分子量身定制的前体和支产生稳定的甲干改催化剂,具有优越的金属利用率
Tigran Margossian1, Kim Larmier1, Sung Min Kim2
1Department of Chemistry and Applied Biosciences, ETH Zürich , Vladimir-Prelog-Weg 1-5, CH-8093 Zürich, Switzerland.
Journal of the American Chemical Society
|April 27, 2017
概括
使用新型前体开发了用于甲干重制的稳定催化剂. 补充氧化通过防止的迁移来显著提高催化剂的稳定性,这对于高效的合成气体生产至关重要.
科学领域:
- 催化科学与工程
- 用于能源应用的材料科学
- 化学反应工程
背景情况:
- 干燥改制甲 (DRM) 产生合成气,但由于反应条件恶劣,需要稳定的催化剂.
- 焦炭形成,烧结和金属扩散是催化剂失活的关键挑战.
- 开发强大的催化剂对于高效和可持续的合成天然气生产至关重要.
研究的目的:
- 使用分子前体在基支持上合成稳定的 (Ni) 纳米粒子.
- 在DRM过程中研究Ni催化剂的失活机制.
- 通过减轻Ni迁移到基支持来提高催化剂的稳定性.
主要方法:
- 一个分子前体的合成,[{Ni(μ2-OCHO) ((OCHO) ((tmeda) }2 ((μ2-OH2)) ] (tmeda =四甲基乙二胺).
- 在基基上形成2nmNi(0) 纳米粒子.
- 操作X射线吸收近边缘结构 (XANES) 光谱,以研究反应条件下的催化剂行为.
- 使用化作为支持来增强催化剂的稳定性.
主要成果:
- 分子前体很容易形成小的Ni0纳米粒子,增强了初始活性并减少了焦炭沉积.
- 操作XANES显示,Ni迁移到的支是主要的失活途径.
- 基支持的Mg-doping有效地减轻了Ni损失,显著改善了DRM的催化剂稳定性.
结论:
- 催化剂的分子设计方法,结合了定制的前体和支持修改,对DRM是有效的.
- 添加成功阻止了的迁移,导致高度稳定和活跃的催化剂.
- 这种策略最大限度地提高了可获得的金属,同时最大限度地减少了关闭,为高效的合成气生产铺平了道路.
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