A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces

Yao，Yao1,2; Zhu，Shangqian1; Wang，Haijiang3,4,5; Li，Hui2,4,5; Shao，Minhua1,6

2020

10.1002/ANGE.202003071

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

Rh is a promising electrocatalyst for the nitrogen reduction reaction (NRR) given its suitable nitrogen-adsorption energy and low overpotential. However, the NRR pathway on Rh surfaces remains unknown. In this study, we employ surface-enhanced infrared-absorption spectroscopy (SEIRAS) and differential electrochemical mass spectrometry (DEMS) to study the reaction mechanism of NRR on Rh. NH (0 ≤ x ≤ 2) is detected with a N=N stretching mode at ≈2020 cm by SEIRAS and a signal at m/z=29 by DEMS. A new two-step reaction pathway on Rh surfaces is proposed that involves an electrochemical process with a two-electron transfer to form NH and its subsequent decomposition in the electrolyte producing NH. Our results also indicate that nitrate reduction and the NRR share the same reaction intermediate NH.

differential electrochemical mass spectrometry nitrate reduction nitrogen reduction reaction reaction mechanism surface-enhanced infrared-absorption spectroscopy

EI

英语

其他

20223412618174

Absorption spectroscopy ; Ammonia ; Electrocatalysts ; Electrolytes ; Gas adsorption ; Light absorption ; Mass spectrometry ; Nitrates ; Reduction ; Spectroscopic analysis ; Surface reactions

Electric Batteries and Fuel Cells:702 ; Light/Optics:741.1 ; Chemistry:801 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2

MATERIALS SCIENCE

2-s2.0-85136208133

Scopus

1.Department of Chemical and Biological Engineering,The Hong Kong University of Science and Technology,Kowloon,Clear Water Bay,Hong Kong
2.Department of Materials Science and Engineering,South University of Science and Technology of China,Shenzhen,1088 Xueyuan Blvd, Nanshan District, Guangdong,518055,China
3.Department of Mechanical and Energy Engineering,South University of Science and Technology of China,Shenzhen,1088 Xueyuan Blvd, Nanshan District, Guangdong,518055,China
4.Shenzhen Key Laboratory of Hydrogen Energy,South University of Science and Technology of China,Shenzhen,1088 Xueyuan Blvd, Nanshan District, Guangdong,518055,China
5.Guangdong Provincial Key Laboratory of Energy Materials for Electric Power,South University of Science and Technology of China,Shenzhen,1088 Xueyuan Blvd, Nanshan District, Guangdong,518055,China
6.Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution,The Hong Kong University of Science and Technology,Kowloon,Clear Water Bay,Hong Kong

Yao，Yao,Zhu，Shangqian,Wang，Haijiang,et al. A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces[J]. ADVANCED MATERIALS,2020,132(26):10565-10569.

Yao，Yao,Zhu，Shangqian,Wang，Haijiang,Li，Hui,&Shao，Minhua.(2020).A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces.ADVANCED MATERIALS,132(26),10565-10569.

Yao，Yao,et al."A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces".ADVANCED MATERIALS 132.26(2020):10565-10569.