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Elucidating the electro-catalytic oxidation of hydrazine over carbon nanotube-based transition metal single atom catalysts |
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| Authors: | Zhang Jin Wang Yaxin Yang Chujie Chen Sian Li Zhengjian Cheng Yi Wang Haining Xiang Yan Lu Shanfu Wang Shuangyin |
| Affiliation: | 1.Beijing Key Laboratory of Bio-inspired Energy Materials and Devices & School of Space and Environment, Beihang University, Beijing, 100191, China ;2.Department of Environmental Engineering, School of Metallurgy and Environment, Central South University, Changsha, 410083, China ;3.State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China ; |
| 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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