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Development of New Generation Ammonia Synthesis Catalyst Process

新一代氨合成催化剂工艺开发

基本信息

批准号：
10355032
负责人：
AIKA Ken-ichi
金额：
$ 17.41万
依托单位：
Tokyo Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (A)
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-10355032/
关键词：
Ammonia Synthesis Ruthenium Catalyst Promoter Effect High Pressure Hydrogen Treatment Activated Carbon Supported Ruthenium Catalyst Methanation

项目摘要

Development of New Generation Ammonia Synthesis Catalyst ProcessAmong several supports, active carbon (AC) was found to be most effective in ruthenium catalysts for ammonia synthesis.Electronic promoter such as alkali nitrate is necessary to be added to Ru/AC. Promoter nitrate must be decomposed under hydrogen stream at high temperature to the corresponding oxide or hydroxide (CsNOィイD23ィエD2→ CsOH, Ba(NOィイD23ィエD2)ィイD22ィエD2→ BaO). In this study, this hydrogen treatment process (including nitrate decomposition and partial methanation of the support AC) was found to be quite important to activate the catalysts. The hydrogen treatment is recommended to be carried out with slow heating rate (10℃/min) of temperature increase up to 550℃. Promoter decomposition was completed up to 365℃, so the extra heat treatment at the high temperature initiated the methanation of carbon support. The last process was found to be the key factor of catalyst activation, where carbon surrounding Ru particle is partially hydrogenated (to give a proper situation of Ru-CsOH interaction). The excess heating (above 550℃) brings either Ru sintering or deformation of carbon support, which gives poor activity.Ru-CsOH/AC which is activated properly gives much higher ammonia activity than the commercial iron catalysts. The basic principle to prepare the second generation ammonia synthesis catalyst was established by this study.

新一代氨合成催化剂的开发在几种载体中，活性碳(AC)被认为是最有效的Ru合成氨催化剂。促进剂硝酸盐必须在高温氢气下分解为相应的氧化物或氢氧化物(CsNOィイD23ィエD2→CsOH，BA(noィイD23ィエD2)ィイD22ィエD2→BaO)。在本研究中，这一氢处理过程(包括载体AC的硝酸盐分解和部分甲烷化)被发现对催化剂的活化非常重要。建议以慢升温速率(10℃/℃)进行氢处理，升温至550min。助剂在365℃时分解完成，因此高温下的额外热处理引发了碳载体的甲烷化。最后一个过程是催化剂活化的关键，其中Ru颗粒周围的碳被部分氢化(以提供一个合适的Ru-CsOH相互作用的位置)。过热(5 5 0℃以上)会导致Ru的烧结或碳载体的变形，活性较差，适当活化的Ru-CsOH/AC具有比商用铁催化剂高得多的氨活性。通过本研究确立了第二代氨合成催化剂制备的基本原理。