP was up to 714 mg/g at pH ~ 6. The characterization results suggested that this excellent adsorption of BC@LDH@HAP arose from the abundant P-, C-, O-containing functional groups rather than larger specific surface area. The spectra of XPS, FT-IR, and XRD uncovered that the adsorption mechanisms of Eu(III) on BC@LDH@HAP involved surface complexation, ion exchange, and precipitation. Moreover, the absorbed Eu(III) was formed into two precipitate induced by P-containing groups and carbonate groups. This research confirmed BC@LDH@HAP is a promising material for the removal of Eu(III) in wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Feng He,Jiahao Zhuang,Bin Lu,Xianglin Liu,Jianling Zhang,Fangna Gu,Minghui Zhu,Jing Xu,Ziyi Zhong,Guangwen Xu,Fabing Su
Developing Ni-based catalysts with high activity and stability in low-temperature methanation is necessary due to their sintering and coking at high temperatures. Here, we report our developed novel Ni-Zr-Al catalysts derived from Ni-Zr-Al ternary hydrotalcites synthesized by a hydrothermal process, followed by a reduction in hydrogen. Comparing with the Ni-Al catalyst derived from Ni-Al hydrotalcite and the commercial Ni-based catalyst, the Ni-Zr-Al catalysts show a remarkably higher low-temperature activity (210−270 °C) in CO 2 methanation. Both the experimental and theoretical calculations confirmed the introduction of Zr into the Ni-Al binary hydrotalcite could generate synergetic effects between Ni and ZrO 2 , resulting in more surface oxygen vacancies, basic sites, and abundant mesopores . In-situ DRIFTS analysis showed the CO 2 methanation to CH 4 follows the intermediate formate route. This work provides a new theoretical understanding of CO 2 activation and methanation, and a practical way to address the existing problem for Ni-based catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhi-Heng Lu,Ibrahim Abdelhai Senosy,Dong-Dong Zhou,Zhong-Hua Yang,Hao-Ming Guo,Xiao Liu
In this work, a novel Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite was synthesized by a facile three-step process and utilized as an adsorbent for the removal of azole fungicides from environmental water. The characterization results revealed that double hydroxide (ZnAl-LDH) and metal organic framework (MIL-53) have been successfully tethered to the shell of Fe 3 O 4 . The main factors affecting the removal efficiencies were investigated, and results revealed that Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite possessed high removal efficiencies for azole fungicides. Furthermore, the adsorption mechanism was investigated and including hydrogen-bonding interaction, chemisorption and π–π interaction. The adsorption kinetic was more consistent with the pseudo-second-order kinetic model, and the whole adsorption process could reach the equilibrium within 5 min. Langmuir adsorption isotherm model could describe the adsorption process most accurately, and the maximum adsorption values of azole fungicides were in the range of 43.54–71.79 mg g −1 . Meanwhile, the adsorption thermodynamics indicated that the adsorption process was exothermic and spontaneous. Hence, Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite had a great application potential in the removal of azole fungicides from the environment.
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Catalysts
·
2020
·Vol. 10
·期 11
·1329
·
IF 3.52
Shijie Hao,Yandi Cai,Chuanzhi Sun,Jingfang Sun,Changjin Tang,Lin Dong
Monolithic Mn-Fe-Ce-Al-O catalyst with honeycomb cordierite ceramic as a carrier was reported for the first time for low temperature deNOxapplication. In the reaction of selective catalytic reduction (SCR) of NO with NH3, a NO conversion of above 80% at 100 °C was obtained. Notably, the catalyst also showed excellent resistance against SO2and H2O. About 60% NO conversion was maintained after successive operation in the mixed stream of SO2and H2O for 168 h. The Brunner−Emmet−Teller (BET) measurement, SEM, EDS, thermogravimetric analysis (TG), FT-IR, and XPS results of the used catalysts indicated that certain amounts of ammonium sulfate was formed on the surface of the catalyst. XPS results revealed that partial of Fe2+was oxidized to Fe3+during the reaction process, and Fe2+species have strong redox ability, which can explain the decrease in activity after reaction. In addition, SO2and H2O induced a transformation of Ce from Ce4+to Ce3+on the surface of the catalyst, which increased the amount of chemisorbed oxygen. Owing to these factors, the addition of Ce and Fe species contributes to excellent resistance of the catalyst to SO2and H2O.Keywords:honeycomb catalyst;Mn-Fe-Ce-Al-O;low temperature denitration;water and sulfur resistance
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POLYMER TESTING
·
2020
·
IF 3.275
Tongyi Wu,Xuejun Lai,Hongqiang Li,Yishen Chen,Yanlin Wang,Tian Liu,Xingrong Zeng
It is of great significance and challenge to efficiently improve the tracking and erosion resistance of silicone rubber along with the growing requirements in the field of outdoor high voltage insulation. In this work, we herein proposed an effective way to address this issue by incorporating vinyltriethoxysilane (ViTES) and layered Mg–Al double hydroxide (LDH) into high temperature vulcanized silicone rubber (HTVSR). ViTES/LDH notably enhanced the tracking and erosion resistance of HTVSR. With addition of 3.33 phr ViTES and 5.00 phr LDH, the anti-tracking performance of HTVSR reached the 1A 4.5 level, and the eroded mass was merely 0.3%. The results of scanning electron microscopy and equilibrium swelling showed that ViTES substantially improved the interfacial interaction between HTVSR and LDH and the crosslinking density of HTVSR, and enhanced the dispersion of LDH sheets in the HTVSR matrix. The possible synergistic suppression mechanism of ViTES/LDH on the tracking and erosion of HTVSR was further studied and demonstrated by the plasma irradiation analysis, thermogravimetry and thermogravimetry-Fourier transform infrared spectrometry. It was indicated that under the high voltage arcing discharge, LDH facilitated the formation of a dense barrier layer consisting of bimetal mixed oxides on the HTVSR surface, exerting outstanding lamellar barrier effect. The further degradation and the generation as well as development of electrical tracking were efficiently suppressed. Our findings provided a new approach to fabricate silicone rubber with excellent tracking and erosion resistance.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2020
·Vol. 94
·期 3
·671-680
·
IF 2.008
Huang Xuelin,Ke Rui,Dong Yinsheng
A hybrid organic–inorganic sol–gel coating was prepared on the surface of cast aluminum–silicon (Al–Si) alloy via dip coating method to improve the anticorrosion ability. In the present work, bis(triethoxysilyl) ethane (BTSE) and 3-glycidoxypropyl-trimethoxysilane (GPTMS) were employed as the precursors to prepare hybrid sol–gel (BG) coating. Nano titanium dioxide (nano-TiO 2 ) was introduced to improve the corrosion resistance of the coating. The microstructures of the BG/nano-TiO 2 (BG-T) coating was characterized by scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), and Fourier-transform infrared (FT-IR) spectroscopy. The results showed that there was a chemical reaction between nano-TiO 2 and BG coating and a complete defect-free coating formed on the surface of Al–Si alloy. Moreover, there were a few only minor cracks appeared on the surface of BG-T coating after 15 days immersion in 3.5 wt.% NaCl solution. The corrosion resistant performances of the coatings were evaluated by the electrochemical tests. The results showed that the nano-TiO 2 particles elevated the corrosion potential and depressed the corrosion current, thereby improved the corrosion resistance. The long-term immersion tests of BG and BG-T coating further showed that the BG-T coating possesses an excellent long-term stability for corrosion protection.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2019
·Vol. 19
·期 11
·7169-7177
·
IF 1.093
Qin Zhuozhuo,Liu Wenxia,Chen Huabin,Chen Jun,Li Zhenzhen
Developing full-spectrum photocatalysts that harvests solar light from ultraviolet to near-infrared light has aroused great interest in photodegradation of organic pollutants, due to the imminent energy crisis and growing pollution issues. Herein, we report an excellent full-spectrum
photocatalyst derived from calcination of an Mg/Zn/Al/Er-hydrotalcite-like compound. The photocatalyst is a stable multi-phase oxide consisting of various syntrophic Er3+-doped metal oxides with different particle sizes and morphology. Its ultraviolet (UV) photocatalytic activity
is maximized by increasing the fraction of Zn2+ and sustaining the pure hydrotalcite-like phase with an appropriate fraction of Mg2+ in preparing the Mg/Zn/Al/Er-hydrotalcite-like precursor. The visible and NIR photocatalytic activities are triggered by an indirect excitation
involving an up-conversion process. The major active species of the photocatalyst in the photodegradation of methyl orange are superoxide anions and photogenerated holes. Nevertheless, hydroxyl radicals also play a moderate role in the photodegradation process. This work finds a new way to
prepare full-spectrum photocatalysts with tunable chemical compositions via an environmentally friendly hydrotalcite-like precursor.
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