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RSC Advances · 2016 ·Vol. 6 ·期 73 ·68695-68704 · IF 3.289

The removal of aqueous uranium by SBA-15 modified with phosphoramide: a combined experimental and DFT study

Yiming Ren,Ruizhu Yang,Lang Shao,Hao Tang,Shaofei Wang,Jianlong Zhao,Jingrong Zhong,Chuipeng Kong

Phosphoramide-modified ordered mesoporous silica (SBA-DEPA) materials were prepared via a two-step process involving: (1) the synthesis of phosphoramide via amidation of phosphoryl chloride with a primary amine and (2) modification of the phosphoramide onto SBA-15. The successful preparation was confirmed by FT-IR and NMR spectroscopy. As indicated by the ICP-AES and XRF analysis results, the phosphoramide group has a grafting ratio as high as 12.5%. The morphological information and N2 adsorption–desorption technique proved the highly ordered structure and large specific area of the material, respectively. An excellent performance for uranium sorption was found with a loading maximum of 311.6 mg g−1, a marked promotion relative to unmodified SBA-15. A strong pH and CO2 dependence suggested that near neutral conditions favored the maximum uranium sorption. To our surprise, the sorption took only 5 min to reach a 90% capacity and 20 min for equilibrium, which is extraordinary when compared to many other sorbent materials. The ionic strength partially influences the sorption, which indicates outer and inner sphere sorption both play parts in the process. A sorption capacity of over 90% of the original indicates the excellent reproducibility of SBA-DEPA. DFT calculations based on cluster models suggested a ‘tri-dentate-like’ structure for the uranyl-surface binding site, which may explain the excellent sorption ability of this material.

研究领域: 环境科学 · 材料科学
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY · 2024 · IF 3.1

Recombinant Esterase (BaCEm) Immobilized on Polyethyleneimine-Impregnated Mesoporous Silica SBA-15 Exhibits Outstanding Catalytic Performance

Zhang Hongjun,Li Yichao,Wei Litian,Wang Zhao,Zhang Yinjun

A recombinant esterase, BaCE m , derived from Bacillus aryabhattai and heterologously expressed in Escherichia coli , was successfully immobilized on polyethyleneimine-impregnated mesoporous silica SBA-15. This immobilization utilized glutaraldehyde as a crosslinker. Optimal conditions were established with a PEI/SBA-15 ratio of 25% (w/w), a pH of 7.5, and a glutaraldehyde concentration of 0.5% (w/w), resulting in a loading capacity of 76.4 mg/g, a recovery activity of 43.5%, and a specific activity of 7917 U/g for BaCE m . The immobilized BaCE m demonstrated high enantioselectivity, with an “E” value of 203.92, in the resolution assay of ( R , S )-ethyl indoline-2-carboxylate. Notably, the immobilized enzyme, compared to its free counterpart, exhibited enhanced thermostability, maintaining 95.4% of its activity after 3 h at 30 °C. It also showed significant tolerance to organic solvents, retaining 48.4% and 28.7% residual activity in 10% v/v acetonitrile and acetone, respectively. Moreover, its storage stability was confirmed, with 68.5% residual activity preserved after 30 days at 4 °C. Remarkably, the immobilized BaCE m retained 58.1% of its activity after 10 reuse cycles, underscoring the potential of polyethyleneimine-impregnated mesoporous silica SBA-15 as an effective support for enzyme immobilization, promising for industrial applications. Graphical Abstract

CAS / MDL: 111-30-8 2635-84-9
研究领域: 生物化学 · 酶工程 · 材料科学
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CHINESE CHEMICAL LETTERS · 2011 ·Vol. 22 ·期 12 ·1497-1500 · IF 0.775

Phase behavior of binary system of bromobenzene–chlorobenzene confined in SBA-15 and MCM-41

Xiao Zheng Lan,Hai Rong Pei,Chuan Xian Cheng

Phase behavior of binary system of bromobenzene–chlorobenzene (C 6 H 5 Br–C 6 H 5 Cl) confined in SBA-15 and MCM-41 (pore diameter 8   nm, 3.8   nm, respectively) has been investigated by means of differential scanning calorimetry (DSC). Phase diagram of C 6 H 5 Br–C 6 H 5 Cl system confined in SBA-15 is a type of the complete miscible both in liquid and solid state, the same phase behavior as the bulk system. However, the phase diagram comprises only one boundary line, which is shifted down 22–36   K with respect to the bulk system. C 6 H 5 Br, C 6 H 5 Cl or the mixture within nanopores of MCM-41 is nonfreezing. The different phase behavior of the system confined in SBA-15 and MCM-41 is thought mainly due to the relative size of pore to molecule.

研究领域: 物理化学 · 材料科学 · 纳米科技 · 热力学
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Inorganic Chemistry Frontiers · 2019 ·Vol. 6 ·期 7 ·1799-1812 · IF 5.934

Selective hydrogenation of CO2 over a Ce promoted Cu-based catalyst confined by SBA-15

Xiaosong Hu,Chaoyue Zhao,Qingxin Guan,Xin Hu,Wei Li,Jun Chen

The chemical transformation of CO2 not only mitigates CO2 released into the atmosphere but also produces fuels and chemicals with important additional value. The activation of stable CO2 molecules is the key difficulty for the efficient conversion of CO2. Herein, we designed a ternary catalyst containing Cu, ZnO, and CeOx and dispersed them in SBA-15 using incipient wetness impregnation. Interestingly, the catalytic performances were improved greatly when the related active components were dispersed inside and outside the pore channels of SBA-15 using the incipient wetness impregnation method. Methanol and CO were controllably produced on the interface of Cu and metal oxides (ZnO and CeOx) due to the synergistic effects between the three active components. The metal oxides play a more important role in CO2 conversion as well as the product selectivity compared to Cu. CeO2 is more efficient than ZnO in promoting the dispersion of Cu nanoparticles and methanol generation. The suitable pore channels of SBA-15 promote the mass transfer and heat transfer while the high specific surface area is favorable to the dispersion of active components, which will facilitate the production of methanol and CO. After continuous hydrogenation evaluation for 100 h, the catalytic performance of the catalyst was still very stable. This work provides a viable strategy to prepare a supported catalyst with highly dispersed active sites, and the catalyst exhibits an efficient catalytic effect on producing methanol and CO.

研究领域: 化学工程 · 催化科学
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RENEWABLE ENERGY · 2022 · IF 8.634

Hierarchical gallium-modified ZSM-5@SBA-15 for the catalytic pyrolysis of biomass into hydrocarbons

Xiaocui Wei,Yanan Liu,Yang Cao,Jin Li,Xianghao Meng,Zhao Zhang,Zhongyi Jiang

The catalytic pyrolysis of biomass is a sustainable approach for biofuel production, contributing to replacing fossil resources with renewable resources . The ZSM-5 zeolite remains an attractive catalyst in the catalytic pyrolysis of biomass, and how to reduce the product diffusion resistance and regulate the surface acidity of ZSM-5 should be explored more deeply. Herein, a hierarchical gallium-modified ZSM-5@SBA-15 catalyst is fabricated through coating a mesoporous layered SBA-15 shell on a hollow ZSM-5 core with gallium modified on the surface, which is effective for increasing hydrocarbon production during the catalytic pyrolysis of biomass process. The synergistic effect of hollowness, mesoporosity, and activity in the hierarchical gallium-modified ZSM-5@SBA-15 catalysts is found to affect the yield and quality of bio-oil. Accordingly, the hierarchical gallium-modified ZSM-5@SBA-15 catalyst with 11 wt% Ga loading exhibits a superior deoxygenation ability, and the relative content of hydrocarbons in bio-oil reach to 49.76 area% which is much higher than that of ZSM-5 (35.30 area%). Furthermore, a possible catalytic pyrolysis mechanism of biomass was also proposed to clarify the potential application of hierarchical gallium-modified ZSM-5@SBA-15 catalysts.

CAS / MDL: 78-10-4
研究领域: 能源科学 · 催化化学
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JOURNAL OF POROUS MATERIALS · 2015 ·Vol. 23 ·期 2 ·529-537 · IF 1.108

Rapid synthesis of tunable-structured short-pore SBA-15 and its application on CO2 capture

Ma Beibei,Zhuang Linzhou,Chen Shuixia

The well-ordered hexagonal short-pore SBA-15 (SSBA-15) has been successfully synthesized via an energy-efficient process under the microwave-hydrothermal condition, in which the formation duration [stirring duration (ripening step) and microwave-hydrothermal treatment duration (aging step)] has been greatly decreased from 48 h for conventional hydrothermal treatment to <2 h. The extension of the ripening duration led to the evidently improved uniformity and regularity of particles while the increase of aging duration resulted in less intrawall pores and more structural mesopores. The optimal condition to get highly ordered SSBA-15 in this work was the duration of 2 h for both steps, and the SSBA-15 obtained was composed of cuboid-like particles, whose pore length was ca. 450 ± 50 nm and pore size was around 10 nm. The SSBA-15 was modified with different amine agents to prepare solid amine adsorbent, the obtained adsorbents showed considerable CO 2 adsorption ability, indicating that this fast-prepared SSBA-15 can be a promising support of CO 2 adsorbents.

CAS / MDL: 124-18-5 78-10-4
研究领域: 材料科学 · 环境科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2018 ·Vol. 316 ·期 1 ·49-59 · IF 1.181

Granulation of short channel SBA-15 adsorbent and application for the removal of U(VI) by packed column

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.

CAS / MDL: 9002-86-2
研究领域: 材料科学 · 环境科学 · 核化学
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SOLID STATE SCIENCES · 2015 · IF 1.839

Eu3+/Sm3+ hybrids based with 8-hydroxybenz[de]anthracen-7-one organically modified mesoporous silica SBA-15/16

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.

研究领域: 材料科学 · 化学
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BIOORGANIC & MEDICINAL CHEMISTRY · 2024 · IF 3.3

Structure optimization of Cmpd-15 as negative allosteric modulators for the β2-adrenergic receptor

Xue Guo,Zhijie Luo,Ying Qi,Xiaoyuan Hei,Xin Zhang,Xuli Cao,Mingcheng Qian,Shuai Zhao,Yanan Hou,Xin Chen

19 derivatives of 1-benzyl-3-arylpyrazole-5-carboxamides ( H 1 - H 19 ) and 5 derivatives of 1-benzyl-5-arylpyrazole-3-carboxamides ( J 1 - J 5 ) have been designed and synthesized as potential negative allosteric modulators (NAMs) for the β 2 -adrenergic receptor (β 2 AR). The new pyrazole derivatives were screened on the classic G-protein dependent signaling pathway at β 2 AR. The majority of 1-benzyl-3-aryl-pyrazole-5-carboxamide derivatives show more potent allosteric antagonistic activity against β 2 AR than Cmpd-15, the first reported β 2 AR NAM. However, the 1-benzyl-5-arylpyrazole-3-carboxamide derivatives exhibit very poor or even no allosteric antagonistic activity for β 2 AR. Furthermore, the active pyrazole derivatives have relative better drug-like profiles than Cmpd-15. Taken together, we discovered a series of derivatives of 1-benzyl-3-arylpyrazole-5-carboxamides as a novel scaffold of β 2 AR NAM.

研究领域: 药理学 · 分子生物学 · 药物化学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2021 · IF 3.171

Coupling effect of bifunctional ZnCe@SBA-15 catalyst in 1,3-butadiene production from bioethanol

Zheng Wang,Sijia Li,Shengping Wang,Jiaxu Liu,Yujun Zhao,Xinbin Ma

A series of bifunctional ZnCe@SBA-15 catalysts with different Zn/Ce ratios were prepared by a solid-state grinding strategy and used in the conversion of ethanol to 1,3-butadiene (ETB). For the supported metal oxides, ZnO serves as the active sites for the dehydrogenation of ethanol, and CeO 2 promotes the aldol-condensation reaction. Based on the results of Py-FTIR and NH 3 -TPD, it suggests that the yield of 1,3-butadiene is positively correlated with the number of weak Lewis acid sites on the catalyst surface, given their benefit for aldol-condensation reactions. The catalyst with an optimal Zn/Ce ratio of about 1:5 has the highest concentration of weak Lewis acid. Coupling with the ZnO sites, it contributes to a 98.4% conversion of ethanol and a 45.2% selective of 1,3-butadiene under relatively mild reaction conditions (375 °C, 101.325 kPa, and 0.54 h −1 ).

CAS / MDL: 10196-18-6
研究领域: 催化化学 · 可再生资源化学
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FUEL · 2016 · IF 3.611

Catalytic adsorptive desulfurization of model diesel fuel using TiO2/SBA-15 under mild conditions

Xiaoling Ren,Guang Miao,Zhiyong Xiao,Feiyan Ye,Zhong Li,Haihui Wang,Jing Xiao

This study investigates catalytic adsorptive desulfurization (CADS) of model diesel fuel using TiO 2 /SBA-15 under mild conditions. The TiO 2 /SBA-15 was prepared by a facile incipient wetness impregnation method and characterized by N 2 adsorption and X-ray diffraction. The CADS referred to ADS performance were evaluated in a batch reactor. High desulfurization uptake of 12.7   mg/g was achieved at low sulfur concentration of 15   ppmw-S by TiO 2 /SBA-15 under CADS, which was two-magnitude higher than that under ADS without the in-situ catalytic oxidation of dibenzothiophene. Kinetic results suggested that the CADS equilibrium over TiO 2 /SBA-15 was reached fast in 0.5   h. In the CADS–TiO 2 /SBA-15 system, the TiO 2 loading, cumene hydroperoxide/dibenzothiophene ratio and CADS temperature were optimized to be 10   wt%, 2, and 35   °C, respectively. Furthermore, desulfurization tests in 5 consecutive CADS-regeneration cycles suggested that the bi-functional TiO 2 /SBA-15 can be regenerated by acetonitrile washing followed with oxidative air treatment. The CADS–TiO 2 /SBA-15 mechanism went through the oxidation of DBT to oxidized DBTO 2 over TiO 2 /SBA-15 by cumene hydroperoxide, which was followed by the adsorption of the oxidized DBTO 2 over TiO 2 /SBA-15. The superior desulfurization uptake at low sulfur concentration range, fast adsorption kinetics, excellent regenerability, operation at mild conditions, and facile and low-cost adsorbent synthesis make the CADS–TiO 2 /SBA-15 system an effective and economic desulfurization approach for ultra-clean fuel production.

CAS / MDL: 80-15-9
研究领域: 化学工程 · 材料科学 · 环境科学
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Journal of Materials Chemistry A · 2015 ·Vol. 3 ·期 18 ·9789-9798 · IF 7.443

Efficient removal of lead from highly acidic wastewater by periodic ion imprinted mesoporous SBA-15 organosilica combining metal coordination and co-condensation

Rong He,Weiming Li,Dayi Deng,Wensen Chen,He Li,Chaohai Wei,Youwen Tang

In order to develop a highly efficient method for direct removal of lead from acidic wastewater (pH 2.0), we introduce a novel highly ordered Pb2+ imprinted mesoporous silica (PbIMS) SBA-15 combining co-condensation and functionalized iminodiacetic acid (IDA). Fourier transform infrared spectroscopy (FTIR) and energy-dispersive X-ray (EDX) analysis provided the components of PbIMS. The solid-state 13C NMR spectra demonstrated the successful embedment of IDA in the mesoporous silica. Furthermore, X-ray photoelectron spectroscopy (XPS) analysis confirmed that Pb2+ was coordinated by the N atom and carboxyl O atom of IDA. The results of transmission electron microscopy (TEM), small angle X-ray diffraction (XRD) and N2 adsorption–desorption measurement confirmed that the PbIMS preserved a highly ordered hexagonal P6mm mesostructure. The Brunauer–Emmett–Teller (BET) surface area was 762 m2 g−1. The saturated adsorption capacity of PbIMS toward lead reached up to 103 mg g−1 at pH 2.0, which was greater even than that of the simply modified SBA-15 by IDA at pH 4.5. The values of selectivity coefficients of PbIMS for six competing metal ions ranged from 67.3 to 12.7. The adsorption of Pb2+ reached equilibrium within 7 min. The adsorption efficiency of PbIMS was above 93% after six extraction–stripping cycles. The investigation conducted with real samples of strongly acidic wastewater demonstrated the ability of PbIMS to efficiently remove lead below the current China regulatory standard.

研究领域: 环境科学 · 材料科学
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