在Co-Based双原子催化剂上从CO2和NO中进行甲基胺电合成的机械洞察
Tianze Xu1, Zifan Wang1, Tianyang Liu1
1Jiangsu Co-Innovation Centre of Efficient Processing and Utilization of Forest Resources, College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China.
通过了解单原子/双原子催化剂的C-N合机制,从二氧化碳和氧化物中进行甲基胺 (MMA) 的电化学合成. 对于高效的MMA生产,Co-Ir-Pc是有前途的.
科学领域:
- 催化剂
- 电化学
- 计算化学
背景情况:
- 甲基胺 (MMA) 是一个重要的工业化学物质.
- 电化学合成为使用二氧化碳和氧化物生产MMA提供了新的途径.
- 由于复杂的机制,实现选择性C-N合仍然存在挑战.
研究的目的:
- 阐明基于Co-phthalocyanine (Co-Pc) 的单原子/双原子催化剂 (SAC/DAC) 的MMA电合成机制.
- 确定控制C-N合选择性的关键因素.
- 引导有效的MMA电合成催化剂的合理设计.
主要方法:
- 恒定潜在密度函数理论 (DFT) 的计算.
- 微动力学模拟
- 吸附的分析,能量障碍,以及中间减少的自由能量.
主要成果:
- 确定了C-N合选择性的三个关键因素:CO2/NO吸附,初始LH阶段屏障和中间过度减少.
- 同基DAC比SAC的表现优越.
- 作为DAC设计的关键,强调过渡金属的亲和力.
结论:
- 2D Co-Ir-Pc是MMA生产的一个有前途的电催化剂,其性能优于Co-Pc单体.
- 提供了关于SAC/DAC的C-N合的机制见解.
- 建立了用于MMA电合成的合理催化剂设计框架.
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