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Mesoporous silicon sulfonic acid as a highly efficient and stable catalyst for the selective hydroamination

Jingbin Wen, Kuiyi You, Minjuan Chen, Jian Jian, Fangfang Zhao, Pingle Liu, Qiuhong Ai, He’an Luo

《化学科学与工程前沿（英文）》 2021年 第15卷 第3期   页码 654-665 doi: 10.1007/s11705-020-1973-2

摘要： In this work, a new mesoporous silicon sulfonic acid catalyst derived from silicic acid has been successfully prepared by the chemical bonding method. The physicochemical properties of mesoporous silicon sulfonic acid catalysts have been systematically characterized using various techniques. The results demonstrate that sulfonic acid groups have been grafted on silicic acid by forming a new chemical bond (Si–O–S). The mesoporous silicon sulfonic acid exhibits excellent catalytic performance and stability in the vapor phase hydroamination reaction of cyclohexene with cyclohexylamine. Cyclohexene conversion of 61% and 97% selectivity to dicyclohexylamine was maintained after running the reaction for over 350 h at 280 °C. The developed mesoporous silicon sulfonic acid catalyst shows advantages of low cost, superior acid site accessibility, and long term reactivity stability. Moreover, a possible catalytic hydroamination reaction mechanism over silicon sulfonic acid was suggested. It has been demonstrated that the sulfonic acid groups of the catalyst play an important role in the hydroamination. The present work provides a simple, efficient, and environmentally friendly method for the hydroamination of cyclohexene to valuable dicyclohexylamine, which also shows important industrial application prospects.

关键词： mesoporous silicon sulfonic acid     catalytic hydroamination     cyclohexene     dicyclohexylamine     vapor phase    

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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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Erratum to: Enhancing the photoelectrochemical performance of p-silicon through TiO coating decoratedwith mesoporous MoS

《能源前沿（英文）》 2022年 第16卷 第5期   页码 876-877 doi: 10.1007/s11708-022-0832-x

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One-pot three-component Mannich reaction catalyzed by sucrose char sulfonic acid

Qiong XU, Zhigao YANG, Dulin YIN, Jihui WANG

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 201-205 doi: 10.1007/s11705-009-0052-5

摘要： Sucrose char sulfonic acid efficiently catalyzed the one-pot three-component Mannich reaction of ketones, aromatic aldehydes and amines in ethanol to afford the corresponding -amino carbonyl compounds in good to excellent yields. A series of heteroaromatic -amino carbonyl compounds can be obtained when using 2-acetylpyrazine as substrate. This reaction can be performed under mild reaction conditions with clean reaction profiles and a simple workup procedure.

关键词： One–pot synthesis     b-amino ketone     char sulfonic acid     2-acetylpyrazine     catalysis    

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Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1804-7

摘要：

● Cu-C-MSNs are developed via a co-doping step of Cu with L(+)-ascorbic acid.

关键词： Cation-π structures     Polarization electric field     Fenton-like process     Contaminants cleavage    

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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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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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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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Effects of nano-silicon and common silicon on lead uptake and translocation in two rice cultivars

Jianguo LIU,Hui CAI,Congcong MEI,Mingxin WANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 905-911 doi: 10.1007/s11783-015-0786-x

摘要： The current study investigated the effects of nano-silicon (Si) and common Si on lead (Pb) toxicity, uptake, translocation, and accumulation in the rice cultivars Yangdao 6 and Yu 44 grown in soil containing two different Pb levels (500 mg·kg and 1000 mg·kg ). The results showed that Si application alleviated the toxic effects of Pb on rice growth. Under soil Pb treatments of 500 and 1000 mg·kg , the biomasses of plants supplied with common Si and nano-Si were 1.8%–5.2% and 3.3%–11.8% higher, respectively, than those of plants with no Si supply (control). Compared to the control, Pb concentrations in rice shoots supplied with common Si and nano-Si were reduced by 14.3%–31.4% and 27.6%–54.0%, respectively. Pb concentrations in rice grains treated with common Si and nano-Si decreased by 21.3%–40.9% and 38.6%–64.8%, respectively. Pb translocation factors (TFs) from roots to shoots decreased by 15.0%–29.3% and 25.6%–50.8%, respectively. The TFs from shoots to grains reduced by 8.3%–13.7% and 15.3%–21.1%, respectively, after Si application. The magnitudes of the effects observed on plants decreased in the following order: nano-Si treatment>common Si treatment and high-grain-Pb-accumulating cultivar (Yangdao 6)>low-grain-Pb-accumulating cultivar (Yu 44) and heavy Pb stress (1000 mg·kg )>moderate Pb stress (500 mg·kg )>no Pb treatment. The results of the study indicate that nano-Si is more efficient than common Si in ameliorating the toxic effects of Pb on rice growth, preventing Pb transfer from rice roots to aboveground parts, and blocking Pb accumulation in rice grains, especially in high-Pb-accumulating rice cultivars and in heavily Pb-polluted soils.

关键词： silicon (Si)     lead (Pb)     rice (Oryza sativa L.)     toxicity     accumulation    

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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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Computer modeling of crystal growth of silicon for solar cells

Lijun LIU, Xin LIU, Zaoyang LI, Koichi KAKIMOTO

《能源前沿（英文）》 2011年 第5卷 第3期   页码 305-312 doi: 10.1007/s11708-011-0155-9

摘要： A computer simulator with a global model of heat transfer during crystal growth of Si for solar cells is developed. The convective, conductive, and radiative heat transfers in the furnace are solved together in a coupled manner using the finite volume method. A three-dimensional (3D) global heat transfer model with 3D features is especially made suitable for any crystal growth, while the requirement for computer resources is kept permissible for engineering applications. A structured/unstructured combined mesh scheme is proposed to improve the efficiency and accuracy of the simulation. A dynamic model for the melt-crystal (mc) interface is developed to predict the phase interface behavior in a crystal growth process. Dynamic models for impurities and precipitates are also incorporated into the simulator. Applications of the computer simulator to Czochralski (CZ) growth processes and directional solidification processes of Si crystals for solar cells are introduced. Some typical results, including the turbulent melt flow in a large-scale crucible of a CZ-Si process, the dynamic behaviors of the mc interface, and the transport and distributions of impurities and precipitates, such as oxygen, carbon, and SiC particles, are presented and discussed. The findings show the importance of computer modeling as an effective tool in the analysis and improvement of crystal growth processes and furnace designs for solar Si material.

关键词： computer modeling     silicon     crystal growth     solar cells    

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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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标题 作者 时间 类型 操作

Mesoporous silicon sulfonic acid as a highly efficient and stable catalyst for the selective hydroamination

Jingbin Wen, Kuiyi You, Minjuan Chen, Jian Jian, Fangfang Zhao, Pingle Liu, Qiuhong Ai, He’an Luo

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

Erratum to: Enhancing the photoelectrochemical performance of p-silicon through TiO coating decoratedwith mesoporous MoS

期刊论文

One-pot three-component Mannich reaction catalyzed by sucrose char sulfonic acid

Qiong XU, Zhigao YANG, Dulin YIN, Jihui WANG

期刊论文

Enhanced Fenton-like process over Cu/L(+)-ascorbic acid co-doping mesoporous silica for toxicity reduction

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

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

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

Effects of nano-silicon and common silicon on lead uptake and translocation in two rice cultivars

Jianguo LIU,Hui CAI,Congcong MEI,Mingxin WANG

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

Computer modeling of crystal growth of silicon for solar cells

Lijun LIU, Xin LIU, Zaoyang LI, Koichi KAKIMOTO

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