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Published on: August 18, 2020
Dual Active Sites Enhanced Plasmon-Driven N2 Photoreduction Over MoO3-X Nanosheets Under Visible Excitation
Huaiwei Zhang1, Liang Bao1, Ying Pan1
1College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou, P. R. China.
Abstract:
Nitrogen photo-fixation used solar energy as a prospective way, has received more attention. In this study, a series of Ru-C/MoO3-x photocatalysts with enhanced localized surface plasmon resonance effects for N2 photo-fixation are developed, which not only construct abundant adsorption active sites but also promote the photocatalytic performances through reducing the N≡N bond dissociation activation energy. Notably, an additional LSPR peak at around 490 nm is observed in the UV-vis DRS spectra upon the introduction of the Ru element. Furthermore, increased N2 adsorption capacity and more efficient carrier separation are obtained via the carbon decoration over the catalysts. Among these, the highest ammonia production rate over the Ru-C co-decorated photocatalyst achieves 864 µmol·gcal -1·h-1. Furthermore, a markedly apparent quantum efficiency exceeding 1.9% is achieved under visible light excitation at 420 nm, representing one of the highest values ever reported for photocatalytic N2 fixation over metal oxide catalysts. Density functional theory calculations illustrate that the photocatalytic nitrogen reduction reaction follows the distal pathway, and the Ru/C composite activity sites in the samples can decrease the energy barrier in the rate-controlling step to further enhance the N2 photoreduction.

