新方法设计高效仿生触媒

最近，常州大学教授吴大禹和合肥物质科学研究院的团队提出了一种简单的机械策略，通过机械诱导的自旋跳跃（SCO）优化催化中心的电子结构，并实现了设计高效仿生触媒的新方法。

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近年来，过渡金属催化剂的合成受到广泛关注。然而，为了改善催化活性/选择性，亟需在原子级精确控制催化中心的电子结构。

吴大禹的团队通过自旋跳跃调控铁催化活性中心的部分自旋跳跃，使混合自旋（MS）纳米片触媒的CO产率达到19.7毫摩尔/克，选择性达到91.6%，远高于高自旋对应物。

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该研究使用了中国稳定高磁场设施（SHMFF）的实验条件来证实催化活性中心的自旋跳跃。密度泛函理论（DFT）计算表明，低自旋3d轨道的电子配置有效增加了O-2p和Fe-3dxy/dyz之间的键合轨道重叠，从而显著促进了CO2的选择性吸附。然而，高自旋3d轨道通过3dz2反键轨道与O-2p轨道重叠，极大地削弱了催化剂和底物之间的键合作用，降低了催化活性。

此外，该研究还通过DFT计算计算了自旋催化背后的物理化学机制。该研究为开发高活性、廉价、环保的CO2还原催化剂奠定了基础，进一步为解决当前能源和环境危机、实现双碳目标提供了重要保障。

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该研究成果已发表在《应用化学国际版》上。

原文链接：https://phys.org/news/2023-04-method-efficient-biomimetic-catalysts.html

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