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

Yao Yao1; Minhua Shao1,6; Haijiang Wang3,4,5; Hui Li2,4,5

2020

10.1002/anie.202003071

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION   影响因子和分区

1433-7851

1521-3773

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. N2Hx (0 <= x <= 2) is detected with a N=N stretching mode at approximate to 2020 cm(-1) 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 N2H2 and its subsequent decomposition in the electrolyte producing NH3. Our results also indicate that nitrate reduction and the NRR share the same reaction intermediate N2Hx.

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

SCI ; EI

英语

NI期刊 ; NI论文

通讯

Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001]

Chemistry

Chemistry, Multidisciplinary

WOS:000526877600001

WILEY-V C H VERLAG GMBH

20201808588061

Electrocatalysts ; Light absorption ; Nitrates ; Mass spectrometry ; Reduction ; Gas adsorption ; Absorption spectroscopy ; Ammonia ; Electrolytes ; 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

CHEMISTRY

Web of Science

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

Yao Yao,Minhua Shao,Haijiang Wang,et al. A Spectroscopic Study of Nitrogen and Nitrate Electrochemical Reduction on Rhodium Surfaces[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020,59(26):10479-10483.

Yao Yao,Minhua Shao,Haijiang Wang,&Hui Li.(2020).A Spectroscopic Study of Nitrogen and Nitrate Electrochemical Reduction on Rhodium Surfaces.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,59(26),10479-10483.

Yao Yao,et al."A Spectroscopic Study of Nitrogen and Nitrate Electrochemical Reduction on Rhodium Surfaces".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 59.26(2020):10479-10483.