FeNC shell-stabilized L10-PtFe intermetallic nanoparticles for high-performance oxygen reduction

doi:10.1016/S1872-2067(25)64661-4

Abstract

Abstract:

In the pursuit of high-performance proton exchange membrane fuel cells (PEMFCs), obtaining durable Pt-based intermetallic catalysts with small particle sizes for oxygen reduction reaction (ORR) stands as a crucial yet challenging topic. Herein, we propose an idea of catalyst design utilizing Fe-phenanthroline (Phen) complex as precursor to integrate metal-nitrogen-carbon (M-N-C) with the strong anchoring effect into carbon shells, synthesizing highly ordered and small-sized (3.59 nm) PtFe intermetallic catalyst coated with iron-nitrogen-carbon (FeNC) shells (L1₀-PtFe@FeNC). The strong Fe-Phen interaction ensures the uniform dispersion of Fe species on Pt seeds so as to form protective shells suppressing the agglomeration and dissolution of PtFe nanoparticles (NPs) under the high-temperature annealing or harsh operational conditions. It exhibits excellent mass activity (MA) that is about five-fold increase compared to the commercial Pt/C, as well as the significantly improved MA retention after 30,000 potential cycles (68.2% vs. 45.3%). Nitrogen-doped carbon (NC) shells and pure carbon (C) shells are used as comparison to demonstrate the advantages of FeNC shells. Durability test results show that NC and C shells obviously degrade after potential cycles, while well-preserved FeNC shells guarantee catalyst stability. Theoretical calculations reveal that the strong binding between FeNC shells and the Pt surface enhances the stability of both the nanoparticles and the FeNC shells.

Key words: Oxygen reduction reaction, Intermetallic PtFe, Surface coating, Iron-nitrogen-carbon, Durability

Yu Chengwen, Liang Lecheng, Mu Zhangyan, Yin Shaoqi, Liu Yuwen, Chen Shengli. FeNC shell-stabilized L1₀-PtFe intermetallic nanoparticles for high-performance oxygen reduction[J]. Chinese Journal of Catalysis, 2025, 75: 125-136.

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https://www.cjcatal.com/EN/Y2025/V75/I8/125

Figures/Tables 6

Scheme 1. Synthesis illustration of the three types of carbon-coated PtFe IMC catalysts.

Fig. 1. Characterizations of structure for L10-PtFe@FeNC catalyst. (a) XRD patterns of PtFe intermetallic catalysts. (b) HR-TEM image of L10-PtFe@FeNC. HAADF-STEM image (c) and their corresponding elemental mappings (d-f) of L10-PtFe@FeNC NPs. (g,h) HADDF-STEM images with the corresponding size distribution (inset). (i) The line intensity profile from (h). (j,k) EDS line-scannig result of the L10-PtFe@FeNC nanoparticle.

Fig. 2. Comparison of elemental distributions for different carbon-coated PtFe catalysts. EDS elemental mappings of Pt and Fe in L10-PtFe@FeNC (a-c), L10-PtFe@NC (d-f), and L10-PtFe@C (g-i) nanoparticles.

Fig. 3. Characterization of electronic structures for L10-PtFe@FeNC catalyst. XPS surveys (a) and Pt 4f spectra (b) of different carbon-coated catalysts. (c) N 1s spectra of L10-PtFe@FeNC and L10-PtFe@NC. (d) Fe 2p spectra of L10-PtFe@FeNC and L10-PtFe/C. XANES (e) and FT-EXAFS (f) data of L10-PtFe@FeNC, L10-PtFe@NC, L10-PtFe/C, Fe foil and FePc: Fe K-edge. WT for the EXAFS signals of L10-PtFe@FeNC (g), FePc (h), L10-PtFe@NC (i), and L10-PtFe/C (j).

Fig. 4. Electrochemical investigation of ORR activity in 0.1 mol L-1 HClO4. (a) CV curves of electrocatalysts in Ar-saturated electrolyte. (b) LSV curves recorded in O2-saturated electrolyte and at a rate of 5 mV s-1. (c) Comparison of MA at 0.9 V (vs. RHE) and ECSA of different catalysts. LSV curves of commercial Pt/C (d), uncoated PtFe IMC (e) and L10-PtFe@FeNC (f) before and after 30k ADT cycles. (g) MA attenuation of catalysts after potential cycles. (h) LSV curves of different carbon-coated PtFe IMCs before and after 30k cycles.

Fig. 5. The origin of enhanced stability of L10-PtFe@FeNC. HR-TEM images of L10-PtFe@FeNC (a), L10-PtFe@NC (c) and L10-PtFe@C (e) before 30k cycles. HR-TEM images of L10-PtFe@FeNC (b), L10-PtFe@NC (d) and L10-PtFe@C (f) after 30k cycles. (g) Calculations of binding energies of different carbon-coated catalysts. The top view (h) and the side view (i) of the L10-PtFe@FeNC atomic model for DFT calculations (blue, green, red and gray spheres represent Pt, Fe, N and C atoms, respectively).

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FeNC shell-stabilized L1₀-PtFe intermetallic nanoparticles for high-performance oxygen reduction

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