4.8 Article

Manipulating dehydrogenation kinetics through dual-doping Co3N electrode enables highly efficient hydrazine oxidation assisting self-powered H2 production

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NATURE COMMUNICATIONS
卷 11, 期 1, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-020-15563-8

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资金

  1. National Natural Science Foundation of China [21601174]
  2. Recruitment Program of Global Experts
  3. Fundamental Research Funds for the Central Universities [WK2060190081]
  4. Natural Science Foundation from science and technology department of Guizhou Province [QHPT[2017]5790-02]

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Replacing sluggish oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) to produce hydrogen has been considered as a more energy-efficient strategy than water splitting. However, the relatively high cell voltage in two-electrode system and the required external electric power hinder its scalable applications, especially in mobile devices. Herein, we report a bifunctional P, W co-doped Co3N nanowire array electrode with remarkable catalytic activity towards both HzOR (-55 mV at 10 mA cm(-2)) and hydrogen evolution reaction (HER, -41 mV at 10 mA cm(-2)). Inspiringly, a record low cell voltage of 28 mV is required to achieve 10 mA cm(-2) in two-electrode system. DFT calculations decipher that the doping optimized H* adsorption/desorption and dehydrogenation kinetics could be the underlying mechanism. Importantly, a self-powered H-2 production system by integrating a direct hydrazine fuel cell with a hydrazine splitting electrolyzer can achieve a decent rate of 1.25 mmol h(-1) at room temperature.

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