4.7 Article

Branched Poly(L-lysine)-Derived Nitrogen-Containing Porous Carbon Flake as the Metal-Free Electrocatalyst toward Efficient Oxygen Reduction Reaction

Journal

ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 4, Pages 3317-3326

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.0c03070

Keywords

branched poly(L-lysine); carbonization; electrocatalyst; nitrogen-containing porous carbon flake; oxygen reduction reaction

Funding

  1. Huazhong University of Science and Technology [3004013134]
  2. National Natural Science Foundation of China [51903099]
  3. 100 Talents Program of the Hubei Provincial Government
  4. National Science Centre Poland [OPUS UMO-2018/29/B/ST8/01265]

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By utilizing renewable biomass branched poly(L-lysine), nitrogen-doped porous carbon materials were successfully synthesized through a metal-free process, achieving high carbon yield and nitrogen doping content. These carbon materials exhibited excellent performance in the oxygen reduction reaction, showing superior stability and endurance compared to Pt/C in basic conditions.
Amino acids are recently being regarded as highly attractive candidates to fabricate thoroughly metal-free and rich nitrogen-containing mesoporous carbons. Nevertheless, the carbonization yield of the lysine is usually just around 5% due to the small molecular size and harsh polymerization condition for lysine to form the stable carbonization counterpart. Renewable biomass branched poly(L-lysine) (BPL) is hereby exploited to synthesize nitrogen-containing porous carbon flake (NPCF). Notably, the fabrication process is essentially an in situ thermal polymerization and pyrolysis with mesoporous silica template strategy, which avoids the usage of metal catalysts. Indeed, a metal-free mesoporous carbon with a high carbon yield of 20.1% and improved nitrogen-doping content of up to 9.6 at. % is achieved. As a result, the as-prepared NPCFs serve as metal-free electrocatalysts toward the efficient oxygen reduction reaction (ORR). In particular, one of the samples (NPCF-700/900) exhibits highly efficient ORR performance of oxygen-reduction voltage at 0.809 V in cyclic voltammogram measurement, onset peak at 0.93 V, and semi wave peak of 0.83 V in rotating disk electrode linear sweep voltammetry curves. The associated kinetic-limiting and diffusion-limiting current densities are 18.4 and -4.89 mA cm(-1), respectively. This can be attributed to the abundance of nitrogen dopant of 8.3 at. % in a high graphitization carbon framework that possesses a large specific surface area (1431 m(2) g(-1)). More importantly, NPCF-700/900 delivers excellent cycle stability and endurance with regards to methanol permeation and CO poisoning, making it a hopeful metal-free ORR electrocatalyst superior to that of the Pt/C in basic conditions.

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