Ambient electrocatalytic nitrogen reduction on a MoO2/graphene hybrid: experimental and DFT studies. Issue 16 (18th July 2019)

• Record Type: Journal Article
• Authors: Wang, Jing; Liu, Ya-ping; Zhang, Hu; Huang, Da-jian; Chu, Ke
• Is Part Of: Catalysis science & technology. Volume 9:Issue 16(2019)
• Page Start: 4248
• Page End: 4254
• Publication Date: 2019-07-18
• Subjects: Catalysis -- Periodicals; 541.395
• DOI: 10.1039/c9cy00907h
• Languages: English
• ISSNs: 2044-4753

Abstract

Abstract : A combination of experimental measurements and DFT calculations revealed that the MoO2 /RGO hybrid could be a highly active and robust catalyst for ambient electrocatalytic NH3 synthesis. Abstract : Rational design of effective electrocatalysts toward the N2 reduction reaction (NRR) is essential for achieving high-efficiency electrocatalytic NH3 synthesis. Herein, a hybrid catalyst of MoO2 nanoparticles on reduced graphene oxide (MoO2 /RGO) was developed to catalyze the NRR under ambient conditions. Electrochemical measurements demonstrated that MoO2 /RGO presented a high NRR activity with an NH3 yield of 37.4 μg h −1 mg −1 and a faradaic efficiency of 6.6% at −0.35 V ( vs. RHE) in 0.1 M Na2 SO4, comparable to or exceeding those of most reported NRR electrocatalysts. Density functional theory calculations disclosed that the MoO2 /RGO hybrid possessed stronger electronic interactions with *N2 H and donated more electrons from active Mo sites to *N2 H relative to MoO2 alone, largely reducing the energy barrier for *N2 H formation, which was the potential-determining step of the NRR process. These results highlight the promising potential of the hybridization strategy and MoO2 /RGO hybrid for applications in ambient electrocatalytic NH3 synthesis.