Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction

doi:10.1016/S1872-2067(21)63991-8

Abstract

Abstract:

Proton exchange membrane fuel cells (PEMFCs) are considered ideal energy-conversion devices because of their environmentally friendly nature and high theoretical energy efficiency. However, cathodic polarization, which is a result of the sluggish oxygen reduction reaction (ORR) kinetics, is a significant source of energy loss and reduces fuel cell efficiency. Further, the need to use Pt in commercial Pt/C cathodes has restricted their large-scale application in fuel cells because of its high cost and poor durability. Thus, improvements in the activity and durability of Pt-based catalyst are required to reduce the amount of Pt required and, thus, costs, while increasing the ORR rate and fuel cell power density and promoting widespread PEMFC commercialization. In recent years, atomically ordered Pt-based intermetallic nanocrystals have received tremendous attention owing to their excellent activity and stability for the ORR. Therefore, in this review, we first introduce the formation of intermetallic compounds from the perspective of thermodynamics and kinetics to lay a theoretical foundation for the design of these compounds. In addition, optimization strategies for Pt-based ordered intermetallic catalysts are summarized in terms of the catalyst composition, size, and morphology. Finally, we conclude with a discussion of the current challenges and future prospects of Pt-based ordered alloys. This review is designed to help readers gain insights into the recent developments in and rational design of Pt-based intermetallic nanocrystals for the ORR and encourage research that will enable the commercialization of PEMFCs.

Key words: Oxygen reduction reaction, Fuel cell, Pt-based catalyst, Intermetallic, Electrocatalysis

Jingsen Bai, Liting Yang, Zhao Jin, Junjie Ge, Wei Xing. Advanced Pt-based intermetallic nanocrystals for the oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2022, 43(6): 1444-1458.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63991-8

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Figures/Tables 7

Fig. 1. (a) Oxygen reduction reaction pathway. (b) Free energy diagram for the four-electron associative ORR on Pt(111). (c) Relationship between the binding free energy of *OOH (ΔGOOH) and that of *O (ΔGO) with respect to ∆GOH on the (111) surfaces of various metals. (d) Curve limiting potential with respect to free energy drawn according to Eqs. 10-13; here, one side of the solid blue line represents strong adsorption, whereas the other side of the solid green line represents weak adsorption. Reprinted from Ref. [21] with permission. Copyright 2018, American Chemical Society.

Fig. 2. Schematic of conditions for the formation of an AmBn intermetallic phase in an A-B binary system at thermodynamic equilibrium. (a) Phase diagram showing the equilibria between disordered solid solution (blue), ordered intermetallic compound (orange), and mixed phases (white) as a function of composition and temperature. At T1 (T1 should be higher than the order-to-disorder transition temperature), a disordered atomic arrangement is preferred over the full range of possible compositions. At T2, an ordered phase appears within a specific range of compositions near the stoichiometric point (marked by a red bar). (b) Diagram showing the Gibbs free energies of the disordered (blue) and ordered (orange) phases as a function of composition at two temperatures: T1 (dashed) and T2 (solid). Reprinted from Ref. [26] with permission. Copyright 2017, John Wiley and Sons.

Fig. 3. (a) Schematic of the core-shell structure formed by acid washing the catalyst. (b) Mass activity of L10-FePt/Pt and commercial Pt/C at the beginning of life (BOL) and after ADT (60 °C). (c) Half-wave potential of L10-FePt/Pt and commercial Pt/C at BOL and after ADT (60 °C). (a-c) Reprinted from Ref. [13] with permission. Copyright 2018, American Chemical Society. (d) High-angle annular dark-field scanning tunneling electron microscopy (HAADF-STEM) image of fully ordered fct-Pt-Fe and hysteresis loops of partially ordered fct-FePt and fully ordered fct-FePt; ORR polarization of fully ordered fct NPs (e), partially ordered fct-Fe NPs (f), and C-fcc-FePt NPs (g) before and after ADT. (d-f) Reprinted from Ref. [33] with permission. Copyright 2015, American Chemical Society. (h,i) Schematic of the synthesis and HAADF-STEM image of L10-FePt/rGO. Reprinted from Ref. [53] with permission. Copyright 2020, American Chemical Society.

Fig. 4. (a) Schematic of L10-CoPt/Pt NPs with a Pt shell (blue, Co; white, Pt). (b,c) Enlarged STEM image of L10-CoPt/Pt NPs with Pt shell (blue, Co; red, Pt). (d) SA and MA of commercial Pt/C, etched A1-CoPt, and L10-CoPt/Pt measured at 0.9 V vs. RHE. (e) ORR polarization curves of L10-CoPt/Pt NPs from BOL to end of life (EOL). (f) MA of L10-CoPt/Pt NPs measured at BOL and EOL in a fuel cell. (a-f) Reprinted from Ref. [55] with permission. Copyright ORR polarization curves of Pt3Co with different Co contents in the Co-metal-organic framework (g) and Pt/40Co-nanocrystals sintered at different temperatures in O2-saturated 0.1 mol/L HClO4 at room temperature at a rotation speed of 900 rpm (h). (i) Potential cycling stability tests of Pt/40Co-NC-900 at 0.6-1.0 V at a scan rate of 50 mV/s. (j) STEM-electron energy loss spectroscopy images of Pt3Co nanoparticle. (g-j) Reprinted from Ref. [56] with permission. Copyright 2019, Elsevier.

Fig. 5. HAADF-STEM images of cubic (a), concave (b), and defect-rich cubic (c) intermetallic Pt3Sn. (a-c) Reprinted from Ref. [67] with permission. Copyright 2016, John Wiley and Sons. (d) Schematic illustration of the structural change of the FePtAu NPs upon annealing. Reprinted from Ref. [72] with permission. Copyright 2012 American Chemical Society. (e) Schematic of L10-Pt-Ni-Co synthesis (acac = acetylacetonate). (f) Linear sweep voltammetry curves of commercial Pt/C, C-A1-PtNi0.8Co0.2, and C-L10-PtNi0.8Co0.2. (g) Mass activities of commercial Pt/C, C-A1-PtNi0.8Co0.2, and C-L10-PtNi0.8Co0.2 at 0.9 V. (e-g) Reprinted from Ref. [76] with permission. Copyright 2019, John Wiley and Sons. (h) Image of L10-W-PtCo. (i) Mass activities of L10-W-PtCo/C and P/C before and after ADT. (j) Pt-Pt bond lengths and oxygen adsorption energies of the studied catalysts. (h-j) Reprinted from Ref. [77] with permission. Copyright 2019 John Wiley and Sons.

Fig. 6. (a) Formation of ordered fct Pt-Fe NPs and N-doped carbon shells. Reprinted from Ref. [35] with permission. Copyright 2015, American Chemical Society. (b) HAADF images of sub-Pt3Co-MC. (c) HAADF-STEM of Pt3Co NPs. (d) Model of ordered Pt3Co NPs. (b-d) Reprinted from Ref. [80] with permission. Copyright 2021, PNAS. (e) HAADF-STEM image of L10-PtZn NP. (f) ORR polarization curves of L10-PtZn/Pt-C. (g) H2-O2 fuel cell polarization curves of L10-PtZn. (e-g) Reprinted from Ref. [84] with permission. Copyright 2020, John Wiley and Sons.

Fig. 7. (a) STEM-ADF image of Pt3Co NWs/C. (b) HAADF-STEM image of Pt3Co NWs/C. (c) ORR-specific activities and mass activities of Pt/C and PtxCoy. (a-c) Reprinted from Ref. [56] with permission. Copyright 2015 American Chemical Society. (d) Synthesis of D-Pt3Co NWs and O-Pt3Co NWs. (e) Transmission electron microscopy (TEM) and high-resolution (HR)TEM images of O-Pt3Co NWs. (f) ORR polarization curves and MAs of different catalysts. (d-f) Reprinted from Ref. [86] with permission. Copyright 2019, American Chemical Society. (g) Schematic of PtPb nanoplate; (h) SAs and MAs of different catalysts [66]. (i) Schematic of Meso-PtNi. (j) ORR polarization curves before and after the ADT of Pt/C, Meso-PtNi_1, and Meso-PtNi_2. (g-j) Reprinted from Ref. [87] with permission. Copyright 2016 John Wiley and Sons.

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