GREEN CHEMISTRY
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2019
·Vol. 21
·期 3
·597-605
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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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高影响因子
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
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有机化学
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Journal of CO2 Utilization
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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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Catalysis Science & Technology
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2022
·Vol. 12
·期 22
·6827-6837
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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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INDUSTRIAL CROPS AND PRODUCTS
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2022
·
IF 6.449
Shaoqing Wang,Zhihe Li,Weiming Yi,Peng Fu,Xueyuan Bai
Catalytic pyrolysis of corn cob lignin were preformed using a tailored HZSM-5 @Al-SBA-15 hierarchical zeolite for the production of value-added aromatic hydrocarbon. Resulted showed that the highly ordered two-dimensional p6mm mesoporous shell could uniformly form on the surface of HZSM-5 core phase. The porosity and acidity of the HZSM-5 @Al-SBA-15 could be tailored by adjusting the TEOS/HZSM-5 mass ratio in the synthesis process. The aromatic hydrocarbon components regulated due to pre-cracking and enhanced diffusion via the mesoporous shell, as well as the retained shape-selectivity of the HZSM-5 core. Herein, the relative content of MAHs reached 45.02% with fewer poly-aromatic hydrocarbons (PAHs) of 25.91% when the TEOS/HZSM-5 mass ratio of 1.0. However, the length of the diffusion path had a certain impact on the anti-coking behavior. The catalytic stability of the hierarchical zeolites was also improved, with less coke formation than HZSM-5 alone. This work demonstrates that using a tailored hierarchical zeolite to regulate aromatic hydrocarbon components is feasible, and provide a reference for the practical application of agricultural crop wastes.
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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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JOURNAL OF NUCLEAR MATERIALS
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2019
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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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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
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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PubMed
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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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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COLLOID AND POLYMER SCIENCE
·
2014
·Vol. 293
·期 1
·109-123
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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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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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