Materials Informatics-Guided Superior Electrocatalyst: A Case of Pyrolysis-Free Single-Atom Coordinated with N-Graphene Nanomesh
Materials Informatics-Guided Superior Electrocatalyst: A Case of Pyrolysis-Free Single-Atom Coordinated with N-Graphene Nanomesh
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DOI：
10.1016/j.nanoen.2021.106868
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发表时间：
2021-12
期刊：
影响因子：
17.6
通讯作者：
Wei Xia;Z. Hou;Jing Tang;Jingjing Li;Watcharop Chaikittisilp;Yena Kim;Koki Muraoka;Hongjuan Zhang-Hongjuan
中科院分区：
文献类型：
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作者：
Wei Xia;Z. Hou;Jing Tang;Jingjing Li;Watcharop Chaikittisilp;Yena Kim;Koki Muraoka;Hongjuan Zhang-Hongjuan
在这项工作中，我们应用材料信息学(MI)技术来预测纳米多孔碳基电催化剂的氧还原反应(ORR)的性能，该反应是质子交换膜燃料电池和金属-空气电池中的一个关键但反应缓慢的反应。通过MI技术确定了掺氮石墨烯纳米网格(NGM)是一种合适的ORR催化剂，为通过无裂解途径制备设计的氮配位单原子催化剂提供了有用的支持。本论文通过在金属间化合物导向的金属间化合物NGM上锚定FePc制备了结构可预测的单原子催化剂(FePc/NGM)。通过FePc中的Fe-N4部分与NGM石墨烯中的氮之间的轴向相互作用，将FePc与碳基质上的无规生成的Fe-Nx基团进行了比较。合成了对ORR具有较高催化活性的Fe-N5。精心设计的FePc/NGM具有突出的电催化活性，这是因为它的低维结构以及FePc的Fe3D轨道与NGM的氮轨道在轴向上的重新杂化引起的电子结构和几何结构的显著变化。这项工作表明，实验与材料信息学的融合对于无机合成化学的实践是不可或缺的。
In this work, we apply materials informatics (MI) techniques for property prediction of nanoporous carbon-based electrocatalyst for oxygen reduction reaction (ORR), which is a key, but sluggish reaction in proton exchange membrane fuel cells and metal–air batteries. Nitrogen-doped graphene nanomesh (NGM) was identified as an appropriate ORR catalyst by the MI techniques, which is a useful support to producing designed nitrogen-coordinated single-atom catalysts via pyrolysis-free pathway. Herein, single-atom catalysts (FePc/NGM) with predictable structures were fabricated by anchoring iron phthalocyanine (FePc) on the MI-guided NGM. Compared with the randomly creating Fe-Nxmoieties on a carbon matrix via pyrolysis, FePc were riveted onto NGM via axial interactions between Fe-N4moieties in FePc and nitrogen in NGM graphene matrix. As a result, Fe-N5with superior catalytic activity for ORR was created. The elaborately designed FePc/NGM possesses an outstanding electrocatalytic activity owing to its low-dimensional structure and the significant change in electronic and geometric structures arising from the rehybridization of Fe 3d orbitals from FePc with the nitrogen orbitals from NGM at the axial direction. This work demonstrates that fusion of experiments with material informatics is indispensable for the practice of the inorganic synthetic chemistry.