DESIGN OF ETHYLENE ADSORBENT BASED ON ANALYSIS OF ADSORPTION GEOMETRY USING MOLECULAR ORBITAL CALCULATION

基于分子轨道计算吸附几何分析的乙烯吸附剂设计

• 批准号: 10650759
• 负责人: TAMON Hajime
• 金额: $ 2.05万
• 依托单位: KYOTO UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 1998
• 资助国家: 日本
• 起止时间: 1998 至 1999
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-10650759/
• 关键词: Molecular orbital method; Analysis of adsorption geometry; Separation of ethane and ethylene; Silica gel; Impregnation of silver nitrate; Impregnation of cuprous chloride; Adsorption selectivity of ethylene; Selection of impregnant; エタン-エチレン吸着分離 /

The surface of silica gel or alumina impregnated with metal cation was modeled and the structure was optimized by ab intio molecular obital (MO) calculation. The interaction energy △E between the model surface and adsorbate (ethylene or ethane) was determined by △E=E1+E2-E3, where E3 is the total energy for the adsorption structure. The isolated energies of adsorbate and adsorption site are E1 and E2. Metal cations are selected to give the maximum values of the interaction energy. AgNOィイD23ィエD2-silica gel, CuCl-silica gel, AgNOィイD23ィエD2-alumina, and CuCl-alumina were prepared by the impregnation method and the chemical vapor deposition (CVD) method. The adsorption selectivity of ethylene was experimentally studied. The adsorption geometry and energy were estimated by the MO calculations. The following conclusions were obtained.1) The MO calculations show that AgNOィイD23ィエD2 and CuCl are useful as impregnants to separate ethylene from ethane.2) AgNOィイD23ィエD2-silica gel and CuCl-alumina can be prepared by CVD method.3) X-ray photoelectron spectroscopy (XPS) measurement and Fourier transform infrared (FT-IR) measurement suggest that the adsorption sites of the adsorbents prepared are AgィイD1+ィエD1, AgNOィイD23ィエD2, CuィイD1+ィエD1,and CuCl.4) The MO calculation and adsorption experiments show that the adsorbents prepared show high ethylene selectivity.

采用从头算分子轨道（MO）方法，对金属离子浸渍硅胶或氧化铝的表面进行了模拟和结构优化。模型表面与吸附质（乙烯或乙烷）之间的相互作用能△E由△E=E1+E2-E3确定，其中E3为吸附结构的总能量。吸附质和吸附位的孤立能分别为E1和E2。选择金属阳离子以给出相互作用能的最大值。采用浸渍法和化学气相沉积法制备了阿尼奥纳米D23纳米D2-硅胶、CuCl-硅胶、阿尼奥纳米D23纳米D2-氧化铝和CuCl-氧化铝。对乙烯的吸附选择性进行了实验研究。通过分子轨道计算，估算了吸附几何构型和吸附能量。结果表明：1）分子轨道计算表明，阿尼奥络合物D23络合物D2和氯化亚铜可作为乙烯/乙烷分离的澄清剂; 2）化学气相沉积法可制备出阿尼奥络合物D23络合物D2-硅胶和氯化亚铜-氧化铝; 3）X射线光电子能谱（XPS）和傅里叶变换红外光谱（FT-IR）测试结果表明，该催化剂具有良好的催化活性。分子轨道计算和吸附实验表明，所制备的吸附剂具有较高的乙烯选择性。

项目成果

Tetsuo Suzuki: "A Theoretical Study on Interaction between AgNO_2-Silica Gel and Adsorbed Molecules by Using Ab Initio MO Method"Proc. of the 8th APCChE Congress. 3. 1781-1784 (1999)

Tetsuo Suzuki：“利用 Ab Initio MO 方法理论研究 AgNO_2-硅胶与吸附分子之间的相互作用”Proc。

Tetsuo Suzuki: "A Theoretical Study on Interaction between Metal Embedded/Impregnated Silica Gel and Adsorbed Molecules by Using Ab Intio MO Method"Fundamentals of Adsorption. 885-890 (1998)

Tetsuo Suzuki：“使用 Ab Intio MO 方法对金属嵌入/浸渍硅胶与吸附分子之间相互作用的理论研究”吸附的基础知识。

Tetsuo Suzuki, Hajime Tamon and Morio Okazaki: "A Theoretical Study on Interactions Between Metal Embedded/Impregnated Silica Gel and Adsorbed Molecules by Using ab Initio MO Method" Fundamentals of Adsorption 6 (Elseuier). 885-890 (1998)

Tetsuo Suzuki、Hajime Tamon 和 Morio Okazaki：“使用从头开始 MO 方法对金属嵌入/浸渍硅胶与吸附分子之间相互作用的理论研究”吸附基础 6 (Elseuier)。

Tetsuo Suzuki: "A Theoretical Study on Interaction between AgNOィイD23ィエD2-Silica Gel and Adsorbed Molecules by Using Ab Initio MO Method"Proc. of the 8th APCChE Congress. Vol.3. 1781-1784 (1999)

Tetsuo Suzuki：“使用 Ab Initio MO 方法进行 AgNO-D23-硅胶与吸附分子相互作用的理论研究”，第八届 APCChE 大会第 3 卷（1999 年）。

Tetsuo Suzuki: "A Theoretical Study on Interaction between Metal Embedded/Impregnated Silica Gel and Adsorbed Molecules by Using Ab Initio MO Method"Fundamentals of Adsorption. 885-890 (1998)

Tetsuo Suzuki：“使用 Ab Initio MO 方法对金属嵌入/浸渍硅胶与吸附分子之间相互作用的理论研究”吸附的基础知识。