具有β-转向偏差序列的催化中的二次结构多样性
Anthony J Metrano1, Nadia C Abascal1, Brandon Q Mercado1
1Department of Chemistry, Yale University , P.O. Box 208107, New Haven, Connecticut 06520-8107, United States.
Journal of the American Chemical Society
|December 29, 2016
概括
对四的结构分析揭示了多种构造,挑战了复杂反应的催化剂的设计和预测. 了解这些结构动态是开发有效催化剂的关键.
科学领域:
- 结构生物学
- 催化剂
- 计算化学
背景情况:
- 基于的催化剂为选择性化学转化提供了潜力.
- 了解形状对于催化剂设计至关重要.
- 之前的研究评估了四分的选择性化.
研究的目的:
- 为了研究四聚的结构.
- 将结构多样性与催化活性相关联.
- 探索对催化剂设计的影响.
主要方法:
- 用于固态结构的X射线晶体学.
- 用于计算分析的密度函数理论 (DFT).
- 核磁共振 (NMR) 光谱用于溶液结构的阐明.
主要成果:
- 35个四序列表现出不同的构造状态.
- 微妙的序列修改导致了显著的形状变化.
- 在多个序列中观察到多个符合性和多态性.
- 结晶和溶液结构的比较显示出形状的灵活性.
结论:
- 催化剂的构造空间比以前所认为的多样化.
- 多种基态构造和动态平衡使催化剂设计和过渡状态预测复杂化.
- 低阻碍性构造性相互转换可能有利于多步骤的反选择性反应.
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