MICROPOROUS AND MESOPOROUS MATERIALS
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2021
·
IF 5.455
Changhao Yan,Shouteng Zheng,Na Chen,Shouqi Yuan,Yao Chen,Bing Li,Yunlei Zhang
In this work, the novel acid-base bi-functional mesoporous SBA-15 catalysts with four kinds of morphologies were synthesized by Mg incorporated and sulfated zirconia (SZ) grafted. The introduction of Mg to mesoporous SBA-15 materials significantly improves the strength of the base. And the supported SZ group exhibit effective Brønsted/Lewis acid strength. The physical and chemical properties of the prepared materials were systematically analyzed by the characterization tests of SEM, TEM, XRD , N 2 adsorption-desorption of, FT-IR, TGA , XPS, NH 3 /CO 2 -TPD and in-suit PY-IR. The obtained catalysts of SZ@Mg-SBA-15 could be applied to the fructose conversion into 5-hydroxymethylfurfural (5-HMF) with the co-solvent system of iPrOH/DMSO ( v / v = 9:1). 5-HMF was achieved under the optimal reaction condition with the highest yield of 98.6%. The result shows that the reaction of fructose dehydration into 5-HMF could be caused by the combination of Brønsted acid site and basic site. This work developed reaction system could avoid the large use of environmentally dangerous solvents, and provides a new economical and feasible method for the large-scale conversion of fructose biomass.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 22
·6827-6837
·
IF 6.177
Penghui Li,Junhua Gao,Jing Shi,Huixiang Wang,Xiangying Xing,Jingzhao Ren,Yu Meng,Liancheng Wang,Baoliang Lv
Linear terminal olefin epoxidation is a significant oxidation reaction for the synthesis of valuable industrial intermediates. As typical olefin epoxidation catalysts, supported tungsten oxides are rich in oxygen vacancies, which have been investigated for improving catalytic performance in other reactions, but the influence on olefin epoxidation is rarely studied. Herein, a series of WO3−x/SBA-15 catalysts with different oxygen vacancy concentrations were obtained by impregnation and sequent hydrogen reduction at 300–600 °C. Their catalytic performances for 1-hexene epoxidation with hydrogen peroxide at 70 °C were studied. It was found that an appropriate concentration of oxygen vacancies could improve epoxidation (the epoxide productivity increased from 135 to 196 μmolepoxide gW−1 min−1) and reduce the apparent activation energy (from 51.6 to 46.9 kJ mol−1). The oxygen vacancies are also beneficial for cycloolefin and other linear olefin epoxidation. In particular, the productivity of cyclooctene oxide was promoted from 4161 to 5744 μmolepoxide gW−1 min−1. This promotion effect was attributed to the increase in the number of Lewis acid sites caused by introducing moderate oxygen vacancies, which could improve the activation of hydrogen peroxide and facilitate epoxidation. In situ FT-IR spectroscopy and density functional theory calculations further indicated that increasing the oxygen vacancies contributes to reducing the energy barrier of the transfer of electrophilic oxygen atoms in active intermediate W–OOH to 1-hexene, thereby promoting epoxidation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2016
·
IF 3.349
Yan Liu,Jian Qiu,Yinhua Jiang,Zhanchao Liu,Minjia Meng,Liang Ni,Changchun Qin,Jianbo Peng
Ce(III) ion-imprinted polymer (Ce(III)-IIP) grafted on Fe 3 O 4 nanoparticles supported by SBA-15 mesopores microreactor was successfully synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization for selective removal of Ce(III) from aqueous solution. The characterization results suggest that the surface ion-imprinted polymer (IIP) synthesized by RAFT is a thin layer. Adsorption isotherm experiments indicated that Redlich-Peterson isotherm model best fitted the experimental data and the adsorption capacity of IIP was obviously higher than that of non-imprinted polymers (NIP) at the same conditions. The kinetics of adsorption followed the Thomas model. Moreover, competitive adsorption studies illustrated that Ce(III)-IIP offers the advantages of selectivity towards Ce(III) compared with NIP even in the presence of other metal ions. All above results indicated the potential application of Ce(III)-IIP for selective removal of Ce(III) from aqueous solution.
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RSC Advances
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2017
·Vol. 7
·期 6
·3443-3449
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IF 3.108
Ying Duan,Min Zheng,Dongmi Li,Dongsheng Deng,Cuicui Wu,Yanliang Yang
The Pd/SBA-15 catalyst was synthesised through the reduction of PdCl2 by the surface-bonded vinyl group on vinyl-functionalized SBA-15, which was prepared via co-polymerization. XRD and XPS characterization confirmed the successful reduction of Pd(II) to Pd(0). Pd/SBA-15 showed a narrow palladium particle-size distribution of about 5–6 nm in the TEM image. The Pd/SBA-15 catalyst was effective for the hydrogenation of aromatic nitro compounds with zero-order kinetics, and the TOF for the hydrogenation of nitrobenzene was 1124 h−1 at 313 K and 1 atm H2. A steric effect was observed for the substituted nitroarenes.
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COLLOID AND POLYMER SCIENCE
·
2014
·Vol. 293
·期 1
·109-123
·
IF 2.41
Liu Yan,Chen Rui,Yuan Dandan,Liu Zhanchao,Meng Minjia,Wang Yun,Han Juan,Meng Xiangguo,Liu Fangfang,Hu Zhaoyong,Guo Wenlu,Ni Liang,Yan Yongsheng
Highly thermal-responsive magnetic Sr(II)-imprinted polymer (Sr(II)-TMIIP) was successfully synthesized as a potential effective adsorbent for selective removal of Sr(II) in aquatic environments. First, magnetic polyethyleneimine-loaded mesoporous SBA-15 (Fe 3 O 4 @PEI-SBA-15) was prepared via a simple polymer-mediated self-assembly method. Then, the surface of Fe 3 O 4 @PEI-SBA-15 was endowed with reactive vinyl groups through modification with 3-(methacryloyloxy)propyl trimethoxysilane (MPS). With the aid of vinyl groups, free radical polymerization of N -isopropylacrylamide (NIPAM), methacrylic acid (MAA), and N , N ′-methylenebisacrylamide (BIS) in the presence of Sr(II) was performed with 2,2′-azobisisobutyronitrile (AIBN) as initiator, which provided a desired imprinted layer coating onto Fe 3 O 4 @PEI-SBA-15. The as-prepared Sr(II)-TMIIP was characterized by Fourier transmission infrared spectra (FT-IR), X-ray diffractometer (XRD), thermogravimetric analysis (TGA), scanning electron microscope (SEM), transmission electron microscope (TEM), vibrating sample magnetometer (VSM), UV, and N 2 adsorption–desorption techniques. The results showed that the Sr(II)-TMIIP exhibited thermal stability, temperature and magnetic sensitivity ( M
s = 10.34 emu/g), and ordered mesoporous structure. Batch mode adsorption studies were conducted to investigate the specific binding kinetics, adsorption equilibrium, and selective recognition ability of Sr(II)-TMIIP. Adsorption equilibrium experiments showed that the adsorption amount strongly depended on temperature and reached a maximum around the lower critical solution temperature (LCST). Regeneration experiments indicated that repeated adsorption and desorption by temperature swings were possible. Compared with the nonimprinted polymer (NIP), the Sr(II)-TMIIP had good temperature response and excellent selectivity and reusability, making it possible in applying for Sr(II) separation and controlled release.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiao Dan Sun,Zhangxin Duan,Jingjing Song,Hanxing Yang,Kai Yan,Zhenhua Tian,Dangge Gao,Jianzhong Ma
Carcinogen Cr(VI) is reduced efficiently into Cr(III) by a photocatalyst, but the produced Cr(III) is difficult to transfer from the photocatalytic active site. The “two birds with one stone” strategy is proposed to realize the in situ growth of ZnIn2S4 nanoplates on SBA-15 and the creation of separated active sites, in which ZnO loading on the porous SBA-15 nanorod was used as a zinc source. Obtained samples ZnIn2S4/SBA-15 (ZIS/SBA) showed the redshift of the absorption band and better separation of photoinduced carriers than pristine ZnIn2S4, due to its smaller size and S defect. All of the Cr(VI) was reduced to Cr(III) by the ZIS/SBA sample during the photocatalytic process, which was 2 times higher than pristine ZnIn2S4. Moreover, 92.8% of Cr(III) was adsorbed simultaneously during photocatalysis due to the electrostatic interaction from SBA-15. In addition, the ZIS/SBA sample showed good recycling stability after 5 times cycles, providing a new strategy for the in situ growth of ZnIn2S4 on the surface of porous materials and a novel way for the simultaneous removal of Cr(VI) and Cr(III) during photocatalysis.
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高影响因子
Journal of Physical Chemistry C
·
2012
·
IF 4.805
Yajuan Hao,Yanzhu Chong,Shuru Li,Hengquan Yang
Au nanoparticles with different sizes were introduced into the nanocages of a mesoporous material SBA-16 with the aid of chemical modification, leading to new Au-supported catalysts Au/SBA-16. These catalysts were characterized with Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), transmission electron microspectroscopy (TEM), N2 sorption, and X-ray photoelectron microspectroscopy (XPS). These results revealed that uniform Au nanoparticles with sizes of a few nanometers were successfully positioned inside the nanocages of SBA-16. Such catalysts were catalytically active in the oxidative esterification of various alcohols even including less reactive straight-chain alcohols. It was found that the activity of this catalyst strongly depended on the Au loading, and the Au loading of 5 wt % (corresponding to Au particles of 2–3 nm in sizes) led to the highest activity. Its activity was much higher than those of the analogous catalysts prepared from commercial silica gel as well as SBA-15. Furthermore, Au/SBA-16 could be reused at least eight reaction cycles without significant decrease in activity and selectivity. Its recyclability was much superior to that of the catalyst derived from commercial silica gel. The underlying reason may be that the unique nanostructure of SBA-16 can effectively prevent the growth of Au nanoparticles into less active, larger particles, as evidenced from TEM investigations. This study not only supplies a new, active, recoverable catalyst for the green transformations of alcohols to esters but also demonstrates that the three-dimensional mesoporous cage-like material SBA-16 has a superior ability in reducing the diffusion resistance and stabilizing metal nanoparticles against growth.
研究领域:
材料化学
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催化
·
纳米技术
·
绿色化学
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Siyu Zhou,Wanni Liu,Dongqi Liu,Xian Shi,Kai Huang,Feng Jiang,Hui Gao,Haian Xia,Ying Guan,Siquan Xu
Efficient catalytic conversion of cellulose into 5-hydroxymethylfurfural (HMF) remains challenging and arouses concern. In this study, iron phosphate (FePO 4 ) was embedded into the SBA-15 mesoporous silica matrix as an available active phase via ultrasound-assisted implantation, and then the abundant silanol nests were utilized to graft sulfonic acid groups to construct an innovative FeP@SBA-15-S catalyst. Through a systematic analysis of the characteristics of crystal, texture, element valence, acidity, hydrophilicity, etc., it was reflected that FeP@SBA-15-S catalyst gave the active FePO 4 component porosity and exhibited bifunctional acidity. Without pretreatment and other acid additives, FeP@SBA-15-S catalyzed cellulose under optimal conditions provided a desired HMF yield of 52 %. More meaningfully, the cellulose and hemicellulose components in native wheat straw could be catalyzed simultaneously by FeP@SBA-15-S catalyst, yielding 61 % HMF and 60 % furfural in one-pot. The cyclability evaluation showed that the FeP@SBA-15-S catalyst still had considerable activity after six continuous runs, with a slight loss in activity attributed to the leaching of active components and pore coverage. A clear catalytic pathway was summarized by GC-MS and 13 C NMR spectrum as cellulose undergoing glucose monomer ring opening, isomerization to fructose, fructose ring closure and final dehydration, and the by-products were also detected as mainly C 3 -C 23 fragments and oligomers.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2018
·Vol. 93
·期 10
·3028-3034
·
IF 2.587
Wei Chen,Yong Sun,Juan Du,Zhihao Si,Xing Tang,Xianhai Zeng,Lu Lin,Shijie Liu,Tingzhou Lei
BACKGROUND 5-(Aminomethyl)-2-furanmethanol (AMF), used widely in medicinal chemistry, is usually synthesized by the reductive amination of furfural or 5-hydroxymethylfurfural (HMF) with ammonia. However, a challenging task when synthesizing this furyl primary amine is to enhance the selectivity of the product due to its high nucleophilicity. Conventional measures have used excessive liquid ammonia and precious metal catalysts. Usually, the molar ratio of ammonia to substrate is up to 30:1. This study employed aqueous ammonia to synthesize AMF by the direct reductive amination of HMF using the non-noble metal Ni/SBA-15 catalyst. RESULTS The Ni/SBA-15 catalyst displayed higher catalytic selectivity in the reductive amination of HMF to AMF compared to other precious metal catalysts, such as Ru/C, Pd/C and Pt/C. The AMF yield of 89.8% was obtained at the relatively mild reaction temperature of 100 °C for 4 h. After the fifth cycle, an acceptable decrease in catalytic activity with 74.2% yield of AMF was observed. CONCLUSION An improved process was developed for preparing AMF by the reductive amination of HMF with aqueous ammonia using the non-noble Ni/SBA-15 catalyst. The high selectivity of nickel catalyst is attributed mainly to the moderate catalytic activity. Moreover, a small amount of water enhanced the yield of AMF by promoting the formation of ammonium ions to prevent the further side reaction of AMF with HMF. Results of recycling experiments and analyses showed that agglomeration, loss and oxidization of nickel species together with carbon deposition were responsible for the slight deactivation of the catalyst. © 2018 Society of Chemical Industry
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Meng Zhang,Bingxian Chu,Guoying Li,Jianze Xiao,Haowen Zhang,Yujie Peng,Bin Li,Peng Xie,Minguang Fan,Lihui Dong
A series of triethanolamine-modified mesoporous SBA-15 catalysts were synthesized by a facile one-pot process, and used as the catalyst for the synthesis of cyclic carbonates through the cycloaddition of CO 2 with epoxides. The properties of catalysts were characterized by nitrogen adsorption–desorption, elemental analysis (EA), Fourier transform infrared (FT-IR) spectra, Magic angle spinning nuclear magnetic resonance (MAS NMR), X-ray diffraction (XRD), scanning electron microscope (SEM), and transmission electron microscopy (TEM), and the results suggested that triethanolamine (TEA) had been successfully immobilized on SBA-15. It was highly active in the cycloaddition reaction, in which the maximum yield of PC could achieve 93.47% under the conditions as follow: catalyst amount of 0.20 g, reaction temperature of 110 °C, reaction pressure of 2.0 MPa and reaction time of 4 h. Notably, the catalyst can be easily recovered by filtration, and it can be retained most of its catalytic stability and activity after five recycling times. On the basis of the experimental results, the interactions between the catalysts and the substrates were studied by DFT calculations, and the possible mechanism for the reaction was proposed.
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FOOD CHEMISTRY
·
2017
·
IF 4.529
Hongwu Wang,Yanqing Liu,Su Yao,Peijie Zhu
In this work, a highly selective molecular imprinted polymer (SBA-15@MIP) was prepared using dicyandiamide (DCD) as the template molecule and mesoporous silica SBA-15 as the carrier. The resulting polymers were characterized by scanning electron microscopy and FT-IR spectra. A highly ordered mesoporous nanostructure was observed for the fabricated polymer. The performance tests showed that the adsorption capacity of SBA-15@MIP for DCD was higher than those of non-imprinted mesoporous silica polymer (SBA-15@NIP) and SBA-15. SBA-15@MIP was successfully used as the solid-phase extraction (SPE) sorbent coupled with HPLC for trace DCD determination in bovine milk and milk powder. Under selected conditions, a favorable linearity between 1 μg/mL and 100 μg/mL was obtained and the detection limit was estimated to be 0.08 μg/mL (bovine milk) and 0.10 μg/mL (milk powder). These results indicated that SBA-15@MIP could be used as an efficient SPE adsorbent for enrichment of DCD in bovine milk and milk powder.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yu Yin,Chunhui Ma,Wei Li,Sha Luo,Zhanshuo Zhang,Shouxin Liu
Facilitated isomerization of cellulose hydrolysis intermediate glucose without unexpected byproducts, which is the rate-determining step in the production of high-value-added biofuels, enables the efficient production of 5-hydroxymethylfurfural (5-HMF) from cellulose. In this work, considering the essential role of the acidity control and shape selectivity of a zeolite catalyst, a NiO-loaded mesoporous NiO/poly(vinyl pyrrolidone) (PVP)-phosphotungstic acid (HPA)@SBA-15 nanoreactor was prepared. This SBA-15 nanoreactor with a pore size of 5.47 nm reduced the concentration of byproducts formic acid (FA) and levulinic acid (LA) through shape selection for intermediates. Well-defined NiO nanoparticles (Ni-to-carrier mass ratio was 1:1) provided the NiO/PVP-HPA@SBA-15 nanoreactor a high Lewis acidity of 99.29 μmol g–1 for glucose catalytic isomerization, resulting in an increase in total reducing sugar (TRS) yield by 5 times. Such a nanoreactor remarkably improved the reaction efficiency of 5-HMF production from cellulose (a 5-HMF selectivity of 95.81%) in the 1-butyl-3-methylimidazolium chloride ([BMIM]Cl)/valerolactone (GVL) biphasic system.
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危险品化学品经营许可证（带存储）