Karmodak Naiwrit, Nørskov Jens K
CatTheory Center, Dept. of Physics, Technical University of Denmark, 2800, Kongens Lyngby, Denmark.
Current affiliation: Department of Chemistry, Shiv Nadar Institute of Eminence, Greater Noida, 201314, India.
Angew Chem Int Ed Engl. 2023 Nov 20;62(47):e202311113. doi: 10.1002/anie.202311113. Epub 2023 Oct 16.
Efficient and inexpensive catalysts for the O reduction reaction (ORR) are needed for the advancement of renewable energy technologies. In this study, we designed a computational catalyst-screening method to identify single and di-atom metal dopants from first-row transition elements supported on defect-containing nitrogenated graphene surfaces for the ORR. Based on formation-energy calculations and micro-kinetic modelling of reaction pathways using intermediate binding free energies, we have identified four potentially interesting single-atom catalysts (SACs) and fifteen di-atom catalysts (DACs) with relatively high estimated catalytic activity at 0.8 V vs RHE. Among the best SACs, MnNC shows high stability in both acidic and alkaline media according to our model. For the DACs, we found four possible candidates, MnMn, FeFe, CoCo, and MnNi doped on quad-atom vacancy sites having considerable stability over a wide pH range. The remaining SACs and DACs with high activity are either less stable or show a stability region at an alkaline pH.
可再生能源技术的发展需要高效且廉价的氧还原反应（ORR）催化剂。在本研究中，我们设计了一种计算催化剂筛选方法，以从负载在含缺陷的氮化石墨烯表面的第一行过渡元素中识别单原子和双原子金属掺杂剂用于ORR。基于形成能计算以及使用中间结合自由能的反应途径的微观动力学建模，我们已识别出四种潜在有趣的单原子催化剂（SAC）和十五种双原子催化剂（DAC），在相对于可逆氢电极（RHE）为0.8 V时具有相对较高的估计催化活性。在最佳的SAC中，根据我们的模型，MnNC在酸性和碱性介质中均显示出高稳定性。对于DAC，我们发现了四种可能的候选物，即掺杂在四原子空位位点上的MnMn、FeFe、CoCo和MnNi，它们在很宽的pH范围内具有相当的稳定性。其余具有高活性的SAC和DAC要么稳定性较差，要么在碱性pH下显示出一个稳定区域。
