Low temperature synthesis of new highly graphitized N-doped carbon for Pt fuel cell supports, satisfying DOE 2025 durability standards for both catalyst and support

Ha Young Lee, Ted H. Yu, Cheol Hwan Shin, Alessandro Fortunelli, Sang Gu Ji, Yujin Kim, Tong Hyun Kang, Byong June Lee, Boris V. Merinov, William A. Goddard, Chang Hyuck Choi, Jong Sung Yu

Research output: Contribution to journalArticlepeer-review

33 Scopus citations

Abstract

For polymer electrolyte membrane fuel cells (PEMFCs), the state-of-the-art electrocatalysts are based on carbon-supported Pt group metals. However, current carbon supports suffer from carbon corrosion during repeated start-stop operations, causing performance degradation. We report a new strategy to produce highly graphitized carbon with controllable N-doping that uses low-temperature synthesis (650 ℃) from g-C3N4 carbon-nitrogen precursor with pyrolysis using Mg. The high graphiticity is confirmed by high-intensity 2D Raman peak with low ID/IG (0.57), pronounced graphitic XRD planes, and excellent conductivity. Without further post-treatment, this highly graphitized N-doped carbon (HGNC) material combines high pyrrolic-N content with high porosity. Supporting Pt on HGNC exhibits excellent oxygen reduction activity for PEMFC with greatly improved durability as proved by real-time loss measurements of Pt and carbon, the first to surpass the DOE 2025 durability targets for both catalyst and support. The Pt/HGNC-65 shows 32% and 24% drop in mass activity after accelerated durability tests of both electrocatalyst and support, respectively, which are less than DOE target of 40% loss. The atomistic basis for this durability is explained via quantum mechanics-based molecular dynamics simulations. Interestingly, it is found that pyrrolic-N strongly interacts with Pt, making the Pt catalyst more stable during fuel cell reaction.

Original languageEnglish
Article number122179
JournalApplied Catalysis B: Environmental
Volume323
DOIs
StatePublished - Apr 2023

Bibliographical note

Publisher Copyright:
© 2022 Elsevier B.V.

Keywords

  • Grand canonical reaction kinetics
  • Graphitized carbon
  • PEMFCs
  • Pyrrolic-N
  • Real-time degradation analysis

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