有协同作用的RuCo原子对,对levulinic酸化有增强的活性
Haonan Zhang1, Yuhang Sun1, Shuo Wang1
1School of Chemical Engineering and Environment, China University of Petroleum, Beijing 102249, China.
Journal of colloid and interface science
|November 28, 2024
概括
一种新型的RuCo-NC双单原子催化剂 (DSAC) 有效地将酸 (LA) 转化为γ-黄 (GVL). 这种催化剂设计克服了传统催化剂的局限性,为这一重要的化反应提供了增强的活性.
科学领域:
- 不同质的催化剂.
- 材料科学是一种材料科学.
- 绿色化学是一种绿色化学.
背景情况:
- 为了生物质的价值化,有效地将氨酸 (LA) 转化为γ-氨酸 (GVL) 是至关重要的.
- 基于 (Ru) 的催化剂对H2解离是有效的,但受到大颗粒的固态阻碍,限制了LA化活性.
- 需要先进的催化剂设计来克服这些局限性并改善GVL生产.
研究的目的:
- 开发一种基于金属的新型催化剂,用于高效地将氨酸 (LA) 化成γ-黄 (GVL).
- 为了研究原子Ru和 (Co) 对在双单原子催化剂 (DSAC) 结构中的协同效应.
- 了解控制增强催化性能的原子级机制.
主要方法:
- 理性设计和合成一个Ru和Co合的地质化伊米达框架 (RuCo合的ZIF-8) 前体.
- 前体的热解形成Ru1Co1NC双单原子催化剂 (DSAC) 与N3Ru1Co1N3协调.
- 对LA化和密度函数理论 (DFT) 计算进行实验性催化测试,以阐明反应机制.
主要成果:
- Ru1Co1NC DSAC显示了LA化到GVL的突出的催化活性,实现了1980h-1.1的周转频率 (TOF).
- 催化剂设计促进了协同作用的Ru-Co原子对的形成,增强了H2解离和CO激活.
- DFT的计算证实,由Co诱导的富含电子的Ru和双原子对中的原子Ru是提高性能的关键.
结论:
- 与传统的基于Ru的催化剂相比,Ru1Co1NC DSAC的性能优越,用于将LA化为GVL.
- 协同作用的Ru和Co的原子对能够精确控制活性点,从而提高催化效率.
- 这项工作通过控制原子级活站点工程来设计高性能催化剂的新策略.
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