Enhancing Catalytic Properties of Iron- and Nitrogen-Doped Carbon for Nitrogen Reduction through Structural Distortion: A Density Functional Theory Study
Enhancing Catalytic Properties of Iron- and Nitrogen-Doped Carbon for Nitrogen Reduction through Structural Distortion: A Density Functional Theory Study
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DOI：
10.1021/acs.jpcc.1c04510
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发表时间：
2021-07
期刊：
影响因子：
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通讯作者：
Weitao Shan;Guofeng Wang
中科院分区：
文献类型：
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作者：
Weitao Shan;Guofeng Wang
在这项研究中，我们进行了第一性原理密度泛函理论计算预测的影响，结构畸变的Fe，N共掺杂碳（Fe-N-C）的催化性能的氮还原反应（NRR）。在嵌入石墨烯层的FeN 4和FeN 3位点上，我们的研究结果表明，压缩应变不仅增强了NRR活性，表现为NRR限制电位的正向变化，而且还将有利的NRR途径从混合路径改变为远端路径。活性增强归因于NRR中间物种 *NNH在应变活性位点上的强结合。此外，我们预测，在FeN 4和FeN 3网站上的NRR选择性提高了压缩应变引起的结构畸变。因此，我们的计算结果表明，可以调节Fe-N-C催化剂的石墨烯层中的压缩应变程度，以提高其对NRR的催化活性和选择性。
In this study, we have performed the first-principles density functional theory calculations to predict the influence of structural distortion on the catalytic properties of Fe, N codoped carbon (Fe–N–C) for the nitrogen reduction reaction (NRR). On both FeN4and FeN3sites embedded in a graphene layer, our results show that compressive strain not only enhances the NRR activity manifested by a positive change in NRR limiting potential, but also changes the favorable NRR pathway from a hybrid path to a distal one. The activity enhancement is attributed to the strong binding of NRR intermediate species, *NNH, on the strained active sites. Moreover, we predict that the NRR selectivity on both FeN4and FeN3sites is improved by the structural distortion induced by compressive strain. Hence, our computational results suggest that the degree of compressive strain in the graphene layer of Fe–N–C catalysts could be tuned to enhance their catalytic activity and selectivity for NRR.