A Spectroscopic Study of Electrochemical Nitrogen and Nitrate Reduction on Rhodium Surfaces
Top Cited Papers
- 21 June 2020
- journal article
- research article
- Published by Wiley in Angewandte Chemie-International Edition
- Vol. 59 (26), 10479-10483
- https://doi.org/10.1002/anie.202003071
Abstract
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.Funding Information
- Shenzhen Peacock Plan (KQTD2016022620054656)
- Development and Reform Commission of Shenzhen Municipality (1106)
- Guangdong Province Introduction of Innovative R&D Team (2016ZT06N500)
- Innovation and Technology Commission (ITC-CNERC14EG03)
This publication has 40 references indexed in Scilit:
- Rational design of electrocatalysts and photo(electro) catalysts for nitrogen reduction to ammonia (NH3) under ambient conditionsEnergy & Environmental Science, 2018
- Electrification and Decarbonization of the Chemical IndustryJoule, 2017
- Photon-Driven Nitrogen Fixation: Current Progress, Thermodynamic Considerations, and Future OutlookACS Catalysis, 2017
- Au Sub‐Nanoclusters on TiO2 toward Highly Efficient and Selective Electrocatalyst for N2 Conversion to NH3 at Ambient ConditionsAdvanced Materials, 2017
- Combining theory and experiment in electrocatalysis: Insights into materials designScience, 2017
- Electrochemical Reduction of N2 under Ambient Conditions for Artificial N2 Fixation and Renewable Energy Storage Using N2/NH3 CycleAdvanced Materials, 2016
- Photoprompted Hot Electrons from Bulk Cross-Linked Graphene Materials and Their Efficient Catalysis for Atmospheric Ammonia SynthesisACS Nano, 2016
- Selective Dinitrogen Conversion to Ammonia Using Water and Visible Light through Plasmon‐induced Charge SeparationAngewandte Chemie, 2016
- Selective Dinitrogen Conversion to Ammonia Using Water and Visible Light through Plasmon‐induced Charge SeparationAngewandte Chemie, 2016
- Review of electrochemical ammonia production technologies and materialsInternational Journal of Hydrogen Energy, 2013