SYNTHESIS OF NOVEL LAYERED METAL HALIDE OXIDES AND THEIR APPLICATION AS CATALYSTS FOR SELECTIVE ALKANE OXIDATION
新型层状金属卤氧化物的合成及其作为烷烃选择性氧化催化剂的应用
基本信息
- 批准号:03650647
- 负责人:
- 金额:$ 1.15万
- 依托单位:
- 依托单位国家:日本
- 项目类别:Grant-in-Aid for General Scientific Research (C)
- 财政年份:1991
- 资助国家:日本
- 起止时间:1991 至 1992
- 项目状态:已结题
- 来源:
- 关键词:
项目摘要
(1) Utilization of Metal Halide Oxides as Solid Catalysts In order to obtain highly effective and functionalized solid catalysts based on layred metal halide oxides for selective oxidations of alkanes with molecular oxygen, fundamental informations on the metal halide oxides in terms of structure, catalytic activity, selectivity, stability, and role of halogen, were accumulated by the synthesis of various layred bismuth halide oxides including samples with novel structures. The bismuth-based halide oxides constitute a large family of layred compound, all of which crystallize into structures consisting of cation-oxygen layr sheets associated with the tetragonal PbO structure, alternating with single or multiple sheets of halide ions. As increasing the multiplicity of the halide ion sheet, the catalytic activity for methane oxidative coupling reaction and the selectivity to C_2-hydrocarbons increased prominently. However, reversely decreased the stability of the catalysts, the activities … More deeaying with the reaction time with the liberation of halogen form the catalyst. It was found that these catalysts were also very active and selective for the oxidative dehydrogenation of ethane to ethylene.(2) Structural Analysis with High Resolution Electron Microscopy(HREM) and Computer Graphics The synthesis of novel layred bismuth hallde oxides is a key issue of this work, thus structural analysis being very important. The structural analyzes has been carried out in the aid of high resolution electron microscopy(HREM) and computer graphics.Kinetics of Methane Oxidative Coupling over Layred Metal Halide Oxide Catalysts On the basis that halogen species liberated from the bulk of the catalyst were not involved in the reaction in the gas phase, it is concluded that halide ions on the surface constitute active site for the reaction and their abilities for the reaction strongly depend on the interaction to the oxygen sheet.(4) Catalytic Properties of Arppe's Phase-Type Metal Halide Oxides Three distinet examples of Arppe's pase(M_<24>O_<31>Cl_<10> ; M=Bi, La, Sm), which has a structure related to that of the layred oxychloride BiOCl, have been used as monophasic catalysts for the oxidative dehydrogenation of methane. The stability and performance of these catalysts rival those of the best catalysts previously described.(5) Catalytic Properties of Metal Halide Oxides Having Multiple Metal-Oxygen Sheet Several distinet types of bismuth-based chloride oxides, all of which have layred structures and are regulated on varying the thicknesses of infinite metal oxygen sheets, have been tested as monophasic catalysts for methane oxidation. It was found that the chlorine sheets between the metal oxygen sheets are responsible for the higher catalytic performance. On the basis of this results, highly integrated metal halide oxide catalysts have been designed for propane oxidation.(6) Intercalation of Halide Ion and Water into the Interlayr of Metal Halide Oxides Is was found that halide ion and water can intercalate into the interlayr between halide sheets of metal halide oxides by immersing in aqueous metal halide solution at ambient temperature. The phenomenon was investigated using XRD,EST and EXAFS.Catalytic Activities of Layred Metal Chloride Oxides for Dehydrohalogenation Various metal chloride oxides having layred structure have been tested as catalysts for the dehydrohalogenation of t-butyl chloride to form olefin and were found active for the reaction, depending on the metal constituents and the structure. Less
为了获得基于层状金属卤化物氧化物的高效功能化固体催化剂,用于分子氧选择性氧化烷烃,通过合成各种层状卤化铋氧化物,包括具有新结构的样品,积累了金属卤化物氧化物在结构、催化活性、选择性、稳定性和卤素作用等方面的基本信息。铋基卤化物氧化物构成了一个大的层状化合物家族,所有这些化合物都结晶成由与四方PbO结构相关的阳离子-氧层片组成的结构,与单片或多片卤化物离子交替存在。随着卤化物离子片数量的增加,甲烷氧化偶联反应的催化活性和对c_2 -烃类的选择性显著提高。随着反应时间的延长,卤素从催化剂中析出,催化剂的活性逐渐衰减。研究发现,这些催化剂对乙烷氧化脱氢制乙烯也具有很强的活性和选择性。新型层状卤化铋氧化物的合成是本工作的关键问题,因此结构分析非常重要。利用高分辨率电子显微镜(HREM)和计算机图形学对其结构进行了分析。层状金属卤化物氧化物催化剂上的甲烷氧化偶联动力学基于从催化剂主体中释放的卤素在气相中不参与反应,得出表面卤化物离子是反应的活性位点,其反应能力强烈依赖于与氧片的相互作用。(4) Arppe相型金属卤化物氧化物的催化性能研究了三种Arppe相型金属卤化物氧化物(M_<24>O_<31>Cl_<10>; M=Bi, La, Sm)作为甲烷氧化脱氢的单相催化剂,其结构与层状氯氧BiOCl相似。这些催化剂的稳定性和性能可与先前描述的最佳催化剂相媲美。几种不同类型的铋基氯化物氧化物都具有层状结构,并受无限金属氧片厚度的调节,已被测试为甲烷氧化的单相催化剂。研究发现,金属氧片之间的氯片是提高催化性能的原因。在此基础上,设计了丙烷氧化用高集成度金属卤化物氧化物催化剂。(6)卤化物离子与水在金属卤化物氧化物层间的插层研究发现,在常温下浸泡在金属卤化物水溶液中,卤化物离子与水可以插层到金属卤化物氧化物的卤化物片层间。采用XRD、EST和EXAFS对该现象进行了研究。层状金属氯氧化物对脱氢卤化反应的催化活性有多种具有层状结构的金属氯氧化物,它们可作为t-丁基氯脱氢卤化生成烯烃的催化剂进行测试,并且根据金属成分和结构的不同,发现对该反应具有活性。少
项目成果
期刊论文数量(5)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
W.Ueda, M.Tamazaki, and Y.morikawa: "Catalytic Activities of Layred Metal Chloride Oxides for the Dehydrohalogenation of t-Butyl Halides." Bull. Chem. Soc. JPN.66. 347-349 (1993)
W.Ueda、M.Tamazaki 和 Y.morikawa:“层状金属氯化物氧化物对叔丁基卤化物脱卤化氢的催化活性”。
- DOI:
- 发表时间:
- 期刊:
- 影响因子:0
- 作者:
- 通讯作者:
R.Burch,S.Chalker,John.M.Thomas,Wataru Ueda,and P.Loader: "An Investigation of Ethene Selectivity in the Methane Coupling Reaction on Chlorineーcontaining Catalysts;" Appl.Catal.,. 82. 77-90 (1992)
R.Burch、S.Chalker、John.M.Thomas、Wataru Ueda 和 P.Loader:“含氯催化剂上甲烷偶联反应中乙烯选择性的研究;”82. 77- 90 (1992)
- DOI:
- 发表时间:
- 期刊:
- 影响因子:0
- 作者:
- 通讯作者:
W.Ueda: "Catalytic Oxidative Dimerization of Methane to FormC _<2ー>Compounds over Arppe's Phase Oxychlorides of Bi,La and Sm," Catal.Lett.10. 83-90 (1991)
W.Ueda:“Bi、La 和 Sm 的 Arppe 相氯氧化物上甲烷催化氧化二聚反应”,Catal.Lett.10 (1991)。
- DOI:
- 发表时间:
- 期刊:
- 影响因子:0
- 作者:
- 通讯作者:
W.Ueda,M.Yamazaki,Y.morikawa.: "Catalytic Activity of Layered Metrl Chleride Oxules for the Dehydrhalogenation of t-Butyl Halides." Bull.Chem Soc.Jpn.66. 347-349 (1993)
W.Ueda、M.Yamazaki、Y.morikawa.:“层状甲基氯化物 Oxule 对叔丁基卤化物脱卤化氢的催化活性。”
- DOI:
- 发表时间:
- 期刊:
- 影响因子:0
- 作者:
- 通讯作者:
Wataru Ueda,Masato Yamazaki,Yutaka Morikawa: "Catalytic Activities of Layered Metal Chloride Oxides for the Dehydrohalogenation of tーButyl Halides" Bull.Chem.Soc.Jpn.66. 347-349 (1993)
Wataru Ueda、Masato Yamazaki、Yutaka Morikawa:“层状金属氯化物氧化物对叔丁基卤化物脱卤化氢的催化活性”Bull.Chem.Soc.Jpn.66 (1993)。
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UEDA Wataru其他文献
近年の洪水時橋梁被害の推移と水理・構造的要因の検討
检查近期洪水期间桥梁损坏的变化以及水力/结构因素
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2022 - 期刊:
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UEDA Wataru;SUZUKI Hiiro;INOUE Takashi;KASHIWADA Jin;NIHEI Yasuo;二瓶泰雄,井上隆 - 通讯作者:
二瓶泰雄,井上隆
Crystalline micorporous transition metal oxide based on vanadotungstate
基于钒钨酸盐的结晶微孔过渡金属氧化物
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2017 - 期刊:
- 影响因子:0
- 作者:
ZHANG Zhenxin;UEDA Wataru - 通讯作者:
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北海道の暖候期における前線の特徴
北海道暖季锋面特征
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2022 - 期刊:
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UEDA Wataru;SUZUKI Hiiro;INOUE Takashi;KASHIWADA Jin;NIHEI Yasuo;二瓶泰雄,井上隆;宮本真希,山田朋人 - 通讯作者:
宮本真希,山田朋人
MODEL EXPERIMENT AND 3D FLOW SIMULATION FOR INFLUENCE OF CAPTURED DRIFTWOOD ON FLUID FORCE OF RIVER BRIDGE
捕获漂流木对河桥流体力影响的模型试验及三维流动模拟
- DOI:
10.2208/jscejhe.78.2_i_277 - 发表时间:
2022 - 期刊:
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UEDA Wataru;SUZUKI Hiiro;INOUE Takashi;KASHIWADA Jin;NIHEI Yasuo - 通讯作者:
NIHEI Yasuo
過去43年間の日本周辺における前線の気候特性
近43年日本各地锋面气候特征
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- 发表时间:
2022 - 期刊:
- 影响因子:0
- 作者:
UEDA Wataru;SUZUKI Hiiro;INOUE Takashi;KASHIWADA Jin;NIHEI Yasuo;二瓶泰雄,井上隆;宮本真希,山田朋人;宮本真希,山田朋人 - 通讯作者:
宮本真希,山田朋人
UEDA Wataru的其他文献
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{{ truncateString('UEDA Wataru', 18)}}的其他基金
Structure engineering of functional solid catalysts by unit-network methodology
单元网络方法的功能固体催化剂的结构工程
- 批准号:
23246135 - 财政年份:2011
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (A)
Nano structurizing and new oxidation catalyst development of perovskite compound oxide by structuralo rganics assistance
结构有机辅助钙钛矿复合氧化物纳米结构及新型氧化催化剂的开发
- 批准号:
18360383 - 财政年份:2006
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (B)
Construction of cluster lattice structured mixed metal oxides using unit synthesis and it's catalytic selective oxidation
单元合成构建簇晶结构混合金属氧化物及其催化选择性氧化
- 批准号:
16360396 - 财政年份:2004
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (B)
Formation of metal oxide cluster lattice and catalytic oxidation properties
金属氧化物簇晶格的形成及催化氧化性能
- 批准号:
13650847 - 财政年份:2001
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (C)
Development of high-performance solid catalysts for selective oxidative dehydrogenation of ethane by structural fine tuning with in-situ XRD
通过原位 XRD 结构微调开发用于乙烷选择性氧化脱氢的高性能固体催化剂
- 批准号:
10450302 - 财政年份:1998
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (B)
Synthesis of Solid-state Metal Phosphate Catalysts Having Chiral Structure
具有手性结构的固态金属磷酸盐催化剂的合成
- 批准号:
08650922 - 财政年份:1996
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for Scientific Research (C)
Synthesis of Solid-state Metal Phosphate Catalysts Having Chiral Structure
具有手性结构的固态金属磷酸盐催化剂的合成
- 批准号:
06650895 - 财政年份:1994
- 资助金额:
$ 1.15万 - 项目类别:
Grant-in-Aid for General Scientific Research (C)
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