The doping and oxidation of 2D black and blue phosphorene: a new photocatalyst for nitrogen reduction driven by visible light. Issue 44 (4th November 2019)

• Record Type: Journal Article
• Authors: Cheng, Yuwen; Song, Yan; Zhang, Yumin
• Is Part Of: Physical chemistry chemical physics. Volume 21:Issue 44(2019)
• Page Start: 24449
• Page End: 24457
• Publication Date: 2019-11-04
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/c9cp04647j
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : Boron doping and the oxidation of black and blue phosphorene can achieve improved N2 reduction reaction performances using sunlight. Abstract : The synthesis of NH3 under ambient conditions using solar energy is the most attractive method of synthesis, and requires efficient and stable photo-catalysts with ultralow overpotentials, because a low overpotential ensures low energy consumption and a high yield of NH3 . Here, by using density functional theory calculations, the catalytic activity enhancements from B decoration and the oxidation of black and blue phosphorene for N2 fixation photo-catalysis are predicted. The results show that the computed overpotentials ( η NRR ) were 0.78 and 0.92 V through the end-on configuration of the B doped black phosphorene (B-Bl P) and blue phosphorene (B-Be P), respectively. In addition, owing to the reduction of the band gap, decoration with B can greatly enhance the visible light and infrared light harvesting of Bl P and Be P, guaranteeing them as ideal potential materials for the visible light reduction of N2 . The formation energy of B decoration and the ab initio molecular dynamics simulation results indicate that B-Bl P and B-Be P are highly stable under ambient conditions (300 K). The oxidation of the Bl P and Be P surfaces can also enhance the N2 reduction reaction (NRR) performances using visible light driving, with the η NRR values being 1.31 and 1.51 V through the end-on and side-on configurations, respectively. In summary, this work offers the opportunity for decorated phosphorene to act as a photo-catalyst for NH3 production.