邻近的sp-混合碳参与 CuO/Graphdiyne 亚纳米集群的分子氧激活
Chuanqi Pan1, Chenyang Wang1, Xinya Zhao1
1Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.
Journal of the American Chemical Society
|March 9, 2022
概括
使用石墨烯中的sp混合碳开发了分子氧激活的高活性催化剂. 这一突破使低温一氧化碳的有效氧化成为可能,
科学领域:
- 材料科学
- 催化剂
- 表面化学
背景情况:
- 分子氧 (O2) 激活是许多氧化反应的基础.
- 开发高效稳定的O2激活催化剂对于工业应用至关重要.
- 具有独特的sp混合碳结构的Graphdiyne提供了新的催化性能.
研究的目的:
- 研究在石墨烯中使用sp混合碳作为电子捐赠剂,用于开发分子氧激活的高活性催化剂.
- 探索 CuO/graphdiyne 亚纳米集团对一氧化碳 (CO) 氧化的催化性能.
- 阐明CuO/graphdiyne界面上的O2激活和CO氧化机制.
主要方法:
- 分纳米集团CuO/石墨烯催化剂的合成.
- 对CO氧化的催化活性进行评估.
- 在现场扩散反射红外里埃变换光谱 (in situ DRIFTS).
- 密度函数理论 (DFT) 的计算.
主要成果:
- 纳米集团CuO/石墨烯催化剂表现出卓越的CO氧化活性,在约133°C时转化50%的CO.
- 这种活性明显高于CuO/石墨烯和CuO/活性碳催化剂.
- DFT和in situ DRIFTS证实,邻近的sp混合碳站点可以在没有能量屏障的情况下快速分离碳酸盐.
- 碳氧化反应通过Eley-Rideal (E-R) 机制进行,低能障碍为0.20 eV.
结论:
- 石墨烯中的sp-混合CC三重键作为有效的电子捐赠者,增强分子氧激活.
- 具有邻近sp混合的C和Cu站点的CuO/graphdiyne子纳米集的接口是桥接模式中高效的O2激活的关键.
- 基于Graphdiyne的材料显著提高了O2激活效率,为有效的低温氧化过程铺平了道路.
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