过渡金属d轨道在单原子催化剂中对于氧化电还原到氨的作用
Lingyan Kong1, Xiongyi Liang1, Maohuai Wang1
1Department of Materials Science and Engineering, City University of Hong Kong, Tat Chee Avenue, Hong Kong Special Administrative Region.
研究人员开发了高效的催化剂,用于从氧化中电化学合成氨. 嵌在碳化中的白金对这种双重效益的NO去除和氨生产过程具有很大的前景.
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
- 电化学 电化学 电化学
背景情况:
- 越来越多的人对从氧化 (NO) 中电化学合成氨 (NH3) 感兴趣,以同时生产NH3和去除NO.
- 在设计有效的催化剂来实现这种直接NO-to-NH3电还原方面,仍然存在挑战.
研究的目的:
- 选和识别嵌入碳化物 (PC) 单层中的高活性过渡金属催化剂,用于NO-to-NH3电还原.
- 阐明过渡金属d轨道在NO激活中的作用,并建立这些催化剂的设计原则.
主要方法:
- 密度函数理论 (DFT) 的计算用于在PC单层中选十种过渡金属 (TM) 候选物.
- 机器学习辅助的理论计算,以了解TM-d轨道对NO激活的影响.
- 综合选包括表面稳定性,选择性,动力障碍和热稳定性.
主要成果:
- 确定了十个有前途的TM嵌入式PC (TM-PC) 候选者,用于NO-to-NH3电还原.
- 揭示了TM-d轨道的V形调整规则,控制吉布斯的自由能量和限制潜力.
- 由于高可行性和催化性能,Pt嵌入式PC单层成为最有前途的催化剂.
结论:
- 嵌入Pt的PC单层是直接NO-to-NH3电还原的非常有前途的催化剂.
- 该研究提供了对NO转换中基于PC的单原子催化剂的活性起源和设计原理的见解.
- 这项工作为同时去除NO和合成氨提供了一个可行的策略.
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