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使用PdAu的双金属催化剂中的吸附物诱导重组动力学的动态研究

Chen Zhou^1,2, Hio Tong Ngan³, Jin Soo Lim⁴

¹Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.

Journal of the American Chemical Society

|August 11, 2022

概括

像Pd/Au这样的双金属催化剂的动态重组是性能的关键. 这项研究揭示了CO诱导的表面变化和动力参数,使合金催化剂在适度条件下能够进行微调.

科学领域:

表面科学
催化剂
材料科学

背景情况:

双金属催化剂对于化学反应至关重要,其活性取决于表面的动态重组.
用一氧化碳 (CO) 和氧气等剂调节催化剂表面是一种有效的策略.
了解重组的机制和动力学至关重要,但由于复杂的变量而具有挑战性.

研究的目的:

通过先进的技术研究 (Pd) 在黄金 (Au) 上的in situ重组动态.
发现Pd/Au系统中CO诱导的重组的以前未知的时间尺度和动力参数.
提供对微调双金属催化剂表面的机制理解.

主要方法:

时间分辨率的温度编程红外反射吸收光谱 (TP-IRAS).
一开始的热力学计算.
机器学习分子动力学 (MLMD) 模拟

主要成果:

在高达373K的CO暴露后,Pd单体重新填充了表面.
在473K以上,Pd完全溶解到地下.
溶解的明显激活能被确定为0.14 eV和0.48 eV,重组发生在1000秒内.

结论:

作为一个探测器和重组Pd/Au111) 表面的代理.
这项研究阐明了合金催化剂在原子水平上的流动性.
已识别的动力参数在适度条件下提供了可控表面修改的机会.

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相关概念视频

Catalysis

Catalysis

The presence of a catalyst affects the rate of a chemical reaction. A catalyst is a substance that can increase the reaction rate without being consumed during the process. A basic comprehension of a catalysts’ role during chemical reactions can be understood from the concept of reaction mechanisms and energy diagrams.