Electrocatalytic nitrogen reduction reaction(NRR)is an environmentally friendly method for sustainable ammonia synthesis under ambient conditions.Searching for efficient NRR electrocatalysts with high activ-ity and selectivity is currently urgent but remains great challenge.Herein,we systematically investigate the NRR catalytic activities of single and double transition metal atoms(TM=Fe,Co,Ni and Mo)an-chored on g-C6N6 monolayers by performing first-principles calculation.Based on the stability,activity,and selectivity analysis,Mo2@g-C6N6 monolayer is screened out as the most promising candidate for NRR.Further exploration of the reaction mechanism demonstrates that the Mo dimer anchored on g-C6N6 can sufficiently activate and efficiently reduce the inert nitrogen molecule to ammonia through a preferred distal pathway with a particularly low limiting potential of-0.06V.In addition,we find that Mo2@g-C6N6 has excellent NRR selectivity over the competing hydrogen evolution reaction,with the Faradaic efficiency being 100％.Our work not only predicts a kind of ideal NRR electrocatalyst but also encouraging more ex-perimental and theoretical efforts to develop novel double-atom catalysts(DACs)for NRR.

Jiajun Wang;Mengyao Shi;Guolin Yi;Lu Wang;Shulai Lei;Ke Xu;Shujuan Li;Jianshuai Mu

Tianjin Key Laboratory of Structure and Performance for Functional Molecules,College of Chemistry,Tianjin Normal University,Tianjin 300387,China;Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices,Hubei University of Arts and Science,Xiangyang 441053,China;Institute of Mathematics,Free University of Berlin,Berlin D-14195,Germany

中国化学快报（英文版）

[1]Jiajun Wang;Mengyao Shi;Guolin Yi;Lu Wang;Shulai Lei;Ke Xu;Shujuan Li;Jianshuai Mu-.Computational prediction of Mo2@g-C6N6 monolayer as an efficient electrocatalyst for N2 reduction)[J].中国化学快报（英文版）,2022(10):4623-4627

C6N6,chored,06V

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