在支持的纳米粒子催化剂上的H2氧化:在金属支持接口上的异质H2激活的证据
Todd Whittaker1, K B Sravan Kumar2, Christine Peterson1
1Department of Chemistry , Trinity University , San Antonio , Texas 78212-7200 , United States.
金属支接口 (MSI) 的水对催化非常重要. 这项研究揭示了H2激活通过MSI的异质解离发生,解释了水
科学领域:
- 不同质的催化
- 表面科学
- 计算化学
背景情况:
- 金属支接口 (MSI) 的水对催化反应有显著的影响.
- 了解水的作用对于优化CO优先氧化 (CO PrOx) 等过程至关重要.
研究的目的:
- 在Au/TiO2和Au/Al2O3催化剂上,在水的存在下研究H2氧化动力学.
- 阐明在MSI中的H2激活机制.
主要方法:
- 对H2氧化的实验动力学研究.
- 使用支持的Au纳米模型进行密度函数理论 (DFT) 计算.
- 在化Au/TiO2上进行红外光谱实验.
主要成果:
- 在MSI中通过异质解离迅速发生H2激活,在Au上形成化物,在支上形成质子.
- 微弱吸附的水通过阻断MSI位点起到显著的抑制作用.
- H2激活动力学与传统的分离化学吸收模型有所不同.
结论:
- 在MSI提出了一种新的异质H2激活机制,并得到实验和计算数据的支持.
- 质子介导的路径占主导地位,传统的布伦斯特德-埃文斯波兰尼关系被改变.
- 这种机制解释了水的抑制作用及其在CO PrOx催化中的有益作用.
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