Impact of Active Site Density on Oxygen Reduction Reactions Using Monodispersed Fe–N–C Single-Atom Catalysts,ACS Applied Materials & Interfaces

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Impact of Active Site Density on Oxygen Reduction Reactions Using Monodispersed Fe–N–C Single-Atom Catalysts
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-03-19 , DOI: 10.1021/acsami.0c01206
Yulan Han ₁ , Qin-Kun Li ₂ , Ke Ye ₁ , Yi Luo ₁ , Jun Jiang ₁ , Guozhen Zhang ₁

Affiliation

Exploring the impact of active site density on catalytic reactions is crucial for reaching a more comprehensive understanding of how single-atom catalysts work. Utilizing density functional theory calculations, we have systematically investigated the neighboring effects between two adjacent Fe–N–C sites of monodispersed Fe–N–C single-atom catalysts on oxygen reduction reaction (ORR). While the thermodynamic limiting potential (U_L) is strongly dependent on the intersite distance and the nature of adjacent active sites in FeN₃, it is almost invariable in FeN₄ until two FeN₄ sites are ∼4 Å apart. Further, under certain conditions, an otherwise unfavorable physisorbed-O₂-initiated 2e^– pathway becomes feasible due to charge transfer between reactive species and graphene support. Our results cast new insight into the rational design of high-density single-atom catalysts and may create an alternative route to manipulate their catalytic activities.

中文翻译：

活性位点密度对单分散Fe–N–C单原子催化剂上氧还原反应的影响

为了更全面地了解单原子催化剂的工作原理，探索活性位点密度对催化反应的影响至关重要。利用密度泛函理论计算，我们系统地研究了单分散Fe–N–C单原子催化剂的两个相邻Fe–N–C位点之间的邻近效应对氧还原反应（ORR）的影响。尽管热力学极限电势（U _L）强烈取决于位点间的距离和FeN ₃中相邻活性位点的性质，但在FeN _4中几乎不变，直到两个FeN ₄位点相距〜4Å。此外，在某些条件下，一个不利否则物理吸附-O ₂ -引发2E ^-由于反应性物种和石墨烯载体之间的电荷转移，这种途径变得可行。我们的结果为高密度单原子催化剂的合理设计提供了新的见识，并可能为操纵其催化活性创造一条替代途径。

更新日期：2020-03-20

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