Journal article
Electrochemistry-Assisted Photoelectrochemical Reduction of Nitrogen to Ammonia
Journal of Physical Chemistry. C, Vol.125(42), pp.23041-23049
2021
Abstract
Ammonia (NH3) is a basic chemical feedstock for the production of fertilizers and pharmaceuticals, and it emerges as a new hydrogen energy carrier for renewable energy sources such as solar and wind power. A photoelectrochemical nitrogen reduction reaction (PEC NRR) under mild operating conditions represents a potentially green and convenient approach for the synthesis of NH3. However, a generally applicable PEC NRR featuring a high NH3 yield and a satisfactory conversion efficiency remains elusive. Herein, we report on a simple and effective electrochemistry-assisted strategy to enhance the PEC fixation of N2 to NH3. Using this strategy, we harness a steel-based cathode-assisted Au/SiO2/Si photocathode to seamlessly combine two critical reaction stepsN2 activation and hydrogenationto realize an NH3 yield rate of 22.0 μg·cm–2·h–1 and a faradic efficiency of 23.7% at −0.2 V versus a reversible hydrogen electrode under one sun illumination. We also provide an accessible reaction setup to avoid the disturbance of a contamination by air, human breath, and N2 stream, leading to a reliable production of NH3 by the PEC NRR. An operando characterization and a theoretical calculation uncover the active sites and reaction mechanism of the whole system for an electrochemistry-assisted PEC NRR. This work demonstrates the capability of an electrochemistry-assisted excitation in PEC NRR, and it introduces a new design concept for addressing pertinent challenges in photoelectrochemical and other chemical fields.
Details
- Title
- Electrochemistry-Assisted Photoelectrochemical Reduction of Nitrogen to Ammonia
- Authors
- Jianyun Zheng (Author) - Hunan UniversityYanhong Lyu (Author) - Hunan First Normal UniversityJean-Pierre Veder (Author) - Curtin UniversityBernt Johannessen (Author) - Australian SynchrotronRuilun Wang (Author) - State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical EngineeringRoland De Marco (Author) - University of the Sunshine Coast, Queensland, Office of the Deputy Vice-Chancellor (Research and Innovation)Aibin Huang (Author) - Chinese Academy of SciencesSan Ping Jiang (Author) - Curtin UniversityShuangyin Wang (Author) - State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering
- Publication details
- Journal of Physical Chemistry. C, Vol.125(42), pp.23041-23049
- Publisher
- American Chemical Society
- DOI
- 10.1021/acs.jpcc.1c07278
- ISSN
- 1932-7455
- Organisation Unit
- University of the Sunshine Coast, Queensland; Office of the Deputy Vice-Chancellor (Research and Innovation)
- Language
- English
- Record Identifier
- 99583107502621
- Output Type
- Journal article
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- Domestic collaboration
- International collaboration
- Web Of Science research areas
- Chemistry, Physical
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology
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