点击次数：

论文类型：期刊论文

发表时间：2019-01-21

发表刊物：PHYSICAL CHEMISTRY CHEMICAL PHYSICS

收录刊物：SCIE

卷号：21

期号：3

页面范围：1110-1116

ISSN号：1463-9076

摘要：N-2 fixation is one of the most challenging tasks in chemistry. Recently, tremendous efforts have been devoted to transition metal-based materials. However, metal-free catalysts for N-2 conversion have been rarely explored. Here, by using density functional theory, we predict, for the first time that a single B-atom decorated BN edge (B@BN) can act as a metal-free catalyst for the conversion of an N-2 molecule to NH3 under ambient conditions. N-2 fixation on the B@BN edge exhibits an extremely low overpotential of only 0.13 V through a distal mechanism. Moreover, fast removal of the produced NH3 molecule is observed with an uphill Gibbs free energy change of only 0.35 V, which is lower than those of ever-reported electrocatalysts such as Mo-doped BN and 2D Mxene. Our findings highlight a novel single atom metal-free catalyst for N-2 fixation, providing a cost-efficient process for sustainable NH3 production.