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首页> 外文期刊>Journal of Materials Chemistry, A. Materials for energy and sustainability >The rational design of single-atom catalysts for electrochemical ammonia synthesisviaa descriptor-based approach
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The rational design of single-atom catalysts for electrochemical ammonia synthesisviaa descriptor-based approach

机译：电化学氨合成血清描述符的单原子催化剂的合理设计

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摘要

Single-atom catalysts (SACs) have been widely studied in electrocatalysis towards renewable energy conversion. Herein, we present a general descriptor-based strategy for the rational design of SACsviadensity functional theory calculations. Taking the electrochemical nitrogen reduction reaction (NRR) as an example, we firstly revealed the scaling relations for adsorption energies of intermediates on a series of 4-B (MB4), 4-C (MC4) and 4-N (MN4) coordinated SACs. Based on this, the activity of the NRR was described by the adsorption free energy of *NH. It's found that MB4, MC(4)and MN(4)followed the same volcano curve of activity, where FeB(4)was optimal with a limiting potential of -0.55 V. On MB4, the H adsorption energies were weaker than on widely studied MC(4)and MN(4)due to the highly occupied H 1s-d antibonding state, which resulted in a higher NRR selectivity of MB4. More strikingly, kinetic calculations suggested that the activation energy of the NRR (0.99 eV) is lower than that of the HER (1.10 eV) on FeB(4)at 0 Vvs.RHE, and hence the ammonia production should be more feasible than hydrogen evolution on FeB4. This work not only reported MB(4)as a potential NRR electrocatalyst, where FeB(4)was the most outstanding, but also generalized the descriptor-based approach to the rational design of widely studied SACs.
机译：单颗粒催化剂（SAC）已广泛研究了可再生能量转化的电常见。这里，我们提出了一种基于描述符的基于描述符的Sacsviadenty功能理论计算的理性设计策略。以电化学氮还原反应（NRR）为例，我们首先揭示了一系列4-B（MB4），4-C（MC4）和4-N（MN4）协调的囊的中间体的吸附能量的扩大关系。基于此，NRR的活性由* NH的吸附无能量描述。发现MB4，MC（4）和Mn（4）遵循相同的活性Volcano曲线，其中2月份（4）是最佳的-0.55 V.在MB4上的电位，H吸附能量弱于广泛由于高占用的H 1S-D抗抗抗抗体状态研究了MC（4）和Mn（4），导致MB4的NRR选择性较高。更引人注目的是，动力学计算表明，NRR（0.99eV）的激活能量低于2月（4）时的NRR（1.10eV），在0VVS.RHE中，因此氨生产应比氢更可行Evolution在2月4日。这项工作不仅报告了MB（4）作为潜在的NRR电催化剂，于2月（4）是最优秀的，而且还推广了基于描述符的基于描述的方法的广泛研究的囊的理性设计。

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