Dandan Guo, Fengyu Liu, Tianqi Liu*, Zhaoqi Ji, Xiaolei Fan, Bin Sun, Peili Zhang, Fei Li and Fusheng Li*,
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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.
期刊介绍：
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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