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Synergistic Effect of Boron Nitride and Carbon Domains in Boron Carbide Nitride Nanotube Supported Single‐Atom Catalysts for Efficient Nitrogen Fixation
Author(s) -
Liu Tianyong,
Dang Qian,
Zhou Xunhui,
Li Jin,
Ge Zhen,
Che Hang,
Tang Shaobin,
Luo Yi,
Jiang Jun
Publication year - 2021
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.202005182
Subject(s) - catalysis , boron nitride , materials science , vacancy defect , nitride , boron , selectivity , redox , nanotechnology , chemistry , inorganic chemistry , crystallography , organic chemistry , layer (electronics)
Developing the low‐cost and efficient single‐atom catalysts (SACs) for nitrogen reduction reaction (NRR) is of great importance while remains as a great challenge. The catalytic activity, selectivity and durability are all fundamentally related to the elaborate coordination environment of SACs. Using first‐principles calculations, we investigated the SACs with single transition metal (TM) atom supported on defective boron carbide nitride nanotubes (BCNTs) as NRR electrocatalysts. Our results suggest that boron‐vacancy defects on BCNTs can strongly immobilize TM atoms with large enough binding energy and high thermal/structural stability. Importantly, the synergistic effect of boron nitride (BN) and carbon domains comes up with the modifications of the charge polarization of single‐TM‐atom active site and the electronic properties of material, which has been proven to be the essential key to promote N 2 adsorption, activation, and reduction. Specifically, six SACs (namely V, Mn, Fe, Mo, Ru, and W atoms embedded into defective BCNTs) can be used as promising candidates for NRR electrocatalysts as their NRR activity is higher than the state‐of‐the art Ru(0001) catalyst. In particular, single Mo atom supported on defective BCNTs with large tube diameter possesses the highest NRR activity while suppressing the competitive hydrogen evolution reaction, with a low limiting potential of −0.62 V via associative distal path. This work suggests new opportunities for driving NH 3 production by carbon‐based single‐atom electrocatalysts under ambient conditions.