Surface Plasmon Enabling Nitrogen Fixation in Pure Water through a Dissociative Mechanism under Mild Conditions

DOI number:10.1021/jacs.9b01375

Journal:JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

Place of Publication:WASHINGTON

Abstract:Nitrogen fixation in a simulated natural environment (i.e., near ambient pressure, room temperature, pure water, and incident light) would provide a desirable approach to future nitrogen conversion. As the N N triple bond has a thermodynamically high cleavage energy, nitrogen reduction under such mild conditions typically undergoes associative alternating or distal pathways rather than following a dissociative mechanism. Here, we report that surface plasmon can supply sufficient energy to activate N-2 through a dissociative mechanism in the presence of water and incident light, as evidenced by in situ synchrotron radiation-based infrared spectroscopy and near ambient pressure X-ray photoelectron spectroscopy. Theoretical simulation indicates that the electric field enhanced by surface plasmon, together with plasmonic hot electrons and interfacial hybridization, may play a critical role in N N dissociation. Specifically, AuRu core-antenna nanostructures with broadened light adsorption cross section and active sites achieve an ammonia production rate of 101.4 mu mol g(-1) h(-1) without any sacrificial agent at room temperature and 2 atm pressure. This work highlights the significance of surface plasmon to activation of inert molecules, serving as a promising platform for developing novel catalytic systems.

Co-author:Hu, Canyu, Xing, Jin, Jianbo, Han, Yong, Chen, Shuangming, Ju, Huanxin, Cai, Jun, Qiu, Yunrui, Gao, Chao, Wang, Chengming, Qi, Zeming, Long, Ran, Song, Li, Liu, Zhi, Xiong, Yujie

First Author:Hu, Canyu

Correspondence Author:Long, R, Xiong, YJ

Document Code:WOS:000468366900024

Document Type:Article

Volume:141

Issue:19

Page Number:7807-7814

ISSN No.:0002-7863

Translation or Not:no