A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces.,Angewandte Chemie International Edition

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A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-03-23 , DOI: 10.1002/anie.202003071
Yao Yao _{1,

2} , Shangqian Zhu ₁ , Haijiang Wang _{3,

4,

5} , Hui Li _{2,

4,

5} , Minhua Shao _{1,

6}

Affiliation

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. N₂H_x (0≤x ≤2) is detected with a N=N stretching mode at ≈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 N₂H_x.

中文翻译：

铑表面电化学还原氮和硝酸盐的光谱研究。

Rh具有合适的氮吸附能和较低的超电势，是用于氮还原反应（NRR）的有前途的电催化剂。但是，Rh表面的NRR途径仍然未知。在这项研究中，我们采用表面增强红外吸收光谱法（SEIRAS）和差示电化学质谱法（DEMS）研究NRR在Rh上的反应机理。Ñ ₂ ħ _X（0≤ X ≤2）与在≈2020cm的N = N伸缩模式检测^-1通过SEIRAS和在信号米/ ž由DEMS = 29。提出了在Rh表面上的新的两步反应途径，该过程涉及具有两电子转移以形成N ₂ H ₂的电化学过程及其随后在产生NH ₃的电解质中的分解。我们的结果还表明，硝酸盐还原和NRR具有相同的反应中间体N ₂ H _x。

更新日期：2020-03-23

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