对于基化石墨烯支持的双原子催化剂上的二氧化碳减少产品的理论理解
Chunyuan Feng1, Lixiang Zhong1
1School of Physics, Beijing Institute of Technology, Beijing, 100081, China. zhonglx@bit.edu.cn.
Physical chemistry chemical physics : PCCP
|April 14, 2025
概括
在基化石墨烯上的双原子催化剂显示出减少二氧化碳的前景. 然而,对于多碳产品的C-C合在能源上是不利的,阻碍了实验实现. 本研究确定了甲和甲醇等C1产品的催化剂.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 计算化学计算化学
背景情况:
- 用添加的石墨烯支持的双原子催化剂 (DAC@NC) 正在积极研究二氧化碳还原反应 (CO2RR).
- 使用DAC从CO2RR中合成所需的C1和C2产品的实验合成仍然具有挑战性.
- 以前的理论研究提出了DAC结构,但实验验证是有限的.
研究的目的:
- 系统地研究二金属DAC@NC (M1-M2@NC) 上的二氧化碳减排途径和产品.
- 阐明阻碍多碳产品形成的能量障碍.
- 为了确定有希望的M1-M2@NC组合用于选择性CO2转换.
主要方法:
- 使用第一原则计算,研究各种双金属DAC@NC系统的二氧化碳减排.
- 被认为催化剂中毒和进化竞争排除了不适合的催化剂.
- 进行了自由能量计算,以分析反应路径和中间稳定性.
主要成果:
- C-C 合步骤始终表现出比化更高的自由能量增量,阻碍了多碳产品的形成.
- 对于大多数C1中间体,C-C合的自由能量障碍超过0.8 eV.
- 与化相比,C-C合的难度解释了通过实验实现C2产品的挑战.
结论:
- 化相对于C-C合的固有能量偏好限制了M1-M2@NC上的CO2RR中多碳化合物的产生.
- 这项研究提供了关于当前DAC@NC催化剂对CO2RR的局限性的基本见解.
- 特定的M1-M2@NC组合被确定为潜在有效的深度降低CO2到C1产品 (甲和甲醇).
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