高等学校化学学报 ›› 2000, Vol. 21 ›› Issue (7): 999.

• 论文 • 上一篇    下一篇

双金属杂原子分子筛CrCoBEA的合成、波谱及催化性能研究

王亚军, 唐祥海, 朱瑞芝, 潘履让   

  1. 南开大学化学系, 天津 300071
  • 收稿日期:1999-07-13 出版日期:2000-07-24 发布日期:2000-07-24
  • 通讯作者: 潘履让(1938年出生),男,教授,从事催化化学研究.
  • 基金资助:

    国家自然科学基金重点项目(批准号:29733070);中国石油化工集团公司(批准号:X597013)资助

Studies on the Synthesis, Spectroscopy and Catalytic Properties of CrCoBEA Metallosilicate

WANG Ya-Jun, TANG Xiang-Hai, ZHU Rui-Zhi, PAN Lü-Rang    

  1. Departmennt of Chemistry, Nankai University, Tianjin 300071, China
  • Received:1999-07-13 Online:2000-07-24 Published:2000-07-24

摘要: 采用水热晶化法首次合成出BEA结构含铬、钴双金属杂原子分子筛CrCoBEA,对晶化时间、晶化温度、成胶配比等合成条件进行了优化研究.采用XRD,FTIR,UVVisDRS,ESR及催化反应等方法测试其物相、波谱性质和催化性能.结果表明,物质的量比为TEOS∶0.017[Cr(acac)3]∶0.017[Co(acac)3]∶(058-0.64)TEAOH∶0.01Al(NO3)3∶(1620)H2O的成胶体系在408428K静态晶化90150h,可合成出结晶度高且晶相单一的CrCoBEA分子筛.铬、钴在晶化过程中进入分子筛骨架,并以多种化学状态高度分散于分子筛上.所合成的杂原子分子筛对环己烯氧化和NO分解反应有较好的催化活性.环己烯氧化反应活性和NO分解反应的活性顺序分别为:CrCoBEA>CoBEA>CrBEA和CrBEA>CrCoBEA>CoBEA.

关键词: 水热晶化, 金属杂原子分子筛, 波谱性质, 选择氧化, NO分解反应

Abstract: Metallosilicates with BEAstructure simultaneously containing chromium and cobalt have been hydrothermally synthesized for the first time under static conditions. By varying temperature, time as well as concentration of the starting materials, the optimal conditions for the synthesis of CrCoBEAmolecular sieve were deduced. The crystallinity, spectroscopic property and catalytic activity of CrCoBEAwere evaluated by means of XRD, FTIR, UV-Vis DRS, ESRand catalytic tests, respectively. The result reveals that crystallization with gel molar composition of TEOS∶0.017[Cr(acac)3]∶0.017[Co(acac)3]∶(0.580.64)TEAOH∶0.01Al(NO3)3∶(1620)H2Oat 408428 Kafter 90150 h gave a high crystallinity, uni-phased Cr-CoBEAmolecular sieve. Both chromium and cobalt ions incorporated into the framework during crystallization were highly dispersed with multiple chemical status. The CrCoBEAmolecular sieve exhibited promising catalytic activities in the selective oxidation of cyclohaxene with dilute H2O2 and the decomposition of NO. The order of activity for selective oxidation of cyclohexene and decomposition of NOwere CrCoBEA>CoBEA>CrBEAand CrBEA>CrCoBEA>CoBEA, respectively.

Key words: Hydrothermal crystallization, Metallosilicates, Spectroscopic property, Selective oxidation, Decomposition of NO

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