单个原子-纳米集群协同作用场所的接口修改,以打破选择性化中的活动-选择性-稳定性权衡
Zemin Chen1, Chufei Wang1, Boning Zhang2
1Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
协同作用的单原子和集群位点 (M1+Mn) 的界面修改优化了电子结构,以增强选择性化. 在催化中,这种策略打破了活动-选择性-稳定性权衡.
科学领域:
- 不同质的催化剂.
- 材料科学 材料科学 材料科学
- 表面化学 表面化学
背景情况:
- 协同作用的单原子和集群站点 (M1+Mn) 显示出在催化过程中克服线性缩放关系的潜力.
- 在M1+Mn站点中,金属实体和未经探索的支接口的空间分离限制了优化和结构属性分析.
- 接口在M1+Mn协同作用站点的中间吸附转移动力学中发挥着关键作用.
研究的目的:
- 为M1+Mn协同作用站点提出和研究一个界面修改策略.
- 调节M1+Mn站点的接口和电子结构,以提高催化性能.
- 探索选择性化过程中界面性质和催化活性之间的关系.
主要方法:
- 系统地改变单原子和集群站点 (Pd1+Pdn) 的支持接口,从酸 (HAP) 改为化碳改性酸 (NC/HAP) 和纯酸.
- 使用修改的Pd1+Pdn位点对基的半化中的催化活性和选择性的评估.
- 使用Pd1+Pdn站点的d频段中心作为描述符来阐明结构-活动相关性的全面调查.
主要成果:
- 观察到Pd1+Pdn接口和化活性之间的火山类相关性,在NC/HAP上具有峰值性能.
- 通过Pd1+Pdn@NC/HAP实现了醇转化为醇的优越活性,达到3707.7mol Pd-1h-1的形成速度,具有97.2%的选择性.
- 确定了Pd1+Pdn位点的d波段中心作为选择性化中火山类型相关性的描述符.
结论:
- 对Pd1+Pdn位点的界面修改优化了电子结构,基质吸附-脱吸动力学和H溢出.
- 该战略有效地打破了在异质催化中活动-选择性-稳定性权衡.
- 这项工作为设计用于选择性转换的先进协同催化场所提供了新的途径.
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