了解Fe和Mo位点之间的协同作用在生物灵感双金属MXene电催化剂上的酸盐减少反应中
Daniel F Abbott1, Yuan-Zi Xu1, Denis A Kuznetsov2
1Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1-5, 8093, Zürich, Switzerland.
Angewandte Chemie (International ed. in English)
|October 31, 2023
概括
铁替代的碳化物 (Mo2 CTx:Fe) 有效地催化了酸盐降解为氨. 这种MXene材料模仿天然酶,为可持续的转化提供了一个有希望的途径.
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
- 催化剂是一种催化剂.
背景情况:
- 大自然利用含有 (Mo) 和铁 (Fe) 的酶来减少酸盐和酸盐.
- 开发模仿这些酶过程的合成催化剂对于可持续的管理至关重要.
研究的目的:
- 为了研究酸盐还原反应 (NO3 RR) 使用一个Fe替代的碳化物MXene (Mo2 CTx:Fe).
- 了解Mo2 CTx:Fe在将酸盐转化为 (NH4+) 的催化机制和性能.
主要方法:
- 在酸性和中性介质中进行电催化酸盐还原实验.
- 在现场的X射线吸收光谱 (XAS) 来探测催化过程中的表面变化.
- 密度函数理论 (DFT) 计算以阐明反应机制和活性位点.
主要成果:
- Mo2 CTx:Fe对NO3 RR表现出显著的NH3产率和法拉第效率 (FE),在中性介质中达到70%FE和12.9μmol h-1 mg-1.
- 用Fe替代的MXene的性能优于单金属Mo2CTx,这归因于表面终端组 (Tx) 的减少性功能丧失.
- 在现场的XAS和DFT计算显示,Fe位点促进了表面氧空缺的形成,这些空缺作为酸盐结合和减少的活性位点.
结论:
- 用Fe替代的Mo2 CTx MXene是一种有效的电催化剂,用于将酸盐减少为氨.
- 通过加入Fe来增强催化活性,这有助于创建氧空缺活性位点.
- 该机制与天然Mo基酸盐还原酶的机制非常相似,突出显示了转换的生物仿真方法.
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