Lithium-mediated nitrogen reduction on two-dimensional MN4-contained periodical macrocyclic structures: A DFT study

IF 2.8 3区化学 Q3 CHEMISTRY, PHYSICAL

Chemical Physics Letters Pub Date : 2025-05-28 DOI:10.1016/j.cplett.2025.142189

Xin Tong , Yanjun Chen , Liujiang Zhou , Huilong Dong

引用次数: 0

Abstract

In this work, the two-dimensional MN4-contained periodical macrocyclic structures, namely, metal-embedded poly-porphyrins (MPPor) and poly-nitrided phthalocyanines (MPNPc), were computationally proposed as cathode catalysts for the lithium-mediated nitrogen reduction (Li-NR). The combined screening on N₂ adsorption and free energy profiles during Li-NR catalysis demonstrated that ScPNPc and FePPor are the suitable candidates. Particularly, the ScPNPc exhibits the lowest discharge overpotential (0.22 V) and the narrowest overall overpotential (0.50 V) along the side-on pathway. Moreover, the screened ScPNPc and FePPor show enhanced catalytic activity than the as-reported MPPcs, ascribing to the modulation effect from the outer coordination environment on the single-atom center.

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含mn4的二维周期大环结构上锂介导的氮还原：DFT研究

在这项工作中，二维含mn4的周期性大环结构，即金属嵌入的聚卟啉（MPPor）和多氮化酞菁（MPNPc），被计算为锂介导的氮还原（Li-NR）的阴极催化剂。通过对Li-NR催化过程中N2吸附和自由能谱的综合筛选，表明ScPNPc和FePPor是合适的候选材料。特别是，ScPNPc在侧通通路上表现出最低的放电过电位（0.22 V）和最小的总过电位（0.50 V）。此外，筛选的ScPNPc和FePPor的催化活性比报道的MPPcs强，这是由于外配位环境对单原子中心的调制作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemical Physics Letters 化学-物理：原子、分子和化学物理

CiteScore

5.70

自引率

3.60%

发文量

798

审稿时长

33 days

期刊介绍： Chemical Physics Letters has an open access mirror journal, Chemical Physics Letters: X, sharing the same aims and scope, editorial team, submission system and rigorous peer review. Chemical Physics Letters publishes brief reports on molecules, interfaces, condensed phases, nanomaterials and nanostructures, polymers, biomolecular systems, and energy conversion and storage. Criteria for publication are quality, urgency and impact. Further, experimental results reported in the journal have direct relevance for theory, and theoretical developments or non-routine computations relate directly to experiment. Manuscripts must satisfy these criteria and should not be minor extensions of previous work.