Single-metal-atom site with high-spin state embedded in defective BN nanosheet promotes electrocatalytic nitrogen reduction. Hexagonal boron nitride nanosheet for effective ambient N 2 fixation to NH 3. Review of electrochemical ammonia production technologies and materials. Beyond fossil fuel-driven nitrogen transformations. Catalytic synthesis of ammonia-A “never-ending story”?. Transformation of the nitrogen cycle: Recent trends, questions, and potential solutions. How a century of ammonia synthesis changed the world. We hope our work will promote experimental synthesis of these NRR electrocatalysts and provide new opportunities to the electrochemical conversion of N 2 to NH 3 under ambient conditions. Band structures, projected density of states, and charge/spin distributions show that the high catalytic activity is due to significant orbital hybridizations and charge transfer between N 2 and MPP catalysts. Through comprehensive reaction path search, the maximum Gibbs free energy changes for NRR on the ZrPP (enzymatic-consecutive hybrid path), NbPP (consecutive path), HfPP (enzymatic-consecutive hybrid path), and RePP (distal path) catalysts are 0.38, 0.41, 0.53, and 0.53 eV, respectively. Four novel metalloporphyrin (MPP, M = Zr, Nb, Hf, and Re) single-atom catalyst candidates have been identified due to their excellent catalytic performance (low onset potential, high stability, and selectivity). We systematically investigated the catalytic performance of 3d, 4d, and 5d transition metals anchored onto two-dimensional extended porphyrin (PP) substrates as nitrogen reduction reaction (NRR) electrocatalysts, employing density functional theory (DFT) calculations and four-step high-throughput screening.
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