Journal
JOURNAL OF COLLOID AND INTERFACE SCIENCE
Volume 606, Issue -, Pages 204-212Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2021.08.032
Keywords
Electrocatalytic N-2 reduction; Metal-free electrocatalysts; Heterostructure; Density functional theory
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Funding
- Natural Science Foundation of Gansu Province [20JR10RA241]
- Central Government Guides Local Science and Technology Development Project [206Z1003G]
- Key Project of Education Department of Hebei Province [ZD2020339]
- Hebei North University General Project [YB2020004]
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Researchers have developed a metal-free BNQDs/C3N4 heterostructure catalyst with outstanding performance in N-2 reduction reaction, surpassing nearly all previously reported metal-free catalysts.
Exploring high-efficiency metal-free electrocatalysts towards N-2 reduction reaction (NRR) is of great interest for the development of electrocatalytic N-2 fixation technology. Herein, we combined boron nitride quantum dots (BNQDs) and graphitic carbon nitride (C3N4) to design a metal-free BNQDs/C3N4 heterostructure as an effective and durable NRR catalyst. The electronically coupled BNQDs/C3N4 presented an NH3 yield as high as 72.3 mu g h(-1) mg(-1) (-0.3 V) and a Faradaic efficiency of 19.5% (-0.2 V), far superior to isolated BNQDs and C3N4, and outperforming nearly all previously reported metal-free catalysts. Theoretical computations unveiled that the N-2 activation could be drastically enhanced at the BNQDs-C3N4 interface where interfacial BNQDs and C3N4 cooperatively adsorb N-2 and stabilize *N2H intermediate, leading to the significantly promoted NRR process with an ultra-low overpotential of 0.23 V. (C) 2021 Elsevier Inc. All rights reserved.
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