具有可调节的催化反应性的异金属CeIV/ VV氧气集群
Xingjie Wang1, Kieran Brunson2, Haomiao Xie1
1International Institute for Nanotechnology and Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States.
Journal of the American Chemical Society
|December 7, 2021
概括
新的Ce12V6氧集群具有可调节的配体显示增强的氧化还原催化. 有机配体提高溶解性和多孔性,提高选择性硫化物氧化等应用的反应性.
科学领域:
- 无机化学
- 材料科学
- 催化剂
背景情况:
- 异金属氧气集群为氧化还原催化提供协同性能.
- (CeIV) /金属 (M) 聚合物是未被充分探索但有前途的催化材料.
研究的目的:
- 设计和合成新的Ce12V6氧基团,使用不同的封装配体.
- 研究这些集群的结构,电子和催化性质.
主要方法:
- 单晶X射线衍射 (SCXRD) 用于结构阐明.
- 用于表征的光谱技术 (红外线,紫外线,ESI-MS,1H NMR,51V NMR).
- 用小角度X射线散射 (SAXS) 来确认溶液的完整性.
- 通过选择性氧化二乙烯硫化物 (CEES) 进行催化试验.
主要成果:
- 用硫酸,硫酸 (OTs) 和硫酸 (NBSA) 连接物成功合成了三种Ce12V6氧基团.
- 结构分析证实了 [Ce12(VO) 6O24]18+ 的古巴核.
- 在OTs和NBSA变体中,连接物功能化增强了溶解性,并引入了多孔性.
- 催化研究表明,随着催化部位的可访问性增加,反应性得到改善.
结论:
- 有机配体引入是一种可行的策略,以提高无机硫酸盐覆盖集群的性能.
- 调节可溶性和多孔性是优化催化活性的关键因素.
- 这些Ce12V6集群显示出作为高效的氧化还原催化剂的潜力.
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