在水溶液中进行选择性CH4-to-C2转换的协调定制的原子接口
1Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion, School of Chemistry and Chemical Engineering, Shandong University, Qingdao, PR China.
Nature communications
|October 15, 2025
概括
这项研究在碳化物气凝上引入了Fe二原子催化剂,用于在温和条件下选择性氧化甲到酸. 新的Fe-O2-Fe接口实现了高选择性和生产率,为工业应用铺平了道路.
科学领域:
- 催化科学是一种催化科学.
- 材料科学是一种材料科学.
- 绿色化学是一种绿色化学.
背景情况:
- 选择性甲氧化成有价值的化学物质是一个重大挑战.
- 为了能源效率和可持续性,需要温和的反应条件.
- 双原子催化剂为化学转换提供了独特的活性场所.
研究的目的:
- 开发和描述具有O2桥接铁二原子接口的Fe双原子催化剂 (Fe-DAC/g-C3N4).
- 在温和条件下研究选择性甲氧化成乙酸的机制.
- 在甲转化中实现高性能和选择性.
主要方法:
- 在碳化物气凝上支持Fe双原子催化剂的合成.
- 使用先进技术对Fe-O2-Fe接口进行表征.
- 对甲氧化反应动力学和机制的实验研究.
- 在环境和工业相关压力下的性能评估.
主要成果:
- 成功构建了Fe-O2-Fe二原子接口,具有精确的Fe-Fe距离 (2.92 ± 0.05 Å).
- 在温和条件下实现近100%的选择性用于酸生产.
- 在环境条件下证明了0.79 mmol gcat-1 h-1的CH3COOH生产率.
- 在1.5 MPa CH4下观察到1.67 mmol gcat-1 h-1 的生产率,具有>96%的选择性.
结论:
- 通过O2桥接的Fe二原子接口对于激活甲C-H键至关重要.
- 一个涉及激素中间体和C-C合的协调机制导致选择性酸的形成.
- 开发的Fe-DAC/g-C3N4催化剂在工业甲价值化方面表现出卓越的性能.
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