Nanoscale
·
2018
·Vol. 10
·期 47
·22348-22356
·
IF 7.233
Xusheng Cheng,Dongxu Wang,Jiancong Liu,Xin Kang,Haijing Yan,Aiping Wu,Ying Gu,Chungui Tian,Honggang Fu
Decreasing Pd usage whilst maintaining a superior performance is promising, but remains a challenge in the catalytic field. Herein, we have demonstrated the highly efficient promotion of Mo2N with a reduced amount of Pd for the liquid-phase hydrogenation reaction. The Mo2N (2–3 nm) was uniformly anchored onto mesoporous SBA-15 by using PMo12 as the Mo source. The small size and good dispersion of Mo2N is favourable for allowing their effective contact with post-loading Pd. This good contact is conducive to developing a synergistic catalyst, which was verified by studying the liquid-phase hydrogenation of p-nitrophenol (PNP) to p-aminophenol (PAP) with NaBH4 as the H source. The conversion ability of PNP to PAP on 1 wt% Pd–Mo2N/SBA-15 was vastly superior to 1 wt% Pd/SBA-15 and even better than 20 wt% Pd/SBA-15. The low-Pd, highly efficient catalysis is ascribed to the transfer of the electrons from Mo2N to Pd for the easy activation of H. The synergy can be affected by the type of support used. SBA-15 is superior to SiO2 and the other supports, which could be related to the large surface area and the plentiful number of pores on SBA-15, which is favourable to the dispersion of Pd and Mo2N, and the transfer/diffusion of the reactants. In particular, a highly efficient catalyst can be achieved at an even more reduced Pd loading (0.05 wt%). The current method describes the design of a highly efficient catalyst for the hydrogenation reaction using low amounts of noble metals.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2013
·
IF 3.172
Yan Zhao,Bing Yan
GaN-functionalized rare earth (Eu 3+ and Tb 3+ ) organic/inorganic mesoporous nanocomposites have been successfully synthesized (designated as RE(L SBA-15) 3 (L GaN); RE = Eu, Tb; L = TAA Si, BTA Si). The organosilane precursor materials (L SBA-15) are synthesized by co-condensation of tetraethylorthosilicate (TEOS) and the functionalized β-diketones (TAA Si and BTA Si) in the presence of Pluronic P123 surfactant as a template. The modified β-diketones ligands are also used to covalently bond with surface-modified GaN and formed another precursor L GaN. Both of the precursors can coordinate with rare earth ions to synthesize the final mesoporous materials via a sol–gel process. FTIR, TEM, XRD, and nitrogen (N 2 ) adsorption/desorption measurements are employed to characterize the mesostructure of RE(L SBA-15) 3 (L GaN). The luminescence properties and thermogravimetric analysis of all the prepared materials are characterized in detail, and the results reveal that a series of uniformed mesopore structure hybrid materials has been achieved. The mesoporous material Eu(BTA Si SBA-15) 3 (BTA Si GaN) has better luminescence intensity, higher quantum efficiency, and longer lifetime than Eu(TAA Si SBA-15) 3 (TAA Si GaN). While the nanocomposite Tb(TAA Si SBA-15) 3 (TAA Si GaN) revealed the strongest characteristic emission of Tb 3+ ions than Tb(BTA Si SBA-15) 3 (BTA Si GaN), the excellent luminescent properties and thermal stability enable the hybrid mesoporous material to have potential applications in optical field.
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高影响因子
DALTON TRANSACTIONS
·
2014
·Vol. 43
·期 22
·8461-8468
·
IF 4.097
Zhuqing Wang,Min Wang,Genhua Wu,Dayu Wu,Aiguo Wu
SBA-15 functionalized with N-[3-(trimethoxysilyl)propyl]ethylene-diamine (TPED) was synthesized and used for the colorimetric detection of Cu2+ and removal of heavy metal ions in aqueous solutions. Compared to free SBA-15, the adsorption ability of diamine-functionalized SBA-15 (depicted as SBA-TPED) increased remarkably, the maximum adsorption capacity of SBA-TPED for Cu2+, Pb2+ and Zn2+ was 27.22, 96.43 and 12.16 mg g−1, respectively. Furthermore, SBA-TPED exhibits high selectivity for Cu2+ with the relative selectivity coefficient of SBA-TPED for Cu2+/Pb2+ being over 10 and for Cu2+/Zn2+ being over 60. The naked-eye detection limit of SBA-TPED for Cu2+ is 0.95 ppm, and the determination of Cu2+ in real water samples also displays satisfactory results. Moreover, SBA-TPED possesses fast kinetics for removing Cu2+ with a saturation time of less than 30 min, and can be regenerated by simple acid treatment.
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高影响因子
SOLID STATE SCIENCES
·
2015
·
IF 1.839
Yan-Jing Gu,Bing Yan
A series of organic–inorganic hybrid materials were prepared by linking lanthanide (Eu 3+ , Sm 3+ ) complexes to mesoporous SBA-15/SBA-16 through 8-hydroxybenz[de]anthracen-7-one modified silane (HBA-Si) as linker. The physical characterizations of these hybrids revealed that they all have high surface area, uniformity in mesostructure. The luminescence properties of these covalently bonded materials (denoted as Ln(HBA-SBA-15) 3 phen and Ln(HBA-SBA-16) 3 phen) were compared with ternary complexes (Ln(HBA) 3 phen) (Ln = Eu, Sm). Eu(HBA-SBA-15(16)) 3 phen hybrids display better thermal stability, whose luminescent lifetimes and quantum efficiencies were matchable with those of Eu(HBA) 3 phen complex in spite of its much lower effective condensation of Eu 3+ species. In addition, the luminescent performance of functionalized SBA-15 hybrids was more favorable than that of functionalized SBA-16 hybrids, revealing that SBA-15 was a better host material for lanthanide complex than mesoporous silica SBA-16.
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RSC Advances
·
2014
·Vol. 4
·期 71
·37470-37478
·
IF 3.708
Jianxiong Xu,Weiwei Liu,Yunfei Yu,Jingjing Du,Na Li,Lijian Xu
A simple synthesis of mesoporous silica nanoparticles with cubic Pmn pore structure (SBA-1) and controlled pore size is reported. The synthesis of mesoporous silica nanoparticles is achieved by employing organic mesomorphous complexes of polyelectrolyte (poly(acrylic acid)) and cationic surfactant (hexadecyl pyridinium chloride) as template, and tetrapropoxysilane as silica source. It is found that the pore size of the synthesized mesoporous silica nanoparticles can be tuned by the incorporation of 1,3,5-trimethylbenzene. By adjusting the amount of 1,3,5-trimethylbenzene in the synthesis, a series of silica nanoparticles with controlled pore size ranging from 2.5 nm to 5.3 nm is obtained. The adsorption properties of the mesoporous silica nanoparticles with different pore size against lysozyme are compared. The results show that mesoporous silica nanoparticles with proper pore size and well ordered pore structure benefit the adsorption and exhibit a low leaching rate.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2013
·
IF 3.535
Huimin Li,Qi Zheng,Jun Luo,Zhixuan Cheng,Jiaqiang Xu
This paper employed a measurement of quartz crystal microbalance (QCM) to investigate the effects of mesopore structures and amount of organic loadings of fluoroalcohol derivatives/SBA-15 (a kind of ordered mesoporous silica sieve) hybrids on the sensing behavior of nerve agent simulant DMMP (dimethyl methylphosphonate). The meso-structure and functional groups of silica-based mesoporous hybrids were examined by SAXS, TEM , N 2 adsorption–desorption isotherms and elemental analysis . The results show that much higher response value and sensitivity are achieved when the hybrid materials have relative higher pore volume and surface area. However, this effect only appears when the mesoporous hybrids have well-ordered porous structure , indicating that ordered meso-structure is critical in fabricating high-performance DMMP sensors. The reason is likely that the ordered meso-structure not only provides a larger number of contactable HFIP groups, but also facilitates molecules diffusion in porous structure. On the other hand, the specific interaction between HFIP/SBA-15 hybrids and DMMP vapor is greatly enhanced as the amount of fluoroalcohol derivatives increases. Therefore, the amount of organic functional groups incorporated plays an important role in determining the selectivity of sensors.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2014
·
IF 2.235
Jun Xiong,Wenshuai Zhu,Wenjing Ding,Lei Yang,Yanhong Chao,Hongping Li,Fengxia Zhu,Huaming Li
A heterogeneous catalyst system was synthesized by immobilizing phosphotungstic acid on ionic liquid-modified mesoporous silica SBA-15 and applied in oxidative desulfurization. Structure and properties of catalyst were characterized by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), N2 adsorption–desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and the contact angle. The results demonstrated that the synthesized catalyst possessed ordered mesopore structure and high special surface area. Due to the introduction of imidazole-based ionic liquid, the catalyst exhibited good wettability for model oil, which had significant contribution to desulfurization activity. Both DBT and 4,6-DMDBT could be removed completely at mild conditions (60 °C, 40 min). The removal of BT also can reach 81.3% within 60 min. Furthermore, the catalyst was recovered and reused in four reaction runs with a slight decrease in activity.
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高影响因子
Catalysis Science & Technology
·
2014
·Vol. 4
·期 11
·4010-4019
·
IF 4.76
Chao Lin,Kai Tao,Hongbo Yu,Dayin Hua,Shenghu Zhou
Molybdenum-doped mesoporous SBA-15, mesoporous SBA-15-supported MoO3/SBA-15, and traditional silica-supported MoO3/SiO2 were successfully synthesized. Various techniques, such as XRD, TEM, BET, UV-DRS, Raman, XPS and IR, were used to characterize the above obtained materials. The studies of TEM, XRD and BET confirmed that the highly ordered mesoporous structure of SBA-15 was maintained in the doped Mo-SBA-15 whereas supported MoO3/SBA-15 showed a significant reduction in surface area due to the deposition of MoO3 nanoparticles into the SBA-15 channels. XPS studies revealed that a high concentration of Mo5+ species appeared in doped Mo-SBA-15 whereas supported MoO3/SBA-15 and MoO3/SiO2 only contained Mo6+ species. The metathesis reaction of 1-butene and ethene to propene was used to evaluate the catalytic performance of Mo-containing materials. The doped Mo-SBA-15 illustrated a superior catalytic performance over the supported MoO3/SBA-15 and MoO3/SiO2 catalysts. The enhancement of catalytic performance for doped Mo-SBA-15 was assigned to the incorporation of Mo species into the SBA-15 framework. Due to the doping method, Mo-SBA-15 exhibited a well-ordered mesoporous structure, a high surface area, and a high concentration of Mo5+ species, which is beneficial to the catalytic performance for metathesis reactions.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2016
·
IF 3.652
Qiang Lu,Zhi-bo Zhang,Xiao-ning Ye,Wen-tao Li,Bin Hu,Chang-qing Dong,Yong-ping Yang
A new technique was proposed to selectively produce 4-ethyl guaiacol (4-EG), a valuable phenolic compound, via low-temperature catalytic fast pyrolysis of softwood biomass using the Pd/SBA-15 catalyst. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to compare 4-EG production from three biomass materials with different lignin types (pine wood, poplar wood and bagasse) and two catalytic patterns (in-situ and ex-situ). Further experiments were performed to reveal 4-EG formation affected by the pyrolysis temperature, catalyst-to-biomass ratio and Pd content of the Pd/SBA-15 catalyst. The results indicated that 4-EG could be selectively produced from pine wood by the in-situ catalytic pattern. 4-EG was a very minor pyrolytic product in the non-catalytic process, while it could be selectively produced in the catalytic process, via the decomposition and hydrogenation of lignin. Our results suggested that several holocellulose-derived pyrolytic products could serve as the hydrogen-donors (H-donors) for the formation of 4-EG, without any extra H-donors. The highest 4-EG yield of 18.44 mg/g from pine wood was obtained at the temperature of 350 °C and catalyst-to-biomass ratio of 2, and the corresponding peak area% (calculated by GC/MS) was 38.34%.
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ChemCatChem
·
2017
·Vol. 9
·期 7
·1337-1342
·
IF 4.803
Kaixuan Yang,Xiao Chen,Lei Wang,Liangliang Zhang,Shaohua Jin,Changhai Liang
Graphical Vapor trail : Metal silicide (Pd 2 Si, Ni 2 Si, CoSi, Fe x Si, and Cu 6.69 Si) catalysts supported by SBA-15 are prepared by chemical vapor deposition. Of the SBA-15-supported metal silicide catalysts, Ni 2 Si/SBA-15 presents a modest activity, notable selectivity to styrene (>90 %), and high stability in the selective hydrogenation of phenylacetylene. Metal silicide (Pd 2 Si, Ni 2 Si, CoSi, Fe x Si, and Cu 6.69 Si) catalysts supported by SBA-15 have been prepared by a chemical vapor deposition method under a H 2 atmosphere using (CH 3 ) 2 SiCl 2 as the Si source. Of the SBA-15-supported metal silicide catalysts, Ni 2 Si/SBA-15 presented a modest activity, notable selectivity to styrene (>90 %), and high stability with respect to the selective hydrogenation of phenylacetylene, which is attributed to the active-site isolation and electron transfer in the silicide. Furthermore, Ni 2 Si/SBA-15 also has a high selectivity to diphenylacetylene and 1,4-butynediol, which demonstrates that Ni 2 Si/SBA-15 is a promising, low-cost catalyst alternative to noble-metal catalysts as a selective hydrogenation catalyst.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 26
·11776-11782
·
IF 2.7
Yuwei Yan,Hongyan Li,Songnan Li,Jiawei Zhang,Jingxiang Zhao,Qinghai Cai
Copper, iron–chloride ionic liquids (ILs) were immobilized on SBA-15 via N-methylimidazole grafting with C–Cl in chloropropylsilane pre-anchored on SBA-15, followed by FeCl3 and CuCl2 coordination to imidazolium chloride to generate a double metal IL-supported mesoporous composite (SIL-CuFe). The prepared composite exhibited an effective catalytic performance for the solvent-free oxidation of styrene to benzaldehdye (BzH) with H2O2 oxidant, offering 51% conversion, a turnover number (TON) of 330.5 mol molFe+Cu−1, and a selectivity of 71% at a reaction temperature of 70 °C. The composite catalyst can be easily recovered and effectively reused without a significant loss in activity and selectivity. The quenching experiments by adding tert-butanol (TBA), 1,4-benzoquinone (p-BQ) and L-histidine (L-HIS) in the reaction system were conducted to identify the type of reactive O species, specifically ˙OH, ˙O2−, and 1O2, produced by catalyst activation with H2O2 and played a main role in the oxidation. The reaction mechanism of the oxidation process is also proposed.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2018
·Vol. 316
·期 1
·49-59
·
IF 1.181
Ji Guojia,Zhu Guiru,Wang Xingjun,Wei Yulin,Wu Hui,Yuan Junsheng,Gao Congjie
In order to reduce the loss of particles during the cycling operation, a technology for the granulation of short channel SBA-15 adsorbent was developed. The adsorption behavior of obtained granules was studied under various factors including initial pH value, contact time in different initial concentration and acid stability by batch experiments. A continuous packed column loaded with granules was performed to remove U(VI) from aqueous solution. The uranium concentration was highly enriched than feed solution. The granules packed in column exhibited excellent reusability through cycling test. The result showed promising application prospect in the uranium extraction from aqueous solution.
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