Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 47, Pages 16820-16825Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201909832
Keywords
electrocatalysis; kinetics; nickel; oxidation states; urea oxidation reaction
Categories
Funding
- MOST [2016YFA0203302]
- NSFC [21875042, 21634003, 51573027, 51673043, 21604012, 21805044]
- STCSM [16JC1400702, 18QA1400800, 17QA1400400, 18QA1400700]
- SHMEC [2017-01-07-00-07-E00062]
- Yanchang Petroleum Group
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
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The electrocatalytic urea oxidation reaction (UOR) provides more economic electrons than water oxidation for various renewable energy-related systems owing to its lower thermodynamic barriers. However, it is limited by sluggish reaction kinetics, especially by CO2 desorption steps, masking its energetic advantage compared with water oxidation. Now, a lattice-oxygen-involved UOR mechanism on Ni4+ active sites is reported that has significantly faster reaction kinetics than the conventional UOR mechanisms. Combined DFT, O-18 isotope-labeling mass spectrometry, and in situ IR spectroscopy show that lattice oxygen is directly involved in transforming *CO to CO2 and accelerating the UOR rate. The resultant Ni4+ catalyst on a glassy carbon electrode exhibits a high current density (264 mA cm(-2) at 1.6 V versus RHE), outperforming the state-of-the-art catalysts, and the turnover frequency of Ni4+ active sites towards UOR is 5 times higher than that of Ni3+ active sites.
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