Computational Design of Two-Dimensional Boron-Containing Compounds as Efficient Metal-free Electrocatalysts toward Nitrogen Reduction Independent of Heteroatom Doping

• DOI: 10.1021/acsami.0c15872
• Publication Date: 2020-11-02T17:48:56Z
• Authors: Wei Nong; Haikuan Liang; Shihan Qin; Yan Li; Chengxin Wang
• Keywords: Heteroatom

As metal-free carbon based catalysts, boron (B)-doped carbonaceous materials have proved to exhibit superior catalytic performance toward nitrogen reduction reaction. However, this strategy of heteroatom doping encounters the synthesis challenges precise control level and homogeneous distribution dopants, in particular, these cannot be utilized electrochemical N2 because poor electrical conductivity. Accordingly, via first-principles calculations, we here predicted two stable two-dimensional crystalline compounds: BC6N2 BC4N, which small band gaps uniform NRR active sp2-B species holey structures. Between them, monolayer originally possesses nice activity with limiting potentials −0.47 V. In proton-rich acid medium, electronic properties B–C–N monolayers could further tailored a metallic characteristic by H pre-adsorption. This drastically improves conductivity enhances their performances as reflected −0.15, −0.34, −0.34 V for enzymatic, distal, alternating mechanisms, respectively. Besides, on BC4N through enzymatic mechanism proceeds potential moderated from −1.20 −0.90 More than that, competing hydrogen evolution reaction can effectively suppressed. The current investigation opens an avenue designing 2D phase MFC catalysts independent gives insightful views surface functionalization impactful improve electrocatalytic catalysts.