Single-Site Electrocatalyst with Pentadentate Carboxamide Ligand for Ammonia Oxidation to Dinitrogen and Hydrazine
Efficient ammonia oxidation electrocatalysis is crucial for converting the chemical energy in ammonia molecules into electricity and for valorizing ammonia into value-added chemicals. This work introduces the single-site catalyst Ru-pdcPy2 with a pentadentate carboxamide ligand for ammonia oxidation, which is capable of oxidizing ammonia directly to hydrazine, possibly via a single-site N–N bond formation mechanism. The combination of nuclear magnetic resonance spectroscopy, mass spectrometry, and electrochemical technique was utilized to investigate the catalytic behavior of the catalyst. Under optimal conditions, the Ru-pdcPy2 achieves a TOF of 32.6 h–1 for N2 generation and a TOF of 8.4 h–1 for N2H4 synthesis during bulk electrolysis.
Authors
- Xiaolei Fan (ORCID: https://orcid.org/0000-0002-9039-6736)
- Zhaoqi Ji (ORCID: https://orcid.org/0000-0001-9999-3839)
- Dandan Guo
- Peili Zhang (ORCID: https://orcid.org/0000-0001-9171-935X)
- Fei Li (ORCID: https://orcid.org/0000-0002-3686-7576)
- Tianqi Liu (ORCID: https://orcid.org/0000-0002-0672-9965)
- Fengyu Liu (ORCID: https://orcid.org/0000-0002-1839-2343)
- Fusheng Li (ORCID: https://orcid.org/0000-0003-3455-0855)
- Bin Sun (ORCID: https://orcid.org/0000-0002-5311-789X)
Institutions
- Harbin Institute of Technology (CN)
- Dalian University of Technology (CN)
- University of Manchester (GB)
- State Key Laboratory of Fine Chemicals
- Zhejiang University (CN)
Publication Details
- Journal
- ACS Catalysis
- Published
- 2025-05-01
- DOI
- https://doi.org/10.1021/acscatal.5c02322
- Citations
- 5
- Primary Topic
- Ammonia Synthesis and Nitrogen Reduction
- Type
- article
- Field-Weighted Citation Impact
- 1.94
Funders
- National Natural Science Foundation of China
- Wenzhou Municipal Science and Technology Bureau
- National Key Research and Development Program of China