4.8 Article

Highly Loaded Independent Pt0 Atoms on Graphdiyne for pH-General Methanol Oxidation Reaction

Journal

ADVANCED SCIENCE
Volume 9, Issue 16, Pages -

Publisher

WILEY
DOI: 10.1002/advs.202104991

Keywords

atomic catalysis; fuel cells; methanol oxidation reactions; two dimensional graphdiyne

Funding

  1. National Nature Science Foundation of China [21790050, 21790051, 22021002]
  2. National Key Research and Development Project of China [XDPB13]
  3. Key Program of the Chinese Academy of Sciences [QYZDY-SSW-SLH015]
  4. National Postdoctoral Program for Innovative Talents [BX20190332]
  5. National Science Foundation for Young Scientists of China [22005311]
  6. China Postdoctoral Science Foundation [2020M670465]

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The Pt/NGDY catalyst prepared using N-doped graphdiyne (NGDY) shows excellent activity, high pH adaptability, and high CO tolerance for methanol oxidation reaction (MOR), making it a promising alternative to noble metal catalysts.
The emergence of platinum-based catalysts promotes efficient methanol oxidation reactions (MOR). However, the defects of such noble metal catalysts are high cost, easy poisoning, and limited commercial applications. The efficient utilization of a low-cost, anti-poisoning catalyst has been expected. Here, it is skillfully used N-doped graphdiyne (NGDY) to prepare a zero-valent platinum atomic catalyst (Pt/NGDY), which shows excellent activity, high pH adaptability, and high CO tolerance for MOR. The Pt/NGDY electrocatalysts for MOR with specific activity 154.2 mA cm(-2) (1449.3 mA mg(Pt)(-1)), 29 mA cm(-2) (296 mA mg(Pt)(-1)) and 22 mA cm(-2) (110 mA mg(Pt)(-1)) in alkaline, acid, and neutral solutions. The specific activity of Pt/NGDY is 9 times larger than Pt/C in alkaline solution. Density functional theory (DFT) calculations confirm that the incorporation of electronegativity nitrogen atoms can increase the high coverage of Pt to achieve a unique atomic state, in which the shared contributions of different Pt sites reach the balance between the electroactivity and the stability to guarantee the higher performance of MOR and durability with superior anti-poisoning effect.

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