Journal of Environmental Chemical Engineering
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2021
·
IF 5.909
Xi Cheng,Qingge Feng,Dachao Ma,Hongcheng Chen,Xu Zeng,Feifan Xing,Jiayang Teng
To eco-friendly catalyze glucose to levulinic acid, recyclable acid catalyst has been researched. The synthesis process of propyl sulfonic acid functionalized SBA-15 was improved and the hydrophobic treatment was performed. The structure and functional groups of materials were characterized by X-ray diffraction, transmission electron microscopy , N 2 adsorption–desorption isotherms, elemental analysis, Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy and simultaneous thermal analysis. The catalytic activity , recyclability and hydrothermal stability of CH 3 -SBA-15-SO 3 H material were researched. The highest yield of levulinic acid at 61.56% was obtained at 180 ℃ for 2.5 h in γ-GVL-water solvent system, and the yield of levulinic acid was only decreased by 2% after 4 times reuse. The high degree of silicon polycondension and hydrophobic surface of CH 3 -SBA-15-SO 3 H were the key to maintain the hydrothermal stability. The CH 3 -SBA-15-SO 3 H solid acid had great potential in development and utilization of biomass resources .
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Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 19
·3636-3645
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IF 5.958
Yifei Ye,Dazhi Li,Ping Xu,Jianmin Sun
Until recently, many metal-based catalysts have been developed for the cycloaddition reaction of CO2 with epoxides. However, the leaching of the active metal component would lead to various environmental problems. A novel nonmetal B-doped Lewis acid–base catalyst with hydrogen bond donor (HBD) groups (B-SBA-15-NH2) was prepared successfully through the hydrothermal process and post-modification. B-SBA-15-NH2 exhibited good catalytic performance for the CO2 cycloaddition reaction, and 95% yield of propylene carbonate and satisfied selectivity (98%) were achieved in the presence of the KI cocatalyst. The efficient catalytic activity of B-SBA-15-NH2 resulted from the synergistic effects of B and HBD groups, together with the functionalized –NH2 groups. B-SBA-15-NH2 also exhibited good generality with acceptable yields for the corresponding cyclic carbonates in the CO2 cycloaddition with various epoxides. Furthermore, the developed B-SBA-15-NH2 catalyst could be easily separated by centrifugation and reused for five runs without an obvious loss in activity. The good activity and stable reusability of the metal-free B-SBA-15-NH2 catalyst demonstrate that it is a promising green candidate catalyst in the field of CO2 conversion.
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2016
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IF 3.958
Mengshuai Liu,Bo Liu,Lin Liang,Fangxiao Wang,Lei Shi,Jianmin Sun
The novel bifunctional Zn/SBA-15 supported ammonium salt (NH 3 I-Zn/SBA-15) as single-component heterogeneous catalyst for the coupling of CO 2 with epoxides was developed. FT-IR, XRD, N 2 adsorption/desorption, TEM, XPS techniques were used to determine the morphological structure and physicochemical properties of NH 3 I-Zn/SBA-15 sample. The catalyst exhibited exceptionally effective activity with 93% yield and 99% selectivity and a high TOF of 306 h −1 to propylene carbonate at 130 °C and 3 MPa of CO 2 for 12 h in the absence of cocatalyst and solvent participation. Also the catalytic system was versatile to the cycloadditions of other epoxides with CO 2 under the optimized reaction conditions. Additionally, the catalyst was easily recycled and reused only with slight loss of activity after five recycles. Besides, a possible catalytic mechanism involving cooperative activation of epoxide and ring-opening by one-component and bifunctional catalyst was proposed. The protocol herein provides important insights on design of novel single-component heterogeneous catalysts for CO 2 relevant transformations.
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Catalysis Science & Technology
·
2017
·Vol. 7
·期 3
·725-733
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IF 5.773
Ning Liu,Zhimin Wu,Meng Li,Shanshan Li,Yongfei Li,Rongdong Yu,Langsheng Pan,Yuejin Liu
Bimetallic Al–La oxides were conjointly precoated on SBA-15 prior to the introduction of potassium fluoride to achieve solid superbases at low temperature by a modified wetness impregnation method. This breaks the tradition of decomposition of KNO3 at high temperature and gives rise to a new approach to generating superbasic sites on SBA-15. The physico-chemical characteristics of the prepared KF/Al–La@SBA-15 materials were investigated using FT-IR, XRD, TG-DTG, N2 adsorption–desorption, TEM, SEM-EDS, acid–base titration, Hammett indicators and CO2-TPD measurements. The results demonstrated that the addition of Al species promoted the dispersion behavior of La species inside the channels, and the bimetallic species could synergistically protect the mesoporous structures of SBA-15 against KF corrosion. With increasing Al content, KF/Al–La@SBA-15 exhibited a long-range ordering of the pores with relatively narrow pore size distribution as well as high specific surface area. The research results showed that the KF/Al–La@SBA-15 (0.4) catalyst possessed a total basicity up to 0.79 mmol g−1 and superbasicity with a strength of 26.5. The catalytic activity of the prepared materials was evaluated in the ring-opening reaction of propylene oxide with methanol. Compared with the SBA-15 supported monometallic oxide (Al or La) catalysts, KF/Al–La@SBA-15 (0.4) exhibited the highest catalytic activity for the ring-opening reaction of propylene oxide with methanol. This is associated with the synergistic effects between Al and La species and the high dispersion of active components on the SBA-15 support.
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Jiaxin Wang,Ying Liu,Baozhong Zhu,Jiuyu Chen,Qing Wang,Yunlan Sun
Amine-modified mesoporous silicon was widely used for CO 2 capture. However, its adsorption capability was significantly affected by temperature and humidity. In this paper, tetraethylenepentamine (TEPA) modified SBA-15 adsorbents were prepared for capturing CO 2 . The effects of the modification method, the concentration of TEPA, the adsorption temperature, and the humidity of atmosphere on CO 2 adsorption capability were studied. Moreover, combined with molecular dynamics (MD) and density functional theory (DFT) computations, the diffusion characteristics and adsorption mechanism were explored. The CO 2 adsorption capability of the adsorbent prepared by the ultrasonic impregnation method was higher than those prepared by the stirring impregnation method, owing to that ultrasonic impregnation could promote the uniformity of TEPA. With the increase of TEPA concentration of SBA-15, the CO 2 adsorption capability increased. SBA-15-2 had the highest CO 2 adsorption capability of 1.17 mmol/g at 30 °C. This was due to the N-containing functional groups, showing good affinity for CO 2 , introduced by TEPA impregnation. When the temperature increased from 30 °C to 70 °C, the CO 2 adsorption capability of all modified SBA-15 adsorbents decreased, since the CO 2 adsorption was an exothermic reaction. SBA-15-2 showed better water vapor resistance than SBA-15-2 (Stir). This was related to the higher dispersity of organic carbon chain introduced by TEPA modification after ultrasonic impregnation. The organic carbon chain of SBA-15-2 increased the water vapor resistance by reducing the hydroxyl group. Finally, from a microscopic aspect, the MD simulation suggested that impregnated TEPA inside SBA-15 may improve CO 2 capture by increasing the thickness of effective adsorption layer. Besides, the DFT simulation showed that TEPA modification increased the adsorption energy of SBA-15 on CO 2 . This serves as a reference for later mesoporous silicon adsorbent research and development on CO 2 capture.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 8
·2443-2451
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IF 5.721
Cong Mao,Jingwei Zheng,Babasaheb M. Matsagar,Ranjith Kumar Kankala,Tansir Ahamad,Yucheng Yang,Kevin C.-W. Wu,Xueqin Zhang
Ruthenium nanoparticles supported onto aluminum-doped mesoporous silica catalysts (Ru/Al–SBA-15) are fabricated using hydrothermal and impregnation methods for catalysis application. The Ru/Al–SBA-15-3 catalyst at a Si/Al molar ratio of 3 exhibited excellent catalytic performance for the hydrogenation of p-phthalic acid with high conversion efficiency (100.0%) and cis-isomer selectivity (84.0%) in water. Moreover, this system displays exceptional stability and recyclability through preserving the conversion efficiency, as well as a cis-isomer selectivity of 90.2 and 83.3%, respectively, after reusing it fourteen times. Such an exceptional system can also be ideal for the hydrogenation of aromatic dicarboxylic acids and their ester derivatives in water. Strong Lewis acid sites due to doped Al species play significant roles in the hydrogenation reaction. Moreover, isotope labeling studies indicated that water molecules effectively participated in the hydrogenation reaction. Hydrogen and water contributed half of the hydrogen atoms for this hydrogenation reaction. In the end, a plausible mechanistic pathway for the hydrogenation of p-phthalic acid using the Ru/Al–SBA-15-3 catalyst in water is proposed.
研究领域:
催化化学
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材料科学
·
有机化学
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 3
·597-605
·
IF 9.405
Shaoqi Yang,Xingmei Lu,Haoyu Yao,Jiayu Xin,Junli Xu,Ying Kang,Yongqing Yang,Guangming Cai,Suojiang Zhang
Selective catalytic hydrotreatment of lignin-derived phenols and dimeric ethers into alkanes is crucial for utilization of lignin and its fragments. Herein, we developed an efficient catalytic system with well-dispersed metal nanoparticles supported on SBA-15 synergistic with an ionic liquid. The catalytic system could catalyze the hydrodeoxygenation (HDO) of various monomeric and dimeric lignin-derived phenols into the corresponding alkanes under acid free conditions. The synergistic [Bmim]PF6-Ru/SBA-15 (1-butyl-3-methylimidazolium hexafluorophosphate) catalysis exhibited the best HDO activity for lignin-derived phenols and dimeric ethers with >99.0% conversion and maximum >98.0% selectivity of the corresponding alkanes. The yield of cyclohexane from diphenyl ether was 97.7% with 100% conversion under 2 MPa H2 at 130 °C for 6 h. The mechanism investigation confirmed that the Ru/SBA-15 catalyst and the anion of [Bmim]PF6 played crucial roles in the hydrogenation process and deoxidization process, respectively. The catalytic system was reused six times for HDO of diphenyl ether to test its stability.
研究领域:
化学工程
·
可再生能源
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JOURNAL OF NUCLEAR MATERIALS
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2019
·
IF 2.547
Hui Dan,Qiang Xian,Li Chen,Tianheng Xiong,Zhengdi Jiang,Facheng Yi,Yi Ding
Mesoporous ammonium molybdophosphate/SBA-15 (AMP/SBA-15) was considered as an excellent adsorbent to remove Cs + from radioactive wastewater. However, AMP/SBA-15 obtained from two-step method suffers from poor stability and low reuse ability. Herein, we reported a facile one-step method to fabricate AMP/SBA-15 using Phosphomolybdic acid (PMA) as acid media. The effect of PMA content on the properties of the resultant AMP/SBA-15 was investigated in detail. And the Cs + adsorption performance of the developed AMP/SBA-15 adsorbents was also evaluated. It was found that the PMA content had a strong influence on the structure and morphology of AMP/SBA-15. The mesoporous structure order of the AMP/SBA-15 decreased with increasing PMA content. The AMP particles were mainly incorporated into the framework of SBA-15. Furthermore, the AMP incorporation rate obtained from one-step method is much higher than that of two-step method. The developed AMP/SBA-15 with AMP in the framework of SBA-15 exhibited good stability and high reuse ability for the removal of Cs + .
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FUEL
·
2019
·
IF 5.128
Li Gao,Zhiyuan Shi,Ubong Jerome Etim,Pingping Wu,Wei Xing,Yi Zhang,Peng Bai,Zifeng Yan
A composite material Beta-SBA-15 (BS) comprising zeolite Beta units and SBA-15-like mesoporous structure was hydrothermally synthesized and served as catalyst support for the hydroisomerization of n-heptane. Materials were characterized by a variety of techniques. Characterization results revealed that Beta-SBA-15 composite has a two-dimensional hexagonal mesoporous channel with a pore size of 6.4 nm and a high concentration of moderate-strength acid sites. Evaluation results showed that Pt/HBS exhibited a relatively high n-heptane conversion (75.57%) with a good selectivity to isoheptanes (90.04%), resulting in the highest isoheptanes yield (68.04%) among all samples. The micro-mesoporous composite structure with moderate surface acidity enhanced diffusion of large isomerized intermediates as well as inhibiting the occurrence of cracking side reactions, achieving a high isoheptanes yield. Experimental data demonstrates that the indexed isomerization factor (IIF) as a performance descriptor can accurately predict the isomerization performance of catalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Jiasheng Zhou,Xiaoxin Zhou,Kunlun Yang,Zhen Cao,Zheni Wang,Chuchen Zhou,Shams Ali Baig,Xinhua Xu
Iron-manganese binary oxides (FeMnO x ) can remove contaminants from aqueous solutions with high efficiency, and mesoporous silica (SBA-15) is widely used as a supporting material due to its large specific surface area and good stability. In this study, SBA-15 was used to support FeMnO x in the synthesis of a novel arsenic (As) adsorbent (FeMnO x /SBA-15), and its characteristics under different reaction conditions, such as pH, temperature, presence of competing ions, and humic acid, were tested. The results showed that the contaminant adsorption efficiency of the novel adsorbent was better than that of bare FeMnO x , as the addition of SBA-15 decreased the agglomeration effect of FeMnO x . Additionally, FeMnO x /SBA-15 underwent calcination to further enhance its performance. The state of iron and manganese in FeMnO x /SBA-15 and the corresponding arsenic removal efficiency were improved by calcination at 350 °C with an FeMnO x /SBA-15 mass fraction of approximately 45%. Almost 90% of As (50 mL, 5.0 mg L −1 ) could be removed by 0.2 g L −1 of FeMnO x /SBA-15 (mass ratio of 45% and calcination temperature of 350 °C). The FeMnO x /SBA-15 could regenerate and still be used after four consecutive cycles. The high As sorption capacity, ability to regenerate, and reusability of FeMnO x /SBA-15 confirmed that this adsorbent is promising for treating As-contaminated drinking water.
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2018
·
IF 3.849
Biao Lu,Zhaowei Wu,Lijuan Ma,Xia Yuan
Phosphotungstic acid (HPW) was immobilized on a sulphonic-acid-functionalized SBA-15 mesoporous molecular sieve through a one-step hydrothermal synthesis method, using non-ionic surfactant pluronic P123 as a structure-directing agent in acidic media, tetraethoxysilane (TEOS) as a silicon source and 3-trimethoxysilyl-1-propanethiol (MPTMS) with hydrogen peroxide (H 2 O 2 ) oxidized to a sulfonic acid group. The obtained composite material HPW-SBA-15-SO 3 H has a high specific surface area, large pore volume and increased strong acidity. The effect of raw-material ratio on the catalyst was investigated. Catalysts that were prepared under optimal conditions of a molar ratio of (MPTMS)/ (MPTMS + TEOS) of 1:10, a molar ratio of (H 2 O 2 )/(MPTMS) of 18:1 and a mass ratio of (HPW)/(TEOS) of 1:10 exhibited an excellent catalytic activity in the esterification reaction of cyclohexene with formic acid. The cyclohexene conversion exceeded 86.7% and the cyclohexyl formate selectivity was 98.1% after 6 h at 353 K with a mole ratio of cyclohexene to formic acid of 1:3 and a catalyst dosage of 5.7% (w/w). The composite catalyst had a higher catalytic stability than the sulfonic-acid-functionalized SBA-15 and SBA-15-immobilized HPW individually. The cyclohexene conversion reached 72.0% even after reused four times. Fourier transform infrared and temperature-programmed desorption of ammonia revealed that a strong interaction existed between the sulfonic-acid group and the HPW, which prevented acid-active component of HPW and sulfonic-acid group loss from the carrier.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Ye Qu,Yanglin Chen,Yifei Ye,Ping Xu,Jianmin Sun
Heterogenization of homogeneous catalysts without the loss of activity is still a huge challenge. Herein, homogeneous [HTMG][His][I] amino acid ionic liquid (IL), consisting of 1,1,3,3-tetramethylguanidine cation, histidine anion and iodine anion, were introduced into the pore channels of SBA-15 substrate with the assistance of supercritical CO 2 (scCO 2 ) media. Due to its low viscosity, high diffusivity and absence of surface tension, scCO 2 enabled [HTMG][His][I] to highly disperse in SBA-15 pore channels. Surprisingly, [HTMG][His][I]/SBA-15 heterogeneous catalyst displayed higher CO 2 cycloaddition activity (95% propylene carbonate yield) than equivalent molar pristine [HTMG][His][I] homogeneous catalyst (69% propylene carbonate yield) under the identical conditions. The significantly enhanced activity was resulted from the synergistic effect of [HTMG][His][I] and SBA-15 support. Moreover, [HTMG][His][I]/SBA-15 performed outstanding universality of various epoxides and reusability. This work developed a promising strategy to heterogenization of homogeneous IL catalyst assisted by scCO 2 as synthetic media and provided an efficient catalyst for CO 2 conversion.
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