论文标题
用于电化学氨合成的单原子催化剂的稳健活性位点设计
Robust Active Site Design of Single Atom Catalysts for Electrochemical Ammonia Synthesis
论文作者
论文摘要
在这项工作中，我们将使用单原子系统作为氨合成的示例材料类提供了一个计算方法学框架，该类别可用于参数选择。 Applying this to Pt$_1$/g-C$_3$N$_4$, Ru$_1$/g-C$_3$N$_4$, and Fe$_1$/g-C$_3$N$_4$, we generate ensembles of limiting potentials, using the ensemble of functionals collected via Bayesian Error Estimation Functionals (BEEF), to robustly predict catalytic activity.然后，我们将其扩展为研究NRR反应中间体之间的尺度，并使用它来识别NNH*作为这些关系的最佳描述符。此外，概述了调查选择性的程序，并提出了一种更强大的分析选择性权衡权衡的方法。对于这个单原子材料类别，我们发现选择位于活性火山的强大结合腿上的催化剂值得进一步探索。鉴于易于将所提出的方法集成到最低的额外计算成本，我们认为这应该成为多电子电化学反应的分析工作流程的常规部分。
In this work, we provide a computational methodological framework using the single-atom systems as an example material class for ammonia synthesis that is robust towards parameter selection. Applying this to Pt$_1$/g-C$_3$N$_4$, Ru$_1$/g-C$_3$N$_4$, and Fe$_1$/g-C$_3$N$_4$, we generate ensembles of limiting potentials, using the ensemble of functionals collected via Bayesian Error Estimation Functionals (BEEF), to robustly predict catalytic activity. We then extend this to study the scaling between NRR reaction intermediates and use it to identify that NNH* as the best descriptor for these relations. In addition, a procedure to investigate selectivity is outlined, and a more robust way to analyze the selectivity-activity trade-off is presented. For this single-atom material class, we find choosing catalysts that lie on the strong binding leg of the activity volcano are worth further exploration. Given the ease of integration of the proposed method with minimal additional computational cost, we believe this should become a routine part of analysis workflow for multi-electron electrochemical reactions.
