Unveiling the Mechanism of Nitrogen Fixation by Single-Atom\nCatalysts and Dual-Atom Catalysts Anchored on Defective Boron Nitride\nNanotubes

Abstract

It\nis challenging to explore stable and high-efficiency electrocatalysts\ntoward nitrogen reduction reaction (NRR) under ambient conditions.\nHerein, the catalytic potential of boron nitride nanotubes (BNNTs)\nembedded with transition-metal (TM) atoms as electrocatalysts for\nNRR has been systematically studied by the first-principles calculation\nmethod. Three single-atom catalysts (SACs), Fe/BNNT, Mn/BNNT, and\nPd/BNNT, were selected out from 13 candidate materials TM/BNNT (TM\n= Fe, Co, Ni, Cu, Zn, Ti, V, Cr, Mn, Mo, Pt, Pd, and Au) by density\nfunctional theory (DFT) calculations, and their limiting potentials\nwere −0.65, −0.61, and −0.91 V, respectively.\nIt indicated that they have good catalytic activity for the reduction\nof N₂ to NH₃. Meanwhile, to further improve\nthe catalytic activity, two dual-atom catalysts (DACs), FeFe/BNNT\nand MnMn/BNNT, were constructed, their limiting potentials were −0.17\nand −0.58 V, respectively. The results show that FeFe/BNNT\nand MnMn/BNNT can greatly improve the catalytic performance. Our work\nprovides a new idea for constructing high-efficiency electrocatalysts\nwith BNNT as a new carrier.