在 - 催化剂上的双功能表面部位上对多和循环乙烯的选择性解
Mei Chia1, Yomaira J Pagán-Torres, David Hibbitts
1Department of Chemical and Biological Engineering, University of Wisconsin-Madison, 1415 Engineering Drive, Madison, Wisconsin 53706, United States.
一种由氧化促进的碳上 (Rh/C) 催化剂选择性地破坏循环和聚中的C-O键. 这种双功能催化剂使用酸位进行环开放和金属位进行化,这对于生物质转化至关重要.
科学领域:
- 不同质的催化剂.
- 生物质转换生物质转换
- 有机化学 有机化学
背景情况:
- 来自生物质的原料含有具有重复性C-O键的循环和聚.
- 这些C-O键的选择性解对于利用生物质至关重要.
- 开发高效和有选择性的催化剂用于C-O债券裂变仍然是一个挑战.
研究的目的:
- 开发一种选择性催化剂,用于生物质衍生化合物中二次C-O键的解.
- 为了阐明涉及酸和金属站点的双功能机制.
- 了解氧化在碳催化剂上的中促进氧化的作用.
主要方法:
- 合成和表征ReO(x) 促进的Rh/C催化剂.
- 氨的温度编程脱吸 (NH 3 TPD) 用于量化酸性位点.
- 密度函数理论 (DFT) 计算来研究反应机制.
- 测试循环和聚的解中的催化剂选择性.
主要成果:
- 由ReO(x) 促进的Rh/C催化剂对二次C-O键解具有很高的选择性.
- NH(3) TPD证实了表面酸性部位的存在,其密度为40μmol g(-1).
- DFT计算表明,上的酸基组通过碳离子中间体促进了C-O键激活.
结论:
- 催化剂通过一种双功能机制运作,将酸催化环开放/脱水与金属催化化相结合.
- 氧化的促进增强了Rh/C催化剂活性和C-O解的选择性.
- 这项工作为设计用于生物质价值化新型双功能催化剂提供了机制性见解.
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