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<p>Electro-catalytic nitrogen (N<sub>2</sub>) reduction reaction (NRR) is a highly efficient approach for synthesizing ammonia (NH<sub>3</sub>). Herein, we have designed a series of transition metal atom-based single-layer organic frameworks (TM<sub>3</sub>(C<sub>6</sub>O<sub>6</sub>)<sub>2</sub>) using density functional theory (DFT) calculations to systematically investigate their electro-catalytic performance for NRR. Our studies indicate that two-dimensional (2D) Re<sub>3</sub>(C<sub>6</sub>O<sub>6</sub>)<sub>2</sub> exhibits the most moderate N<sub>2</sub> activation and lowest limiting potential of − 0.31&#xa0;V among the 24 TM<sub>3</sub>(C<sub>6</sub>O<sub>6</sub>)<sub>2</sub> candidates. Also, Re<sub>3</sub>(C<sub>6</sub>O<sub>6</sub>)<sub>2</sub> can severely mitigate the competitive process of hydrogen evolution reaction (HER), which suggests remarkable performance regarding efficiency and selectivity of NRR. More interestingly, a feasible self-assembly strategy is proposed due to its suitable lattice matching compared with Cu(111) bulk, further contributing to its successful synthesis. This work may provide solid theoretical support for the rational design of outstanding electro-catalysts toward sustainable NH<sub>3</sub> synthesis.</p>

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Re3(C6O6)2 monolayer: a promising metal–organic framework-based electro-catalyst for N2 reduction reaction

  • 期刊论文

  • 发表日期：

    2025年1月22日

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  • Honglan Li,
  • Lei Yang,
  • Xinglin Yang

摘要

Electro-catalytic nitrogen (N2) reduction reaction (NRR) is a highly efficient approach for synthesizing ammonia (NH3). Herein, we have designed a series of transition metal atom-based single-layer organic frameworks (TM3(C6O6)2) using density functional theory (DFT) calculations to systematically investigate their electro-catalytic performance for NRR. Our studies indicate that two-dimensional (2D) Re3(C6O6)2 exhibits the most moderate N2 activation and lowest limiting potential of − 0.31 V among the 24 TM3(C6O6)2 candidates. Also, Re3(C6O6)2 can severely mitigate the competitive process of hydrogen evolution reaction (HER), which suggests remarkable performance regarding efficiency and selectivity of NRR. More interestingly, a feasible self-assembly strategy is proposed due to its suitable lattice matching compared with Cu(111) bulk, further contributing to its successful synthesis. This work may provide solid theoretical support for the rational design of outstanding electro-catalysts toward sustainable NH3 synthesis.