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Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要： The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co3O4–CeO2 composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co3+/Co2+ and Ce4+/Ce3+ redox pairs, than bulk CeO2 and/or Co3O4. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co3O4–CeO2. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词： Co3O4–CeO2 composite oxides     cyclohexanone     cyclohexanol     ultrasonic-assisted co-precipitation     selective oxidation     solvent-free    

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Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporouscomposite

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 264-273 doi: 10.1007/s11705-010-1007-6

摘要： Adsorption of pure CO and N and separation of CO /N mixture in MFI zeolite and MFI/MCM-41 micro/mesoporous composite have been studied by using atomistic simulations. Fully atomistic models of MFI and MFI/MCM-41 are constructed and characterized. A bimodal pore size distribution is observed in MFI/MCM-41 from simulated small- and broad-angle X-ray diffraction patterns. The density of MFI/MCM-41 is lower than MFI, while its free volume and specific surface area are greater than MFI due to the presence of mesopores. CO is preferentially adsorbed than N , and thus, the loading and isosteric heat of CO are greater than N in both MFI and MFI/MCM-41. CO isotherm in MFI/MCM-41 is similar to that in MFI at low pressures, but resembles that in MCM-41 at high pressures. N shows similar amount of loading in MFI, MCM-41 and MFI/MCM-41. The selectivity of CO over N in the three adsorbents decreases in the order of MFI>MFI/MCM-41>MCM-41. With increasing pressure, the selectivity increases in MFI and MFI/MCM-41, but decreases in MCM-41. The self-diffusivity of CO and N in MFI decreases as loading increases, while in MFI/MCM-41, it first increases and then drops.

关键词： adsorption     diffusion     CO2     flue gas     zeolite     micro/mesoporous composite    

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Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2037-2049 doi: 10.1007/s11705-023-2358-0

摘要： Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years, it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic particles. Herein, we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide. The prepared materials exhibited excellent properties for U(VI) ions removal from aqueous solutions under various conditions. The experimental data show that the U(VI) adsorption features fast adsorption kinetics, high adsorption capacity and ideal selectivity toward U(VI). The adsorption process is of spontaneous and endothermic nature and ionic strength independence, and the adsorbents can be easily regenerated by acid treatment. Compared to pristine KIT-6, the introduction of magnetism does not reduce the efficiency of the material to remove U(VI) while exerting its role as a recovery adsorbent. The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.

关键词： magnetic nanoparticle     3D mesoporous silica     amino functionalization     adsorption of U(VI)     acid resistance    

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Facile controlled synthesis of hierarchically structured mesoporous Li4Ti5O12/C/rGO composites as high-performance

Cehuang FU, Shuiyun SHEN, Ruofei WU, Xiaohui YAN, Guofeng XIA, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第4期   页码 607-612 doi: 10.1007/s11708-021-0798-0

摘要： In this paper, a facile strategy is proposed to controllably synthesize mesoporous Li4Ti5O12/C nanocomposite embedded in graphene matrix as lithium-ion battery anode via the co-assembly of Li4Ti5O12 (LTO) precursor, GO, and phenolic resin. The obtained composites, which consists of a LTO core, a phenolic-resin-based carbon shell, and a porous frame constructed by rGO, can be denoted as LTO/C/rGO and presents a hierarchical structure. Owing to the advantages of the hierarchical structure, including a high surface area and a high electric conductivity, the mesoporous LTO/C/rGO composite exhibits a greatly improved rate capability as the anode material in contrast to the conventional LTO electrode.

关键词： Li4Ti5O12     phenolic-resin-based carbon     mesoporous composite     graphene    

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Review on research and application of mesoporous transitional metal oxides in water treatment

Minghao SUI, Lei SHE

《环境科学与工程前沿（英文）》 2013年 第7卷 第6期   页码 795-802 doi: 10.1007/s11783-013-0521-4

摘要： This paper reviews the application of mesoporous transitional metal oxides in water treatment on basis of the catalysis and adsorption. Mesoporous transitional metal oxides are characterized by their intrinsic features, such as a high surface area, a highly ordered array of unidimensional pores with a very narrow pore size distribution, and highly dispersed active sites. Finally, the suggestions of further study on application are proposed.

关键词： mesoporous materials     transitional metal oxides     catalysis     adsorption     water treatment    

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Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1581-1592 doi: 10.1007/s11705-023-2327-7

摘要： Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al2O3, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including SO4•‒, OH •, and O2•‒) and singlet oxygen (1O2) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al2O3 promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

关键词： Cu–Al bimetallic oxides     mesoporous silica spheres     peroxydisulfate     bisphenol A    

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Synthesis of ordered cerium-doped cubic mesoporous silica using long-chain ionic liquid as template

YUE Hongxia, ZHAO Hongmei, LIU Longjiang, WANG Siping, Ruan Qiong, WANG Tongwen

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 135-139 doi: 10.1007/s11705-008-0031-2

摘要： The long-chain ionic liquid 1-hexadecyl-3-methylimidazolium chloride (CmimCl) was used as a template to prepare cerium-doped MCM-48 materials in basic medium by a hydrothermal synthesis procedure. The effect of the amount of Ce salt and CmimCl/Si on the synthesis were discussed in detail. This mesoporous material exhibits a pore architecture which is cubic 3 gyroid and possesses a large surface area and a narrow pore distribution. Cerium in calcined porous framework exists in the form of well-dispersed tetrahedral coordination. The CmimCl shows a high tendency toward self-aggregation that allows the formation of the cerium-doped gyroid mesostructure by using the appropriate amount of Ce salt.

关键词： mesoporous     CmimCl/Si     tendency     mesostructure     synthesis procedure    

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Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 95-103 doi: 10.1007/s11705-014-1405-2

摘要： Titanium-containing mesoporous materials (Ti-MCM-41) were obtained by hydrothermal synthesis. Such materials are active catalysts for the transesterification of dimethyl oxalate and phenol to produce diphenyl oxalate. To understand the role of the Ti in the catalytic process, Ti-MCM-41 samples with different Si/Ti ratios (from 5 to 100) were prepared and the samples were analyzed by Fourier transform infrared spectroscopy, UV-visible spectroscopy, and ammonia temperature programmed desorption. It was concluded that the Ti is incorporated into the framework of the MCM-41 and formed weak Lewis acid sites. In addition, the number of Ti(IV) sites increased as the amount of titanium increased. X-ray powder diffraction, N adsorption-desorption and transmission electron microscopy results showed that the Ti-MCM-41 samples have a hexagonal arrangement of mono-dimensional pores. A large number of Ti(IV) sites coupled with the mesoporous structure and large pore diameters are favorable for the transesterification catalytic properties of Ti-MCM-41.

关键词： Ti-MCM-41     mesoporous molecular sieve     acid sites     transesterification     hydrothermal synthesis    

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The modification of titanium in mesoporous silica for Co-based Fischer–Tropsch catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1224-1236 doi: 10.1007/s11705-022-2139-1

摘要： Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a one-pot hydrothermal crystallization method. The characterization including powder X-ray diffraction, Brunauer–Emmett–Teller, transmission electron microscope, temperature-programmed reduction, temperature-programmed desorption, Fourier transform infrared and ultraviolet-visible-near infrared spectrometer was performed to explore the physical and chemical structures of both the supports and the catalysts. The results showed that titanium was successfully incorporated into the mesoporous silica framework with a limited amount of titanium (Si/Ti > 20), and the mesoporous structure was retained. However, the increased titanium content inevitably resulted in the formation of anatase TiO 2 particles on the support surface. The increased incorporated titanium strengthened the interactions between cobalt species and supports, which was favorable for the cobalt species dispersion, despite the limited cobalt oxide reducibility. The enhanced metal-support interactions were beneficial for the CO/H2 ratio at the active cobalt sites, which facilitated the formation of more C5+ hydrocarbons. This study provides a promising method for support modification with incorporated-heteroatoms for the rational development of Fischer–Tropsch catalysts.

关键词： Fischer–Tropsch synthesis     titanium incorporation     mesoporous silica     metal-support interactions     C5+ selectivity    

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Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 329-338 doi: 10.1007/s11705-018-1741-8

摘要：

Copper nanoparticles-decorated polyaniline-derived mesoporous carbon that can serve as noble metal-free electrocatalyst for the hydrazine oxidation reaction (HzOR) is synthesized via a facile synthetic route. The material exhibits excellent electrocatalytic activity toward HzOR with low overpotential and high current density. The material also remains stable during the electrocatalytic reaction for long time. Its good electrocatalytic performance makes this material a promising alternative to conventional noble metal-based catalysts (e.g., Pt) that are commonly used in HzOR-based fuel cells.

关键词： copper nanoparticles     mesoporous carbon     noble metal-free electrocatalyst     hydrazine oxidation reaction     polyaniline    

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Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1198-1210 doi: 10.1007/s11705-021-2133-z

摘要： Sulfonic acid functionalized mesoporous silica based solid acid catalysts with different morphology were designed and fabricated. The synthesized materials were characterized by various physicochemical and spectroscopic techniques like scanning electron microscope-energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller surface area, thermogravimetric analysis and n-butylamine acidity. The shape of catalysts particles plays an important role in its activity. The sulfonic acid functionalized mesoporous silica catalysts of spherical shape and the cube shape were assessed for catalytic activity in biodiesel production. The catalytic biodiesel production reaction over the catalysts were studied by esterification of free fatty acid, oleic acid with methanol. The effect of various reaction parameters such as catalyst concentration, acid/alcohol molar ratio, catalyst amount, reaction temperature and reaction time on catalytic activity were investigated to optimize the conditions for maximum conversion. It was sulfonated cubic shape mesoporous silica which exhibited better activity as compared to the spherical shape silica catalysts. Additionally, the catalyst was regenerated and reused up to three cycles without any significant loss in activity. The present catalysts exhibit superior performance in biodiesel production and it can be used for the several biodiesel feedstock’s that are rich in free fatty acids.

关键词： solid acid catalyst     mesoporous silica     sulfonic acid     biodiesel     esterification     oleic acid    

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Enhancing the photoelectrochemical performance of p-silicon through TiO coating decorated with mesoporous

《能源前沿（英文）》 2021年 第15卷 第3期   页码 772-780 doi: 10.1007/s11708-021-0783-7

摘要： MoS2 is a promising electrocatalyst for hydrogen evolution reaction and a good candidate for cocatalyst to enhance the photoelectrochemical (PEC) performance of Si-based photoelectrode in aqueous electrolytes. The main challenge lies in the optimization of the microstructure of MoS2, to improve its catalytic activity and to construct a mechanically and chemically stable cocatalyst/Si photocathode. In this paper, a highly-ordered mesoporous MoS2 was synthesized and decorated onto a TiO2 protected p-silicon substrate. An additional TiO2 necking was introduced to strengthen the bonding between the MoS2 particles and the TiO2 layer. This meso-MoS2/TiO2/p-Si hybrid photocathode exhibited significantly enhanced PEC performance, where an onset potential of +0.06 V (versus RHE) and a current density of −1.8 mA/cm2 at 0 V (versus RHE) with a Faradaic efficiency close to 100% was achieved in 0.5 mol/L H2SO4. Additionally, this meso-MoS2/TiO2/p-Si photocathode showed an excellent PEC ability and durability in alkaline media. This paper provides a promising strategy to enhance and protect the photocathode through high-performance surface cocatalysts.

关键词： photoelectrocatalysis     hydrogen evolution     Si photocathode     mesoporous MoS2    

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Effect of the degree of template removal from mesoporous silicate materials on their adsorption of heavy

Farouq TWAIQ,M.S. NASSER,Sagheer A. ONAIZI

《化学科学与工程前沿（英文）》 2014年 第8卷 第4期   页码 488-497 doi: 10.1007/s11705-014-1459-1

摘要： The key aim of this study is to evaluate the adsorption of heavy oil from aqueous solutions with different oil contents over mesoporous silicate materials having different surfactant template contents. The mesoporous silicate materials have been synthesized from tetraethylorthosilicate as a silica precursor and cetyltrimethylammonium bromide as a template using the sol-gel technique. Four samples were prepared by (1) totally removing the template using the calcination process, (2) partially removing the template via ethanol extraction, (3) partially removing the template via water extraction, and (4) keeping the template as synthesized, respectively. These four samples have been characterized using X-ray diffraction, nitrogen adsorption, thermal gravimetric analysis and Fourier transformed infrared. The effect of the degree of template removal of these mesoporous materials for the oil removal has been investigated. The oil removal is inversely proportional to the surfactant content in the mesoporous material, being highest for the calcined sample but lowest for the as-synthesized sample. The kinetic of oil adsorption over the calcined material has been also studied and the data obtained fit well a second-order model.

关键词： heavy oil     mesoporous silicate material     kinetics     template removal     adsorption    

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Using ultrasound to improve the sequential post-synthesis modification method for making mesoporous Y

Rongxin Zhang, Peinan Zhong, Hamidreza Arandiyan, Yanan Guan, Jinmin Liu, Na Wang, Yilai Jiao, Xiaolei Fan

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 275-287 doi: 10.1007/s11705-019-1905-1

摘要： Mesoporous Y zeolites were prepared by the sequential chemical dealumination (using chelating agents such as ethylenediaminetetraacetic acid, H EDTA, and citric acid aqueous solutions) and alkaline desilication (using sodium hydroxide, NaOH, aqueous solutions) treatments. Specifically, the ultrasound-assisted alkaline treatment (i.e., ultrasonic treatment) was proposed as the alternative to conventional alkaline treatments which are performed under hydrothermal conditions. In comparison with the hydrothermal alkaline treatment, the ultrasonic treatment showed the comparatively enhanced efficiency (with the reduced treatment time, i.e., 5 min vs. 30 min, all with 0.2 mol·L NaOH at 65°C) in treating the dealuminated Y zeolites for creating mesoporosity. For example, after the treatment of a dealuminated zeolite Y (using 0.1 mol·L H EDTA at 100°C for 6 h), the ultrasonic treatment produced the mesoporous zeolite Y with the specific external surface area ( ) of 160 m ·g and mesopore volume ( ) of 0.22 cm ·g , being slightly higher than that by the conventional method (i.e., = 128 m ·g and = 0.19 cm ·g ). The acidic property and catalytic activity (in catalytic cracking of -octane) of mesoporous Y zeolites obtained by the two methods were comparable. The ultrasonic desilication treatment was found to be generic, also being effective to treat the dealuminated Y zeolites by citric acid. Additionally, the first step of chemical dealumination treatment was crucial to enable the effective creation of mesopores in the parent Y zeolite (with a silicon-to-aluminium ratio, Si/Al= 2.6) regardless of the subsequent alkaline desilication treatment (i.e., ultrasonic or hydrothermal). Therefore, appropriate selection of the condition of the chemical dealumination treatment based on the property of parent zeolites, such as Si/Al ratio and crystallinity, is important for making mesoporous zeolites effectively.

关键词： zeolite Y     mesoporous zeolite     post-synthesis treatment     ultrasound     chemical dealumination treatment     alkaline desilication treatment    

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Crystalline mesoporous transition metal oxides: hard-templating synthesis and application in environmental

Zhen MA, Bei ZHOU, Yu REN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 341-355 doi: 10.1007/s11783-012-0472-1

摘要： Mesoporous silicas such as MCM-41 and SBA-15 possess high surface areas, ordered nanopores, and excellent thermal stability, and have been often used as catalyst supports. Although mesoporous metal oxides have lower surface areas compared to mesoporous silicas, they generally have more diversified functionalities. Mesoporous metal oxides can be synthesized via a soft-templating or hard-templating approach, and these materials have recently found some applications in environmental catalysis, such as CO oxidation, N O decomposition, and elimination of organic pollutants. In this review, we summarize the synthesis of mesoporous transition metal oxides using mesoporous silicas as hard templates, highlight the application of these materials in environmental catalysis, and furnish some prospects for future development.

关键词： mesoporous materials     silica     metal oxide     hard-templating     environmental catalysis    

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标题 作者 时间 类型 操作

Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective

期刊论文

Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporouscomposite

Shengchi ZHUO, Yongmin HUANG, Jun HU, Honglai LIU

期刊论文

Magnetic KIT-6 nano-composite and its amino derivatives as convenient adsorbent for U(VI) sequestration

期刊论文

Facile controlled synthesis of hierarchically structured mesoporous Li4Ti5O12/C/rGO composites as high-performance

Cehuang FU, Shuiyun SHEN, Ruofei WU, Xiaohui YAN, Guofeng XIA, Junliang ZHANG

期刊论文

Review on research and application of mesoporous transitional metal oxides in water treatment

Minghao SUI, Lei SHE

期刊论文

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

期刊论文

Synthesis of ordered cerium-doped cubic mesoporous silica using long-chain ionic liquid as template

YUE Hongxia, ZHAO Hongmei, LIU Longjiang, WANG Siping, Ruan Qiong, WANG Tongwen

期刊论文

Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

期刊论文

The modification of titanium in mesoporous silica for Co-based Fischer–Tropsch catalysts

期刊论文

Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

期刊论文

Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

期刊论文

Enhancing the photoelectrochemical performance of p-silicon through TiO coating decorated with mesoporous

期刊论文

Effect of the degree of template removal from mesoporous silicate materials on their adsorption of heavy

Farouq TWAIQ,M.S. NASSER,Sagheer A. ONAIZI

期刊论文

Using ultrasound to improve the sequential post-synthesis modification method for making mesoporous Y

Rongxin Zhang, Peinan Zhong, Hamidreza Arandiyan, Yanan Guan, Jinmin Liu, Na Wang, Yilai Jiao, Xiaolei Fan

期刊论文

Crystalline mesoporous transition metal oxides: hard-templating synthesis and application in environmental

Zhen MA, Bei ZHOU, Yu REN

期刊论文