通过协调工程来操纵Cu单个原子位点的d轨道,用于的选择性氧化
Shuchun Li1, Changsheng Cao1, Jiabin Chen2
1Key Laboratory of Advanced Carbon-Based Functional Materials (Fujian Province University), Fuzhou University, Fuzhou, 350016, Fujian, China.
Nature communications
|July 2, 2025
概括
我们通过操纵d轨道来设计铜单原子催化剂 (SAC),以实现高效的-氧化. 这种轨道工程增强了利用过氧化的催化活性和选择性.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 表面化学 表面化学
背景情况:
- 单原子催化剂 (SAC) 提供原子级控制,但缺乏轨道级操纵用于催化转向.
- 直接将转化为的氧化是至关重要的,但选择性和高效地进行氧化具有挑战性.
研究的目的:
- 为了在铜SAC中实现轨道水平的控制,以增强氧化.
- 开发一个双参数优化策略,涉及轨道配置和站点密度.
主要方法:
- 铜SAC的d轨道工程形成Cu-N3协调.
- 高金属负载 (33.2重量%) Cu SAC合成.
- 在现场ATR-IR光谱和密度函数理论 (DFT) 计算.
主要成果:
- 三协调的Cu SAC (Cu-N3-33.2) 实现了85.8%的转化率和680.3h-1的周转频率在60°C.
- 动态形成的Cu-O中间体中的p-d轨道杂交降低了H2O2激活屏障0.98 eV.
- 高密度的原子Cu位点通过消耗单片氧 (1O2) 抑制过度氧化.
结论:
- Cu SACs的轨道工程能够精确控制选择性氧化的催化行为.
- 结合轨道配置和地点密度的双参数方法重新定义了SAC设计原则.
- 这项工作介绍了一种高效的催化系统,用于使用H2O2.2,直接氧化到.
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