在液态金属催化剂上观察到对二氧化碳减排的高选择性的原子尺度解释
Charlie Ruffman1, Krista G Steenbergen2, Nicola Gaston1
1MacDiarmid Institute for Advanced Materials and Nanotechnology and Department of Physics, University of Auckland, Private Bag, 92019, Auckland, New Zealand.
液体金属催化剂,如-和-锡合金,使得二氧化碳 (CO2) 的选择性电化学减少能够形成. 这种反应性源于液体表面的移动吸附气,而不是固态.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 计算化学的计算化学
背景情况:
- 低温的液体金属,特别是- (Ga-In) 和-锡 (Ga-Sn) 合金,对于电化学减少二氧化碳 (CO2) 形成具有很高的选择性 (>95%).
- 这种选择性催化只能在液态中观察到,而不是合金是固体时.
研究的目的:
- 阐明液体Ga-In和Ga-Sn合金增强的二氧化碳减排选择性背后的机制.
- 研究表面动力学和吸附在催化过程中的作用.
主要方法:
- 密度函数理论 (DFT) 分子动力学模拟.
- 超动力学模拟用于探索反应路径和能量障碍.
主要成果:
- 二氧化碳通过与吸附 (Hads) 的反应间接减少,而不是直接吸附.
- 反应障碍在 (In) 或锡 (Sn) 位点 (0.26 eV) 与 (Ga) 位点 (0.47 eV) 相比较较低.
- 吸附的流动性在固体表面是有限的,但在液体表面是显著的,由液体运动驱动,方便进入In/Sn站点.
结论:
- 液体金属表面的动态运动对于实现低障碍二氧化碳减排至关重要.
- 催化活性与吸附物种在液体金属上的移动性有关,而不是固态和液态之间的固有差异.
- 这些发现对使用液态金属催化剂的质子化反应具有广泛的影响.
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