MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Qingqing Ma,Nan Wang,Guozhu Liu,Li Wang
Pd catalysts on mesoporous silica SBA-15 functionalized with alkyltriethoxysilane (alkyl = methyl, ethyl, propyl and isobutyl) were prepared. The effects of grafting sequence on the grafting amount were studied. The catalysts were characterized by XRD , FT-IR, elemental analysis , thermogravimetric analysis , nitrogen adsorption-desorption, TEM and XPS , and evaluated using catalytic hydrogenation of 2-ethyl-anthraquinone. The grafting amount increases with increasing the alkyl chain length of alkyltriethoxysilane. The highest grafting amount with the carbon content of 1.56% is obtained using an ante-grafting procedure where the grafting is performed prior to the removal of template, and this catalyst shows the highest activity and selectivity (98.3%). The accordant relationship between the activity of Pd/SBA-15 catalysts and their grafting amount indicates a positive effect of hydrophobicity of SBA-15 created by grafting on the catalytic hydrogenation of 2-ethyl-anthraquinone.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Wei Qian,Lina Lin,Yunxiang Qiao,Xiuge Zhao,Zichen Xu,Honghui Gong,Difan Li,Manyu Chen,Rong Huang,Zhenshan Hou
The N-doped carbon layer coated SBA-15 support has been accomplished via a pyrolysis process . The ultra-low loading Ru nanoparticles ( ca. 0.1 wt.%) was incorporated into the support by impregnation and the sequential reduction. The images of HAADF-STEM revealed that the Ru particles with sub-1-nm size (0.2-0.7 nm) were uniformly dispersed on the support. The ultrafine Ru particles displayed the excellent activity for the hydrogenation of olefins , arenes, phenol derivatives and heteroarenes in aqueous phase. The aliphatic or alicyclic compounds were produced selectively without the hydrogenolysis of C O and C N bonds. The high turnover frequency (TOF) values can reach up to 10,000 h −1 . Notably, the activity of these catalysts improved dramatically with decreasing the sizes of Ru particles. Meanwhile, the N-doped carbon layer coating endowed the high stability of the Ru catalysts and prevented the leaching of the Ru species owning to the strong interaction between doped-N atoms and the ultrafine Ru particles. Overall, this work provides a highly attractive strategy to construct the supported sub-1-nm Ru particles utilized for the aqueous hydrogenation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Lixue Gai,Lin Guo,Qingda An,Zuoyi Xiao,Shangru Zhai,Zhongcheng Li
Functionalized SBA-15 has attracted considerable interest owing to its highly ordered mesoporous structure, well thermal stability and great potential applications. Meanwhile, as was demonstrated, polypyrrole (PPy) with good electrical conductivity is also a very popular absorber-related candidate. Herein, long-rod shape SBA-15/PPy-X composites were successfully synthesized via a simple hydrothermal treatment by combining in situ chemical oxidative polymerization method. The SBA-15/PPy-X composites exhibited effective absorption band (RL < −10 dB) and electromagnetic wave absorption capacities in comparison with the pristine SBA-15 sample, which were pertinent to the properties of strong dielectric loss and better impedance matching, implying enhanced dielectric properties by modifying with suitable amount of PPy species. The minimum reflection loss (RL) of SBA-15/PPy-0.5 composites reached −44.7 dB with a very low filler loading (15 wt%), corresponding to the thickness of 3.5 mm at 8.9 GHz. Besides, the effective absorption bandwidth was up to 6.1 GHz (11.1–17.2 GHz) and 3.8 GHz (7.4–11.2 GHz) with the thickness of 2.5 mm and 3.5 mm, respectively, which can cover most of the Ku-band (12–18 GHz) and X-band (8–12 GHz). The results indicated that the newly designed silica-based SBA-15/PPy-X composites can be promising EMW absorbers with an excellent performance at a target frequency (typical radar channels).
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Yan-Yun Meng,Qing-Da An,Zuo-Yi Xiao,Shang-Ru Zhai,Zhan Shi
Through hydrothermal synthesis and impregnation-reduction processes, a series of Pd-based nanocomposites using N-doped carbon layers coated ZrSBA-15 as the supports have been manufactured, aiming to upgrade the catalytic activity and stability of the catalysts. Pentaethylenehexamine (PEHA) was served as a nitrogen source to generate N-doped carbon (CN) layers that were pre-deposited into the acidic platelet framework ZrSBA-15, and then followed by introducing Pd 0 nanoparticles (NPs) onto it, finally leading to the formation of target composite Pd/CN-ZrSBA-15. The samples were characterized by XRD , TEM, SEM, N 2 adsorption-desorption isotherm, FTIR, XPS etc. The catalytic performance of as-prepared catalysts was evaluated by the aerobic oxidation of benzyl alcohol and the reduction of 4-NP, respectively. Duo to the platelet-like morphology with shortened channels and the modification of N-doped carbon layers, which could effectively decrease pore blocking in the process of preparation and reactions as well as enhance the metal-support interaction, the derived catalysts could afford 85% conversion of benzyl alcohol and 100% selectivity of benzaldehyde, and the conversion of 4-NP was also up to 96%. More remarkably, the catalysts could be reused at least ten times without significantly loss in catalytic activity.
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ADVANCED MATERIALS
·
2022
·Vol. 35
·期 3
·2208078
·
IF 32.086
Shaocheng Liu,Zhenyu Guo,Xianxin Wu,Xinfeng Liu,Zijian Huang,Liang Li,Jinwen Zhang,Huanping Zhou,Ling-Dong Sun,Chun-Hua Yan
While quasi-two-dimensional (quasi-2D) perovskites have emerged as promising semiconductors for light-emitting diodes (LEDs), the broad-width distribution of quantum wells hinders their efficient energy transfer and electroluminescence performance in blue emission. In particular, the underlying mechanism is closely related to the crystallization kinetics and has yet to be understood. Here for the first time, the influence of bifunctional zwitterions with different coordination affinity on the crystallization kinetics of quasi-2D perovskites is systematically investigated. The zwitterions can coordinate with Pb 2+ and also act as co-spacer organic species in quasi-2D perovskites, which collectively inhibit the aggregation of colloidal precursors and shorten the distance of quantum wells. Consequently, restricted nucleation of high- n phases and promoted growth of low- n phases are achieved with moderately coordinated zwitterions, leading to the final film with a more concentrated n distribution and improved energy transfer efficiency. It thus enables high-efficiency blue LEDs with a recorded external quantum efficiency of 15.6% at 490 nm, and the operation stability has also been prolonged to 55.3 min. These results provide useful directions for tuning the crystallization kinetics of quasi-2D perovskites, which is expected to lead to high-performance perovskite LEDs.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
·
IF 3.898
Haocui Zhang,Zhourong Xiao,Mei Yang,Jijun Zou,Guozhu Liu,Xiangwen Zhang
Ni/SBA-15 modified by highly dispersed cerium-oxide was prepared with the aid of sucrose for steam reforming of JP10 (C 10 H 16 ). Their characterization showed that addition of appropriate amount ceria led to the formation of highly dispersed CeO 2 and Ni, and the CeO 2 covered smaller nickel particles like strawberry seeds to form much more interface between them. Their catalytic activity exhibited higher stability over time on stream of 6.5 h with conversion higher than 95% and higher carbon resistance (mass loss less than 4.5% by TG), which may derive from good properties below: (1) much more interface enhanced cooperation effect and increased turnover frequency at the interface; (2) the stronger interaction between Ni and ceria to suppress sintering by formation of Ni-O-Ce solid solution; (3) the large amount of oxygen vacancies from the formation of Ni-O-Ce solid solution and highly dispersed CeO 2 to facilitate the water–gas–shift reaction and carbon removal.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 40
·61446-61456
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IF 5.19
Zhao Zheng-Yin,Xiong Jun,Wang Yuan,Cui Caixi
It is significant to explore the advanced oxidation process (AOP) for antibiotic degradation. Herein, a peroxymonosulfate (PMS) activator, Sr 2 FeO 4 /SBA-15 (SFS) heterogeneous catalyst, was synthesized by in situ growth of Sr 2 FeO 4 on the surface of SBA-15. In SFS/PMS catalytic system, Sr atom provided electrons to Fe(II) ↔Fe(III) ↔Fe(II) redox cycle through Sr-O-Fe bonds for PMS activation. The SFS catalyst could activate PMS to generate a free radical coexistence system, including sulfate radical (SO 4 ∙ − ) and hydroxyl radicals (∙OH). The catalyst possessed high catalytic activity and high stability. The degradation efficiency of sulfapyridine (SAD) over the SFS/PMS catalytic system could reach 99.0% after 90 min reaction. After the 5th reuse, the degradation efficiency of SAD was still more than 94.0%, and the phase structure of the catalyst did not alter. The low ion leaching concentration would be more conducive to reuse and avoiding secondary pollution, in comparison to homogeneous catalysts. This catalyst can be widely applied to organic wastewater treatment.-->
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tuo Xin,Rongkun Zhou,Qiuju Xu,Xiangcheng Yuan,Zilong Zheng,Yiqing Li,Qi Zhang,Jinzhang Liu
Aqueous rechargeable Zn-ion batteries (ZIBs) have been regarded as a complement to LIBs due to their merits in terms of high safety, low cost, environmentally benignity, and long cycle life. However, the Zn metal anode suffers from corrosion and parasitic reactions in the aqueous electrolyte, which lead to growth of byproduct flakes and hydrogen gas evolution in the Zn platting/stripping process. Here, an organic additive, 15-crown-5 ether (15-CE-5), is added into the aqueous ZnSO 4 electrolyte to improve the Zn anode performance by altering the Zn 2+ solvation sheath. Other CE molecules such as 12-CE-4 and 18-CE-6 are also tested, while their efficacies are inferior compared to that of 15-CE-5. The optimal concentration of 15-CE-5 in the ZnSO 4 electrolyte is found to be 2 wt%, which enables the best performance of Zn anode in either Zn||Zn symmetric cells or MnO 2 ||Zn full cells. Using this modified electrolyte, the Zn||Zn symmetric cell exhibits a cycle life of 770 h when tested at 2 mA cm −2 and a set capacity of 2 mAh cm −2 , and the MnO 2 ||Zn full cell shows enhanced and stable capacity over 1000 cycles. The experimental results are elucidated by theoretical studies including molecule dynamics simulations and density functional theory calculations.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Haibiao Yu,Xiu Jia,Peng Wang,Ying Xiong,Weijun Shan,Congge Zhang,Zhimeng Song
A series of x wt%Al-SBA-15 catalysts prepared by modified wetness impregnation was investigated for γ-valerolactone (GVL) decarboxylation to butene . It was found that the impregnation of Al species not only remained the ordered mesoporous structure of parent SBA-15, but also created large amounts of Brønsted and Lewis acid sites on the surface of catalyst. The considerable amount of solid acid sites and the suitable Brønsted/Lewis acid ratio endowed 2.23 wt%Al-SBA-15 catalyst an excellent catalytic performance. Under the optimized conditions, the GVL conversion and butene yield can reach 99.8% and 96.6% at 320 °C, respectively. Mechanism studies indicated that the decarboxylation of γ-protonated PEA controlled speed of the whole reaction. Moreover, the catalytic activity of regenerated 2.23 wt%Al-SBA-15 catalyst was satisfactory after eight cycle tests, and the butene yield could still reach 92.2%.
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International Journal of Environmental Science and Technology
·
2021
·Vol. 19
·期 8
·7205-7216
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IF 2.86
Wu Chunlai,Liu Qiong,Peng Chuanyun,Xu Wenwen
In this work, novel glutamic acid-functionalized SBA-15 was prepared for sensitive and selective lead and copper ions removal from wastewater sample. The material was characterized by X-ray diffractometry, scanning electron microscope, Brunauer–Emmett–Teller surface area measurement and Fourier transform infrared spectroscopy. The as-prepared material maintains the coordination properties of glutamic acid to lead and copper ions and exhibited better adsorption performance than that of pure SBA-15. The effects of different parameters such as pH of the solution, adsorption time, initial concentration, ion selectivity and regeneration were investigated on the Pb(II) and Cu(II) adsorption by the prepared adsorbent. It was found that the adsorption process can reach equilibrium within 20 min and can be described by pseudo-second-order kinetic model. Adsorption isotherm analysis showed that the adsorption was in accordance with Langmuir adsorption isotherm model, and the maximum adsorption capacity of lead and copper ions was 12.14 mg/g and 13.29 mg/g, respectively. In addition, common co-existed ions have no interference on Pb(II) and Cu(II) adsorption. Moreover, adsorption–elution cyclic results demonstrated that Pb(II)- and Cu(II)-adsorbed composite adsorbent could be effectively regenerated by 0.5 mol/L of HCl, and the regenerated adsorbent could be employed for repeated use without significant deterioration in its real performances, demonstrating the good stability of the adsorbents. Therefore, the composite adsorbent can be used potentially to remove Pb(II) and Cu(II) ions from water samples in practical applications for environmental remediation. Graphic abstract Glutamic acid-functionalized SBA-15 can be used as adsorbent for efficient adsorption/desorption of Pb(II) and Cu(II) from wastewater.
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Frontiers in Chemistry
·
2021
·
IF 5.221
Chang Siyuan,He Xuejun,Li Bingfeng,Pan Xin
Upgrading of biomass derived 5-hydroxymethylfurfural (HMF) has attracted considerable interest recently. A new highly HMF-tolerant strain of Burkholderia contaminans NJPI-15 was isolated in this study, and the biocatalytic reduction of HMF into 2,5-bis(hydroxymethyl)furan (BHMF) using whole cells was reported. Co-substrate was applied to improve the BHMF yield and selectivity of this strain as well as HMF-tolerant level. The catalytic capacity of the cells can be substantially improved by Mn2+ ion. The strain exhibited good catalytic performance at a pH range of 6.0–9.0 and a temperature range of 25°C–35°C. In addition, 100 mM HMF could be reduced to BHMF by the B. contaminans NJPI-15 resting cells in presence of 70 mM glutamine and 30 mM sucrose, with a yield of 95%. In the fed-batch strategy, 656 mM BHMF was obtained within 48 h, giving a yield of 93.7%. The reported utilization of HMF to produce BHMF is a promising industrially sound biocatalytic process.
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MICROCHEMICAL JOURNAL
·
2020
·
IF 3.594
Lianjing Zhao,Dehao Kong,Zepei Wu,Guannan Liu,Yuan Gao,Xu Yan,Fangmeng Liu,Xiaomin Liu,Chenguang Wang,Jiuwei Cui,Geyu Lu
The combination of nanomaterials and DNA has captured extensive attention in the fields of sensor, catalysis, biomedicine and material science. The applications of DNA functionalized MoS 2 nanosheets (NSs) in biosensor and biomedicine in turn present an fascinating topic about biointerface science between DNA and MoS 2 NSs. The surface interaction between DNA and MoS 2 NSs was explored by adsorption and desorption experiments. The results indicated that van der waals force played an crucial role in DNA adsorption by MoS 2 NSs. Additionally, it was proved that the quenching of dye labelled DNA probe by MoS 2 NSs was attributed to fluorescence resonance energy transfer. Based on the extraordinarily high quenching efficiency of MoS 2 NSs and different adsorption affinity of MoS 2 NSs toward aptamer and aptamer-targeted protein, an aptameric biosensor was fabricated to detect carbohydrate antigen 15–3. The fabricated biosensor not only displayed high sensitivity with the detection limit of 0.0039 U/mL (S/N = 3), but also exhibited good stability and selectivity. The proposed sensing platform provided an easy-constructed and cost-effective protocol to detect other aptamer targeted biomolecules. The fundamental study of biointerface science on DNA and MoS 2 NSs will facilitate their potential applications in various fields.
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