Developing efficient and light pollution electrocatalytic nitrogen reduction reaction (NRR) method for dinitrogen (N2) fixation is a very important and challenging issue in the field of energy and environment. However, the existing multiple-step screening methods for NRR electrocatalysts are inefficient, and it is urgent to search for suitable descriptor to shorten screening process. Herein, by density functional theory (DFT) calculation, the structures, electronic structures and NRR activity of TM3C24X12 (TM-X MOF, TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, and Mo, X = NH, and S) are investigated, and a descriptor relevant to magnetism Δ(μB_TM-μB_X) is proposed. An “inverted-volcano” relationship between Δ(μB_TM-μB_X) and ΔGN2→NNH reflects direct relevancy between the descriptor and N2 activation capability, leading the way to the two-step screening method. Mo-S MOF is predicted to be the best among catalysts prefer end-on N2 adsorption according to the descriptor, which is verified via a modified three-step screening method, showing that Mo-S MOF has a low limiting potential of −0.41 V and a satisfying activation energy of 0.85 eV in the determining step. The descriptor provides new thoughts for revealing the activity mechanism of 2D-MOF catalysts shortening the screening steps, and finding high-performance catalysts.

中文翻译：

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缩短筛选过程，转向高性能 2D-MOF NRR 电催化剂，以 [公式省略] 作为 N2 活化能力的描述符


开发高效、轻污染电催化氮还原反应 （NRR） 固定二氮 （N2） 是能源与环境领域中非常重要且具有挑战性的问题。然而，现有的 NRR 电催化剂多步筛选方法效率低下，亟需寻找合适的描述符以缩短筛选过程。本文通过密度泛函理论 （DFT） 计算，研究了 TM3C24X12 （TM-X MOF， TM = Sc， Ti， V， Cr， Mn， Fe， Co， Ni， Cu， Zn 和 Mo， X = NH， and S） 的结构、电子结构和 NRR 活性，并提出了与磁性 Δ（μ B_TM-μ B_X） 相关的描述符。Δ（μ B_TM-μ B_X） 和 ΔGN2→NNH 之间的“倒火山”关系反映了描述符和 N2 激活能力之间的直接相关性，为两步筛选方法开辟了道路。根据描述符，预测 Mo-S MOF 是首选端接 N2 吸附的催化剂中最好的，该描述符通过改进的三步筛选方法进行了验证，表明 Mo-S MOF 具有 -0.41 V 的低极限电位和 0.85 eV 的令人满意的活化能在确定步骤中。该描述符为揭示 2D-MOF 催化剂的活性机制、缩短筛选步骤和寻找高性能催化剂提供了新的思路。