晁自胜
1.纳米结构材料合成及应用;2. 催化绿色化学;3.清洁能源合成;4. 碳资源综合利用。
个性化签名
- 姓名:晁自胜
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学术头衔:
博士生导师
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学科领域:
物理化学
- 研究兴趣:1.纳米结构材料合成及应用;2. 催化绿色化学;3.清洁能源合成;4. 碳资源综合利用。
晁自胜,理学博士,教授。1967年出生于兰州市。1985-1992年,在兰州大学化学系读本科和硕士;1992-1995年于厦门大学化学系读博士,获理学博士学位。1995-1998年在中石化北京石油化工科学研究院从事博士后研究工作,并任职高工。1998任厦门大学化学化工学院副教授。2001年1月起在美国纽约州立大学(SUNY Buffalo)生物与化学工程系从事客座研究。2004年6月回国,任湖南大学化学化工学院教授、化学工艺学科博士生导师、湖南省“芙蓉学者计划”特聘教授。
长期从事催化新材料和石油化工等领域的研究,主持过国家“973”项目子课题、国家自然科学基金、国家教育部骨干教师资助计划、“211”工程重点建设项目和中石化技术开发项目等课题,作为主要研究人员参与了2项美国自然科学基金课题和国内10多项国家和部省级课题。研究成果主要包括:开发了具有独立知识产权的氟化碱土促进的氟氧化稀土催化剂体系,并用于甲烷氧化偶联及乙烷氧化脱氢制乙烯;在国内率先系统地开展了纳米分子筛研究,取得了一系列成果,并已在中石化系统得到工业应用;在分子筛膜合成和气体分离应用领域,取得了重要进展;在国际上首次合成了碱土-过渡金属混合氧化物介孔材料,并用于低碳烃氧化反应。发表研究论文100多篇(SCI和EI收录60多篇),拥有中国发明专利8项,曾获国家教育部科技进步一等奖和福建省运省青年科技奖。
主要研究领域:1.纳米结构材料合成及应用;2. 催化绿色化学;3.清洁能源合成;4. 碳资源综合利用。
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11
【期刊论文】Preparation and characterization of hexagonal mesoporous titanium–cobalt oxides
晁自胜, Cheng-Gao Sun a, Li Taoa, Hai-Jun Liang a, Cai-Juan Huang a, He-Sheng Zhai b, Zi-Sheng Chao a, *
Materials Letters 60(2006)2115-2118,-0001,():
-1年11月30日
Hexagonal mesoporous Co–Ti oxides were synthesized via a supramolecular assembly route, using a non-ionic surfactant, polyoxyethylene fatty alcohol (AEO9). The textural and electronic properties of the specimens were characterized by means of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), high resolution transition electron microscopy (HRTEM) and N2-physisorption at 77 K. The application of the mesoporous Co–Ti oxides in the catalytic oxidation of cyclohexane was explored.
Mesoporous material, Titanium–cobalt oxide, Nanomaterials, Sol-gel preparation
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【期刊论文】Specific Ion and pH Effects on Supramolecular Assembly of Mesostructured V-Mg Oxides
晁自胜, Zi-Sheng Chao† and Eli Ruckenstein*
Langmuir 2004, 20, 7517-7525,-0001,():
-1年11月30日
Mesostructured V-Mgoxides were synthesized using the surfactant cetyltrimethylammonium bromide (CTAB) as template, V2O5, V(acac)3 (vanadium acetylacetonate), or NH4VO3 as vanadium source, and Mg(NO3)2, MgCl2, MgSO4, (MgCO3)4
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【期刊论文】Phase Behavior of Mesostructured V-Mg-O
晁自胜, Zi-Sheng Chao and Eli Ruckenstein*
Langmuir 2003, 19, 4235-4245,-0001,():
-1年11月30日
Mesostructured vanadium-magnesium oxides (V-Mg-O) were synthesized using vanadium pentoxide and magnesium nitrate as sources and cetyltrimethylammonium bromide (CTAB) or the mixture of CTAB and hexadecylamine (HDA) as template. The effects of surfactant concentration,pHof the reaction medium, aging time, and temperature as well as aging mode (static or dynamic) were systematically investigated. The pH of the reaction medium and the surfactant concentration and nature were found to be the key parameters in the formation of V-Mg-O mesophases. When CTAB was employed alone as template and its concentration was higher than the critical micelle concentration, single lamellar mesophases were obtained in both acidic and neutral media. When the mixture of surfactants was used as template and its concentration was sufficiently low, only microporous phases were obtained in strongly acidic media (pHe 4), even at elevated aging temperatures and/or for long aging times. A mixture of mesophases could be, however, obtained in weakly acidic and neutral media (pH ) 4-7). At high surfactant concentrations, a single lamellar structure was generated in strongly acidic media and a mixture of mesophases in the weakly acidic and neutral ones. Only amorphous solids were generated in the basic range of pH, regardless of the surfactant concentration employed. With the change in aging time, numerous metastable phases have been identified, particularly in weakly acidic and neutral media.Somecomments about the mechanisms of formation of the mesophases conclude the paper.
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【期刊论文】Control of Magnesium Containing Vanadium Mesoporous Materials
晁自胜, Zi-Sheng Chao and Eli Ruckenstein*
Langmuir 2002, 18, 8535-8545,-0001,():
-1年11月30日
Magnesium containing vanadium mesoporous materials were synthesized using vanadium(V) oxide and magnesium nitrate as sources and cetyltrimethylammonium bromide (CTAB) and the mixture of CTAB andhexadecylamine(HDA)as templates.Theeffects of theMg/Vmolar ratioandthe surfactant concentration in the initial batches, the pH employed, and the length of aging time on the structural properties of the synthesized materials were investigated. Both CTAB alone and the mixture CTAB + HDA were effective in templating magnesium containing vanadium mesoporous materials, with a larger average pore size in the latter case. The degree of crystallinity of the mesoporousV-Mg-Owas found to increase with increasing surfactant concentration in the initial batches. However, a too large amount of surfactant increased tremendously the viscosity of the system, generating difficulties in the preparation. At a given pH, the degree of crystallinity of the mesoporous materials increased with increasing Mg/V molar ratio in the initial batch, attaining a maximum followed by a decrease. At a given Mg/V molar ratio in the initial batch, the degree of crystallinity increased with increasing pH, passed though an optimum for a pH ) 7, and then decreased. The analysis of the composition of the mesoporous materials revealed that the amount of magnesium included in the samples was small and increased only slightly with increasing amount in the initial batches; the increase of the pH increased, however, much more the amount of Mg included in the mesoporous materials. The stability toward heating at various temperatures increased with increasing amount of magnesium in the samples. Possible explanations for the effects found are suggested.
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【期刊论文】Structural and Morphological Control of Mesostructures: Vanadium Based Nanofibers
晁自胜, Zi-Sheng Chao and Eli Ruckenstein*
Chem. Mater. 2002, 14, 4611-4618,-0001,():
-1年11月30日
Mesostructured vanadium-magnesium oxides (V-Mg-O) with various morphologies weresynthesized at room temperature using MgCl2 and V2O5 as source materials and a large number of surfactants as templates. It was found that, among the surfactants employed, the quaternary ammonium surfactants with long alkyl chains, such as cetyltrimethylammonium bromide (CTAB), or the nonionic surfactant Triton-X 100 could template V-Mg-O mesostructures. In the former case, the synthesized specimen had a lamellar structure and nanofibrous morphology. In the latter case, the specimen had a lamellar structure but a particulate morphology. Among the binary mixtures of cationic, anionic, or nonionic surfactants employed, only the combinations between a quaternary ammonium surfactant and hexadecylamine (HDA) were effective in templating a lamellar mesophase with nanofibrous morphology. The binary surfactants were more effective than the single surfactants in generating a higher regularity of the lamellar mesostructure. Mesostructured V-Mg-O could be synthesized even using binary mixtures consisting of HDA and a quaternary ammonium surfactant with a short alkyl chain, such as benzyltrimethyl (neither of the two was effective when used alone). The mesostructured V-Mg-O nanofibers synthesized with binary mixtures of surfactants were more stable during heating at high temperatures than those synthesized with a cationic surfactant alone.
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晁自胜, Zi-Sheng Chao and Eli Ruckenstein*
Langmuir 2002, 18, 734-743,-0001,():
-1年11月30日
The mesostructured V-Mg-O was synthesized at room temperature using vanadium acetylacetonate and magnesium chloride as source materials. The effects of a number of factors, such as the nature of the surfactant, the pH, and the vanadium/magnesium molar ratio in the formation of mesoporous V-Mg-O phases were investigated for a fixed molar concentration of surfactant. The synthesized samples were examined by X-ray diffraction, Brunauer-Emmett-Teller analysis, transmission electron microscopy, and energy dispersive spectroscopy. The anionic surfactants sodium dodecyl sulfate (SDS) and sodium dodecylbenzene sulfonate (SDBS) generated amorphous structures, while the cationic surfactant cetyltrimethylammonium bromide (CTAB) generated lamellar mesoporous structures with various degrees of crystallinity. Equimolar mixtures of an anionic surfactant, SDS, and a cationic surfactant (dodecyltrimethylammonium bromide (DTAB), myristyltrimethylammonium bromide (MTAB), cetylpyridium bromide (CPB), and cetyltrimethylammonium bromide (CTAB)), particularly the mixture SDS+CTAB, generated ordered lamellar structures with high crystallinity. It was found that the ordered arrangement ("crystallinity") of the pores was strongly dependent on the vanadium/magnesium molar ratios in the initial batches; too large or too small ratios were unfavorable to the crystallinity and generated distorted hexagonal (wormlike) mesostructures. The optimum vanadium/magnesium molar ratio regarding the crystallinity was found to be in the range 1:1 to 1:1.5, and the mesoporous phase had a lamellar structure. For both the single and the mixtures of anionic and cationic surfactants, the higher the pH, the more favorable was the formation of a lamellar-structured mesoporous V-Mg-O phase.
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【期刊论文】Synthesis of Mesoporous V-Mg-O Nanofibers
晁自胜, Eli Ruckenstein* and Zi-Sheng Chao
Nano Lett., Vol. 1, No.12, 2001,-0001,():
-1年11月30日
A mesostructured V-Mg-O was synthesized for catalytic purposes using vanadium(V) oxide and magnesium chloride as sources and various surfactants or surfactant mixtures as templates. Among the surfactants employed, it was found that cetyltrimethylammonium bromide (CTAB) and the mixture of CTAB and hexadecylamine (HDA) templated fibrous lamellar-like mesostructures. The mixture of CTAB+HDA was more efficient in templating the fibrous mesoporous V-Mg-O than the individual surfactants.
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【期刊论文】Rh/SiO2催化剂上甲烷部分氧化制合成气反应机理的研究
晁自胜, 严前古, 吴延华, 杨乐夫, 罗春容, 翁维正, 万惠霖
Journal of Natural Gas Chemistry Vol. 9 No.1 2000,-0001,():
-1年11月30日
运用TPSR、TR-FTIR和化学捕获技术(CH3I作捕获剂),探讨了Rh/Si02催化剂上的POM反应机理,由此提出热分解氧化机理,认为CHx(x=l~3)和CHxO(x=1~3)可能是反应物种。
甲烷, 反应机理, 部分氧化, 合成气, Rh/, SiO2催化剂
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【期刊论文】1H MAS NMR characterization of hydrogen over silica-supported rhodium catalyst
晁自胜, CHAO Zisheng, WU Tinghua, YE Jianliang, CHEN Guozhou & WAN Huilin
SCIENCE IN CHINA (Series B), February 2001 Vol. 44 No.1,-0001,():
-1年11月30日
Hydrogen species in both SiO2 and Rh/SiO2 catalysts pretreated in different atmospheres (H2, O2, helium or air) at different temperatures (773 or 973 K) were investigated by means of 1H MAS NMR. In SiO2 and O2-pretreated catalysts, a series of downfield signals at -7.0, 3.8-4.0, 2.0 and 1.5-1.0 were detected. The first two signals can be attributed to strongly adsorbed and physisorbed water and the others to terminal silanol (SiOH) and SiOH under the screening of oxygen vacancies in SiO2 lattice, respectively. Besides the above signals, both upfield signal at −110 and downfield signals at 3.0 and 0.0 were also detected in H2-pretreated catalyst, respectively. The upfield signal at −110 originated from the dissociative adsorption of H2 over rhodium and was found to consist of both the contributions of reversible and irreversible hydrogen. There also probably existed another dissociatively adsorbed hydrogen over rhodium, which was known to be β hydrogen and in a unique form of "delocalized hydrogen". It was presumed that the β hydrogen had an upfield shift of ca.-20-50, though its 1H NMR signals, which, having been masked by the spinning sidebands of Si-OH, failed to be directly detected out. The downfield signal at 3.0 was assigned to spillover hydrogen weakly bound by the bridge oxygen of SiO2. Another downfield signal at 0.0 was assigned to hydrogen held in the oxygen vacancies of SiO2 (Si-H species), suffering from the screening of trapped electrons. Both the spillover hydrogen and the Si-H resulted from the migration of the reversible hydrogen and the β hydrogen from rhodium to SiO2 in the close vicinity. It was proved that the above migration of hydrogen was preferred to occur at higher temperature than at lower temperature.
silica, rhodium, catalyst, hydrogen, spillover, 1H MAS NMR.,
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晁自胜, 林海强, 陈国周, 吴廷华, 万惠霖, 闵恩泽
高等学校化学学报,2001,1(22):10-15,-0001,():
-1年11月30日
NaY分子筛合成体系中添加铝的络合剂(乙二胺四乙酸、柠檬酸和醋酸),可有效地减小分子筛的晶粒尺寸及增加分子筛的晶化速度和SiO2Al2O3物质的量比。在添加柠檬酸的合成体系中,考察了柠檬酸的添加量对NaY分子筛晶化行为的影响。发现存在着一个最佳的柠檬酸的添加量范围,即n(柠檬酸):n(氧化铝)≤2:1,在此范围内,NaY的晶化速率和硅铝比较高,而晶粒尺寸较小。
超微分子筛, NaY, 合成, 晶粒尺寸, 络合剂
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