DOI码：

10.1021/jacs.9b01375

发表刊物：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

刊物所在地：

WASHINGTON

摘要：

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.

合写作者：

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

第一作者：

Hu, Canyu

通讯作者：

Long, R, Xiong, YJ

论文编号：

WOS:000468366900024

文献类型：

Article

卷号：

141

期号：

19

页面范围：

7807-7814

ISSN号：

0002-7863

是否译文：

否