On the promising performance of single Ta atom in efficient nitrogen fixation

Summary The electrocatalytic nitrogen reduction reaction (NRR) with atomic Ta catalysts as supported by carbon materials is investigated using a combination of experiments and theoretical calculations. The Ta catalysts were prepared via photodeposition (Ta-GO) and impregnation (Ta-NC), respectively. Surprisingly, the Ta-GO catalyst exhibits excellent NRR efficiency with an ammonia yield rate of 19.97 μ g N H 3 h − 1 m g C a t . − 1 (14.26 m g N H 3 h − 1 m g T a − 1 ) and a Faraday efficiency (FE) of 8.52%. By contrast, the Ta-NC species exhibits lower atomic efficiency (yNH3 = 17.71 μ g N H 3 h − 1 m g C a t . − 1 [3.34 m g N H 3 h − 1 m g T a − 1 ]) but higher NRR selectivity (FE = 17.86%). The reaction mechanisms have been revealed by computation, based on which the electronic origins for the performances of atomic Ta at different coordination environments are discussed. This work demonstrates the potential of Ta to conduct an efficient NRR process, and the promising electronic structure for constructing highly efficient Ta catalysts is discussed.