甲与甲醇:Cu-CHA的结构活动关系
Dimitrios K Pappas1, Elisa Borfecchia2,3, Michael Dyballa1
1Center for Materials Science and Nanotechnology (SMN), Department of Chemistry, University of Oslo , 1033 Blindern, 0315 Oslo, Norway.
Journal of the American Chemical Society
|September 26, 2017
概括
在低温下,铜交换的化物,特别是Cu-SSZ-13,可以将甲转化为甲醇. 通过控制活跃的铜部位,优化条件和材料组成可以最大限度地提高甲醇的生产率.
科学领域:
- 催化剂
- 材料科学
- 化学工程
背景情况:
- 甲选择性部分氧化为甲醇对于化学合成至关重要.
- 交换的热石具有低温甲转换的潜力.
- -SSZ-13是这种转化的一个有前途的材料.
研究的目的:
- 研究反应参数和元素组成对Cu-SSZ-13甲转化性能的影响.
- 确定和描述过程中涉及的活性铜物种.
- 优化条件以最大限度地提高甲醇的生产率.
主要方法:
- 测量甲醇产量的活动测试.
- 射线吸收光谱 (XAS) 用于确定铜的物种化.
- 反应参数和材料组成的系统变化 (Si:Al和Cu:Al比率).
主要成果:
- 在O2的存在下形成活性Cu (II) 位点,高温和延长的激活时间增加了它们的数量.
- 甲醇的生产率与材料的可减少性呈现线性相关性.
- 优化的条件和材料组成产生了0.2molCH3OH/molCu的甲醇生产率.
- 在低Si:Al和Cu:Al比率的2Al Z2Cu (II) 位点中发现了高数量的不活跃物.
- 确定Z[Cu(II) OH]复合物是活性位点的非活性前体.
结论:
- 这项研究阐明了铜在Cu-SSZ-13中部分氧化甲的作用.
- 最佳的工艺条件和材料成分对于最大限度地提高甲醇产量至关重要.
- 了解活性位点的形成和失活途径是催化剂开发的关键.
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