在Ni{110}上逆转水气转换或Sabatier甲化? 在近环境压力下稳定的表面物种
Matteo Roiaz1, Enrico Monachino1, Carlo Dri1,2
1Physics Department, University of Trieste , via Valerio 2, I-34127 Trieste, Italy.
Journal of the American Chemical Society
|March 9, 2016
概括
这项研究使用先进的光谱学揭示了 (110) 的复杂表面相互作用. 主要发现包括多种一氧化碳物种和反应性中间体的鉴定.
科学领域:
- 表面科学
- 催化剂
- 材料化学
背景情况:
- 了解金属催化剂的气体表面相互作用对于优化化学过程至关重要.
- 基催化剂广泛用于甲化和水气转移反应等工业应用.
- (110) 表面为基本表面化学研究提供了明确的模型系统.
研究的目的:
- 研究各种气体混合物 (CO,CO2,H2) 与 (110) 表面的相互作用.
- 在近环境条件下识别稳定的表面物种和反应中间体.
- 阐明二氧化碳在表面上的激活和转化机制.
主要方法:
- 现场红外可见总频率生成 (IR-vs-SFG) 振动光谱.
- 近环境压力X射线光电子光谱 (NAP-XPS).
- 在10~-1 mbar压力下进行可变温度研究 (300~525 K).
主要成果:
- 原子碳,石墨烯前体和五种不同的CO物种的识别.
- 有证据表明共吸收效应,H诱导的CO激活和表面重建.
- 碳酸盐物种和一个转基因稳定的活性CO2中介物的观察.
- 在表面的乙稳定性减去.
结论:
- 这项研究提供了关于上CO和CO2复杂表面化学的详细见解 (110).
- 已识别的中间体,如活性碳二氧化碳,对于理解逆水气转移和萨巴蒂尔甲化反应至关重要.
- 表面重建和共吸收在改变表面的反应性方面发挥着重要作用.
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