AUTHOR=Wang Yuan , Qian Xu , Zheng Guokui , Tian Ziqi , Zhang Qiuju 

TITLE=Boron-Doped MXenes as Electrocatalysts for Nitrogen Reduction Reaction: A Theoretical Study

JOURNAL=Frontiers in Chemical Engineering

VOLUME=3

YEAR=2021

URL=https://www.frontiersin.org/journals/chemical-engineering/articles/10.3389/fceng.2021.702129

DOI=10.3389/fceng.2021.702129

ISSN=2673-2718

ABSTRACT=<p>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 <italic>d</italic>-orbitals (<italic>J. Am. Chem. Soc.</italic>, 2019, 141 (7), 2884), it is supposed to be able to effectively activate the triple bond in N<sub>2</sub>. 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<sub>4</sub>C<sub>3</sub>O<sub>2</sub>, B@Ti<sub>4</sub>N<sub>3</sub>O<sub>2</sub>, and B@Ti<sub>3</sub>N<sub>2</sub>O<sub>2</sub> 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.</p>