A Spectroscopic Study on the Nitrogen Electrochemical Reduction Reaction on Gold and Platinum Surfaces

Yao, Yao1,3; Zhu, Shangqian1; Wang, Haijiang4; Li, Hui3; Shao, Minhua1,2

2018-01-31

10.1021/jacs.7b12101

Journal of the American Chemical Society   影响因子和分区

0002-7863

The electrochemical reduction of nitrogen to ammonia on Au-based catalysts showed a reasonably high Coulombic efficiency. The pathway of this promising reaction, however, is not clear partially due to the lack of information on reaction intermediates. Herein, surface-enhanced infrared absorption spectroscopy (SEIRAS) was employed to study the reaction mechanisms of nitrogen reduction on an Au thin film for the first time. During the nitrogen reduction, the N2Hy species was detected with bands at 1453 (H-N-H bending), 1298 (-NH2 wagging), and 1109 cm(-1) (N-N stretching) at potentials below 0 V against reversible hydrogen electrode. This result indicates that the nitrogen reduction reaction on Au surfaces follows an associative mechanism, and the N N bond in N-2 tends to break simultaneously with the hydrogen addition. By comparison, no absorption band associated with N was observed on Pt surfaces under the same reaction condition. This result is consistent with the low efficiency of nitrogen reduction on Pt due to the much faster kinetics of hydrogen evolution reaction.

SCI ; EI

英语

NI期刊 ; NI论文 ; ESI高被引

其他

Shenzhen Key Laboratory project[ZDSYS201603311013489]

Chemistry

Chemistry, Multidisciplinary

WOS:000424313000047

AMER CHEMICAL SOC

20180604757299

Absorption spectroscopy ; Efficiency ; Electrolytic reduction ; Hydrogen ; Light absorption ; Nitrogen ; Platinum ; Reaction intermediates ; Reaction kinetics ; Spectroscopic analysis

Precious Metals:547.1 ; Light/Optics:741.1 ; Chemistry:801 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Production Engineering:913.1

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Kowloon, Hong Kong, Peoples R China
2.Hong Kong Univ Sci & Technol, Energy Inst, Kowloon, Hong Kong, Peoples R China
3.South Univ Sci & Technol China, Dept Mat Sci & Engn, 1088 Xueyuan Blvd, Shenzhen 518055, Guangdong, Peoples R China
4.South Univ Sci & Technol China, Dept Mech & Energy Engn, 1088 Xueyuan Blvd, Shenzhen 518055, Guangdong, Peoples R China

Yao, Yao,Zhu, Shangqian,Wang, Haijiang,et al. A Spectroscopic Study on the Nitrogen Electrochemical Reduction Reaction on Gold and Platinum Surfaces[J]. Journal of the American Chemical Society,2018,140(4):1496-1501.

Yao, Yao,Zhu, Shangqian,Wang, Haijiang,Li, Hui,&Shao, Minhua.(2018).A Spectroscopic Study on the Nitrogen Electrochemical Reduction Reaction on Gold and Platinum Surfaces.Journal of the American Chemical Society,140(4),1496-1501.

Yao, Yao,et al."A Spectroscopic Study on the Nitrogen Electrochemical Reduction Reaction on Gold and Platinum Surfaces".Journal of the American Chemical Society 140.4(2018):1496-1501.