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.

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

Fortunelli A;
2023

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.
2023
Istituto di Chimica dei Composti OrganoMetallici - ICCOM -
Grand canonical reaction kinetics; Graphitized carbon; PEMFCs; Pyrrolic-N; Real-time degradation analysis
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/414973
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