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Elucidating the electro-catalytic oxidation of hydrazine over carbon nanotube-based transition metal single atom catalysts

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Abstract

Elucidating the reaction mechanism of hydrazine oxidation reaction (HzOR) over carbon-based catalysts is highly propitious for the rational design of novel electrocatalysts for HzOR. In present work, isolated first-row transition metal atoms have been coordinated with N atoms on the graphite layers of carbon nanotubes via a M-N4-C configuration (MSA/CNT, M=Fe, Co and Ni). The HzOR over the three single atom catalysts follows a predominant 4-electron reaction pathway to emit N2 and a negligible 1-electron pathway to emit trace of NH3, while their electrocatalytic activity for HzOR is dominated by the absorption energy of N2H4 on them. Furthermore, FeSA/CNT reverses the passivation effect on Fe/C and shows superior performance than CoSA/CNT and NiSA/CNT with a recorded high mass activity for HzOR due to the higher electronic charge of Fe over Co and Ni in the M-N4-C configuration and the lowest absorption energy of N2H4 on FeSA/CNT among the three MSA/CNT catalysts.

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Acknowledgements

Project supported by Beijing Natural Science Foundation (No. 2194076), the National Natural Science Foundation of China (Nos. 21908001, 21872003, and U19A2017), and the Fundamental Research Funds for the Central Universities. XAS measurements were performed on the soft X-ray and XAS beamlines of the Australian Synchrotron, Victoria, Australia. The electron microscopy carried out at ORNL was supported by the U.S. Department of Energy, Office of Basic Energy Sciences and through a user proposal supported by ORNL’s Center for Nanophase Materials Sciences. This research was also supported by the high performance computing (HPC) resources at Beihang University.

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  1. Beijing Key Laboratory of Bio-inspired Energy Materials and Devices & School of Space and Environment, Beihang University, Beijing, 100191, China

    Jin Zhang, Yaxin Wang, Sian Chen, Zhengjian Li, Haining Wang, Yan Xiang & Shanfu Lu

  2. Department of Environmental Engineering, School of Metallurgy and Environment, Central South University, Changsha, 410083, China

    Chujie Yang & Yi Cheng

  3. State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China

    Shuangyin Wang

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  1. Jin Zhang
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Elucidating the electro-catalytic oxidation of hydrazine over carbon nanotube-based transition metal single atom catalysts

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Zhang, J., Wang, Y., Yang, C. et al. Elucidating the electro-catalytic oxidation of hydrazine over carbon nanotube-based transition metal single atom catalysts. Nano Res. 14, 4650–4657 (2021). https://doi.org/10.1007/s12274-021-3397-9

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