Embedding Double Transition Metal Atoms in B-Modified Two-Dimensional Carbon-Rich Conjugated Frameworks for Efficient...

It is important to develop an efficient green catalyst for electrochemical nitrogen reduction under environmental conditions to replace the Haber-Bosch process with high energy consumption, limited economic scale of production, and high CO₂ emissions, but there are still some difficulties in its development and design. In this work, based on 2D CCFs, a B-modified rectangular-shaped expanded phthalocyanine bimetallic atomic catalyst is proposed. Because both the TM-d orbital and the B-sp³ hybrid orbital can accept the lone pair and feedback electrons of N₂, and there are significantly different valence electron distributions between the two different metals and boron, this catalyst not only keep the advantages of metal catalysts but also play the role of the B atom to further increase the polarity of nitrogen and activate N₂. In order to evaluate the catalytic performance of this catalyst, its stability, activity, selectivity, reactivity, and other aspects are screened and analyzed by density functional theory calculation. Among them, the FeNb-BPc CCF catalyst has better N₂ adsorption capacity under ambient conditions, exhibits excellent catalytic activity through a continuous mechanism, and has a lower limiting potential of -0.24 V. We believe that this work opens a new path for the rational design of efficient N₂ reduction reaction catalysts and also provides a theoretical basis for experimental development.