Boron-Doped MXenes as Electrocatalysts for Nitrogen Reduction Reaction: A Theoretical Study
Yuan Wang, Qian Xu, Guokui Zheng, Ziqi Tian, Qiuju Zhang
Abstract
Electrocatalytic nitrogen reduction reaction (NRR) is a promising and sustainable approach for ammonia production. Since boron as an active center possesses electronic structure similar to that of transition metals with d -orbitals ( J. Am. Chem. Soc. , 2019, 141 (7), 2884), it is supposed to be able to effectively activate the triple bond in N 2 . MXenes can be applied as substrates due to the large specific surface area, high conductivity, and tunable surface composition. In this work, the catalytic performance of a series of MXenes-supported single boron atom systems (labeled as B@MXenes) has been systematically studied by using density functional theory (DFT). B@Nb 4 C 3 O 2 , B@Ti 4 N 3 O 2 , and B@Ti 3 N 2 O 2 were screened out owing to outstanding catalytic activity with limiting potentials of −0.26, −0.15, and −0.10 V, respectively. Further analysis shows that the unique property of boron that can intensely accept lone pair and back-donate the anti-bond of nitrogen contributes to the activation of inert triple bond. This work provides a new idea for the rational design of NRR catalyst and is of great significance for the future development of nitrogen reduction catalysts.