Choi, Changhyeok Gu, Geun Ho Noh, Juhwan Park, Hyun S. Jung, Yousung 2024-01-19T14:30:47Z 2024-01-19T14:30:47Z 2021-10-21 2021-07 2041-1723 https://pubs.kist.re.kr/handle/201004/116812 A key challenge to realizing practical electrochemical N-2 reduction reaction (NRR) is the decrease in the NRR activity before reaching the mass-transfer limit as overpotential increases. While the hydrogen evolution reaction (HER) has been suggested to be responsible for this phenomenon, the mechanistic origin has not been clearly explained. Herein, we investigate the potential-dependent competition between NRR and HER using the constant electrode potential model and microkinetic modeling. We find that the H coverage and N-2 coverage crossover leads to the premature decrease of NRR activity. The coverage crossover originates from the larger charge transfer in H+ adsorption than N-2 adsorption. The larger charge transfer in H+ adsorption, which potentially leads to the coverage crossover, is a general phenomenon seen in various heterogeneous catalysts, posing a fundamental challenge to realize practical electrochemical NRR. We suggest several strategies to overcome the challenge based on the present understandings. Practical electrochemical N-2 reduction reaction is challenged by competing side reactions. Here a combination of DFT and mikrokinetic modelling reveals the potential-dependent competition between electrochemical ammonia production and hydrogen evolution on a single-site iron catalyst embedded in N-doped graphene. English Nature Publishing Group Understanding potential-dependent competition between electrocatalytic dinitrogen and proton reduction reactions Article 10.1038/s41467-021-24539-1 1 Nature Communications, v.12, no.1 Nature Communications 12 1 Y scie scopus 000677489800006 2-s2.0-85110585621 Multidisciplinary Sciences Science & Technology - Other Topics Article ELECTROCHEMICAL AMMONIA-SYNTHESIS FINDING SADDLE-POINTS SINGLE-ATOM CATALYSTS ELASTIC BAND METHOD AMBIENT CONDITIONS OXYGEN REDUCTION DOPED GRAPHENE N-2 FIXATION NITROGEN ELECTROREDUCTION 전기화하 촉매 질소 암모니아