过渡金属双原子催化剂的合理设计在缺陷的h-BN中用于CO2化和循环添加
Tairen Long1, Yue Zhang2, Zexing Cao1
1State Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 360015, China.
ACS applied materials & interfaces
|August 24, 2025
概括
双原子催化剂 (DAC) 在转化二氧化碳 (CO2) 成为化学物质方面具有前景. 这项研究设计了用于二氧化碳化和循环添加的M1-P1/VBN催化剂,表现出极好的催化性能.
科学领域:
- 材料科学
- 催化剂
- 计算化学
背景情况:
- 二氧化碳 (CO2) 转化对于应对能源和环境挑战至关重要.
- 双原子催化剂 (DAC) 为有效利用二氧化碳提供了一个有前途的途径.
- 缺陷的六角化物 (h-BN) 为单原子催化剂提供了稳定的支.
研究的目的:
- 在理论上设计和研究用于二氧化碳转化的新型M1-P1/VBN催化剂.
- 探索二氧化碳热化成酸 (HCOOH) 和二氧化碳循环添加与氧化物 (PO) 碳酸盐 (PC) 的催化机制.
- 评估设计的DAC的催化性能,反应途径和稳定性.
主要方法:
- 使用第一原理计算 (DFT) 来研究电子结构和反应机制.
- 在各种条件下使用微动力学模拟来评估催化活性.
- 进行稳定性分析以确认M1-P1/VBN系统的稳定性.
主要成果:
- 设计了M1-P1/VBN催化剂,其中包括缺陷的h-BN上的单一过渡金属 (Ir,Rh,Co) 和.
- 双活性金属位有效地激活和吸附关键反应分子 (CO2,H2,PO).
- 在CO2化中Co1-P1/VBN表现出色,而在温和条件下Rh1-P1/VBN在CO2循环添加中表现高.
结论:
- 设计的M1-P1/VBN催化剂具有卓越的二功能催化活性,可利用二氧化碳.
- 在金属类型,小分子的结合强度和吸附自由能量之间观察到强烈的相关性.
- 这项研究为开发高效的二氧化碳转化技术提供了先进的理论见解.
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