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. 2019 Nov 18;58(47):16820-16825.
doi: 10.1002/anie.201909832. Epub 2019 Oct 11.

A Lattice-Oxygen-Involved Reaction Pathway to Boost Urea Oxidation

Longsheng Zhang  1 , Liping Wang  1 , Haiping Lin  2 , Yunxia Liu  2 , Jinyu Ye  3 , Yunzhou Wen  1 , Ao Chen  1 , Lie Wang  1 , Fenglou Ni  1 , Zhiyou Zhou  3 , Shigang Sun  3 , Youyong Li  2 , Bo Zhang  1 , Huisheng Peng  1
Affiliations

A Lattice-Oxygen-Involved Reaction Pathway to Boost Urea Oxidation

Longsheng Zhang et al. Angew Chem Int Ed Engl. .

Abstract

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, 18 O 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.

Keywords: electrocatalysis; kinetics; nickel; oxidation states; urea oxidation reaction.

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References

    1. J. Zhang, T. He, M. Wang, R. Qi, Y. Yan, Z. Dong, H. Liu, H. Wang, B. Xia, Nano Energy 2019, 60, 894.
    1. N. Senthilkumar, G. Kumar, A. Manthiram, Adv. Energy Mater. 2018, 8, 1702207.
    1. S. Yao, S. Wolfson, B. Ahn, C. Liu, Nature 1973, 241, 471.
    1. M. Wester, F. Simonis, N. Lachkar, W. Wodzig, F. Meuwissen, J. Kooman, W. Boer, J. Joles, K. Gerritsen, Artif. Organs 2014, 38, 998.
    1. B. Boggs, R. King, G. Botte, Chem. Commun. 2009, 4859.

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