High‐performance BCN‐C heterostructured electrocatalyst derived from covalent triazine frameworks for nitrogen reduction

Abstract

AbstractDesigning and synthesizing heterostructure‐based catalysis combining two‐dimensional (2D) materials has attracted enormous attention in materials chemistry, especially for electrocatalysis, due to their tunable electronic properties and structure. In this work, a boron carbon nitride (BCN)‐coupled carbon (BCN‐C) heterostructure with improved electronic performance was synthesized starting from C‐ and N‐enriched 2D covalent triazine frameworks (CTFs) via a simple thermal transformation process using NaBH4 as the B source. The characterizations results showed that the B released from NaBH4 reacted with N and C in CTF, forming the BCN‐C heterostructure coupling the BCN and carbon with a strong interfacial effect. The electrocatalytic NRR experiments and density functional theory (DFT) calculation revealed that the interfacial electronic properties and large numbers of active sites of the BCN‐C heterostructure benefited the NRR. The BCN‐C‐1 catalyst showed a high Faradaic efficiency of 27.8% and an NH3 yield of 4.3 μg h−1 mgcat.−1 in 0.1 M HCl electrolyte, owing to its high specific surface area (288 m2/g) with a large number of exposed active sites and the Mott–Schottky effect from the BCN‐C heterostructure. This work highlights the design and synthesis of metal‐free catalysts with high activity and selectivity and makes them excellent candidates for electrocatalytic applications.