基于三酸盐的石墨碳化物支持的单原子催化剂的计算选,用于1,2-二乙烯脱
Huanglan Xue1, Yu Huang1, Yi Li1,2
1State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350108, People's Republic of China.
The Journal of chemical physics
|August 26, 2025
概括
这项研究确定了1,2-二乙脱的最佳过渡金属催化剂,Fe@TGCN在乙生产中表现出色. 通过改变中间吸附和产品脱吸,基修饰增强了选择性.
科学领域:
- 材料科学
- 计算化学
- 催化剂
背景情况:
- 1,2-二乙烯 (1,2-DCE) 脱是环境修复和化学合成的关键反应.
- 开发用于选择性1,2-DCE脱的高效电催化剂仍然是一个重大挑战.
- 基于triazine的石墨碳化物 (TGCN) 为催化剂开发提供了一个有前途的支架.
研究的目的:
- 系统地研究1,2-DCE脱反应 (DCEDR) 的过渡金属原子加载TGCN (TM@TGCN).
- 确定适用于生成乙烯,乙烯和乙的催化剂.
- 阐明DCEDR的机制和催化剂修改的作用.
主要方法:
- 用密度功能理论 (DFT) 的计算来选八个TM@TGCN催化剂.
- 使用五步选方法来确定催化剂的性能.
- 研究了基修饰对催化剂选择性的影响.
主要成果:
- Fe@TGCN证明了将1,2-DCE降解为乙的最低限制潜力 (-0.47V对于 gauche-C2H4Cl2和-0.50V对于 trans-C2H4Cl2).
- Fe@TGCN与反应物的最佳相互作用由其位于火山图片顶部的位置证实.
- 通过减弱中间吸附和减少产品脱吸能量,基修饰增强了对乙烯的选择性.
结论:
- 铁@TGCN是一种高效的电催化剂,可选择性地将1,2-DCE脱为乙.
- 对于调整DCEDR选择性至关重要的是基功能化等基修饰策略.
- 这项研究为DCEDR设计先进的电催化剂提供了理论指导.
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