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温度依赖的选择性和检测隐藏的碳沉积在甲氧化过程中

Ulrike Küst^1,2, Weijia Wang³, Changda Wang⁴

¹Division of Synchrotron Radiation Research, Lund University, P.O. Box 118, SE-221 00 Lund, Sweden.

ACS catalysis

|April 25, 2024

概括

在甲氧化过程中,使用先进的光谱学发现了隐藏的碳沉积途径. 这项研究揭示了以前被忽视的影响催化剂活性的反应通道.

科学领域:

不同质的催化剂.
表面科学是一门科学.
化学反应工程化学反应工程

背景情况:

反应产物通常在催化剂表面或气相中观察到.
催化剂体内的溶解原子可以掩盖反应路径,导致低估碳沉积等现象.
碳沉积显著影响催化活性,特别是在碳化合物氧化过程中.

研究的目的:

开发和演示一种在异质催化中发现隐藏的沉积道的方法.
在 (Pd) 催化剂上对甲氧化过程中的碳沉积进行研究.
了解温度和氧气供应对反应通路的影响.

主要方法:

使用时间解析的环境压力X射线光电子谱学 (AP-XPS).
在直接在催化剂表面以上的气相中测量产品形成率.
在不同温度 (350525 °C) 和压力 (几毫巴) 的缺氧条件下对多晶Pd催化剂进行实验.

主要成果:

仅在氧气质量转移有限条件下观察到一氧化碳 (CO) 的产生.
数据表明,碳沉积甚至发生在氧气质量转移极限之外.
揭示了溶解的碳物种可以代表一个重要的,以前隐藏的反应途径.

结论:

时间解析的AP-XPS通过监测气相产物来有效检测隐藏的沉积道.
在Pd上甲氧化过程中的碳沉积比以前假设的更为普遍.
了解这些隐藏的途径对于准确评估和控制催化过程至关重要.

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