Development of Highly Active Metallosilicate Catalysts for Propane Aromatization

高活性丙烷芳构化金属硅酸盐催化剂的研制

• 批准号: 02505006
• 负责人: INUI Tomoyuki
• 金额: $ 29.7万
• 依托单位: KYOTO UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Developmental Scientific Research (A)
• 财政年份: 1990
• 资助国家: 日本
• 起止时间: 1990 至 1992
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-02505006/
• 关键词: Aromatization; Straight-chained saturated hydrocarbons; Ga-silicate; Ot modification; Coke formation; Long-term catalytic test; Full-automatic flow reactor; Computational chemistry; 飽和炭化水素; 低級パラフィン; プロパン転化; 芳香族炭化水素; ペンタシル型メタロシリケート; ガリウムシリケート

Aromatization of C2-C20 straight-chained saturated hydrocarbons was studied on Ga-and Zn-silicates with MFI structure. The conversions increased but the aromatic selectivities decreased with the increase in C number up to C5. For hydrocarbons higher than C6, the selectivities were almost same due to the direct cyclization. The aromatic selectivities were much improved by using Pt incorporated Ga-silicate, which had moderated cracking ability with maintaining the dehydrogenation ability. Effectiveness of Pt modification to improve the catalyst life was reconfirmed and furthermore addition of basic components, which neutralized the surface acidic sites, was also found to be effective. The mechanism of coke formation, property of the formed coke, and rejuvenating treatment method were examined in detail. The long-term catalytic tests for propane aromatization were conducted using a full-automatic flow reactor. On the other hand, to understand the dynamic diffusion process in micropores and the acidic properties of microporous materials, a new evaluating method by computational chemistry was developed. It was applied for this system and proved to be powerful method to comprehend microscopic phenomena.

研究了C2-C20直链饱和烃在具有MFI结构的Ga-和Zn-硅酸盐上的芳构化反应。随着C数增加到C5，转化率增加，但芳烃选择性下降。对于C6以上的烃，由于直接环化，选择性几乎相同。通过使用掺有 Pt 的 Ga-硅酸盐，芳烃选择性大大提高，其在保持脱氢能力的同时具有适度的裂化能力。再次证实了 Pt 改性对提高催化剂寿命的有效性，此外，中和表面酸性位点的碱性成分的添加也被发现是有效的。对焦炭的形成机理、成型焦的性质以及再生处理方法进行了详细研究。丙烷芳构化的长期催化试验是使用全自动流动反应器进行的。另一方面，为了了解微孔中的动态扩散过程和微孔材料的酸性特性，开发了一种新的计算化学评估方法。它被应用于该系统并被证明是理解微观现象的有力方法。

项目成果

Tomoyuki Inui: "Environments of Iron in Fe-Silicates Synthesized by the Rapid Crystallization Method" J.Catalysis. 139. 482-489 (1993)

Tomoyuki Inui：“快速结晶法合成的硅酸铁中铁的环境”J.Catalysis。

Hideo Nagata: "Synthesis and Catalytic Performance of Fe-Cr-Bimetallosilicate Having a Pentasil Pore Structure" Applied Catalysis A : General. 94, No.1. 17-30 (1993)

Hideo Nagata：“具有 Pentasil 孔结构的 Fe-Cr-双金属硅酸盐的合成和催化性能”应用催化 A：概述。

Tomoyuki INUI: "Highly selective Synthesis of Tthene from Methanol on a Novel NickelーSilicoaluminophophate Catlyst" J.Chem.Soc.,Chem.Comun.205-206 (1990)

Tomoyuki INUI：“在新型镍硅铝磷酸盐催化剂上从甲醇中高度选择性合成乙烯”J.Chem.Soc.,Chem.Comun.205-206 (1990)

伊藤潤一: "Znを主成分として含む多元メタロシリケート触媒による軽質ナフサ留分の芳香族化" 石油学会誌. 36. 114-120 (1993)

Junichi Ito：“使用含有Zn作为主要成分的多组分金属硅酸盐催化剂的轻质石脑油馏分的芳构化”日本石油学会学报36. 114-120(1993)。

Yoshiaki Nakazaki: "Simulation of Dyanamic Behaviors of Simple Aromatic hydrocarbons inside the Pores of Pentasil Zeolite" J.Catalysis. 136. 141-148 (1992)

Yoshiaki Nakazaki：“Pentasil 沸石孔隙内简单芳香烃的动态行为模拟”J.Catalysis。