Focus on the catalysts to resist the phosphate poisoning in high-temperature proton exchange membrane fuel cells

doi:10.1016/S1872-2067(24)60162-2

Chinese Journal of Catalysis ›› 2025, Vol. 68: 155-176.DOI: 10.1016/S1872-2067(24)60162-2

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Focus on the catalysts to resist the phosphate poisoning in high-temperature proton exchange membrane fuel cells

Liyuan Gong^a^,^b^,^c, Li Tao^c^,^d^,^*(), Lei Wang^a, Xian-Zhu Fu^a^,^*(), Shuangyin Wang^c^,^d^,^*()

^aCollege of Materials Science and Engineering, Shenzhen University, Shenzhen 518055, Guangdong, China
^bCollege of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, Guangdong, China
^cState Key Laboratory of Chemo/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, the National Supercomputer Centers in Changsha, Advanced Catalytic Engineering Research Center of the Ministry of Education, Hunan University, Changsha 410082, Hunan, China
^dGreater Bay Area Institute for Innovation, Hunan University, Guangzhou 511300, Guangdong, China

Received:2024-08-16 Accepted:2024-10-08 Online:2025-01-18 Published:2025-01-02
Contact: * E-mail: taoli@hnu.edu.cn (L. Tao), xz.fu@szu.edu.cn (X. Fu), shuangyinwang@hnu.edu.cn (S. Wang).
About author:Li Tao received his Master degree in 2016 and his Ph.D. degree in 2019 from Hunan University under the supervision of Prof. Shuangyin Wang. He is currently an associate professor of the College of Chemistry and Chemical Engineering, Hunan University. His research interests are in thermoelectric coupling catalysis, defect chemistry and fuel cell.
Xian-Zhu Fu is currently a professor in the college of Materials Science and Engineering, Shenzhen University. He received his Ph.D. degree in Chemistry from Xiamen University in 2007. Then he joined the Department of Materials and Chemical Engineering at University of Alberta in Canada as a post-doctoral research flow and Lawrence Berkeley National Lab as a visiting scholar. From 2012-2017, he worked at the Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences. His research interests focus on electrochemistry/electrocatalysts for energy materials and devices, electronic materials and process.
Shuangyin Wang received his bachelor’s degree in 2006 from Zhejiang University and his Ph.D. in 2010 from Nanyang Technological University, Singapore. He is currently a Professor of the Key Laboratory for Graphene Materials and Devices and College of Chemistry and Chemical Engineering, Hunan University. His research interests are defect chemistry of electrocatalysts, HT-PEMFCs, and electrosynthesis.
Supported by:
National Key R&D Program of China(2021YFA1500900);National Natural Science Foundation of China(22425021);National Natural Science Foundation of China(22102053);Provincial Natural Science Foundation of Hunan(2024JJ2012);Science and Technology Innovation Program of Hunan Province(2022RC1036);Guangdong Basic and Applied Basic Research Foundation(2024A1515012889);Shenzhen Science and technology program(JCYJ20210324122209025);Major Program of the Natural Science Foundation of Hunan Province(2021JC0006)

Abstract

Abstract:

Investigating highly effective electrocatalysts for high-temperature proton exchange membrane fuel cells (HT-PEMFC) requires the resistance to phosphate acid (PA) poisoning at cathodic oxygen reduction reaction (ORR). Recent advancements in catalysts have focused on alleviating phosphoric anion adsorption on Pt-based catalysts with modified electronic structure or catalytic interface and developing Fe-N-C based catalysts with immunity of PA poisoning. Fe-N-C-based catalysts have emerged as promising alternatives to Pt-based catalysts, offering significant potential to overcome the characteristic adsorption of phosphate anion on Pt. An overview of these developments provides insights into catalytic mechanisms and facilitates the design of more efficient catalysts. This review begins with an exploration of basic poisoning principles, followed by a critical summary of characterization techniques employed to identified the underlying mechanism of poisoning effect. Attention is then directed to endeavors aimed at enhancing the HT-PEMFC performance by well-designed catalysts. Finally, the opportunities and challenges in developing the anti-PA poisoning strategy and practical HT-PEMFC is discussed. Through these discussions, a comprehensive understanding of PA-poisoning bottlenecks and inspire future research directions is aim to provided.

Key words: Fuel cell, High-temperature, Phosphate acid poisoning, Activity degradation, Electrocatalyst design

Liyuan Gong, Li Tao, Lei Wang, Xian-Zhu Fu, Shuangyin Wang. Focus on the catalysts to resist the phosphate poisoning in high-temperature proton exchange membrane fuel cells[J]. Chinese Journal of Catalysis, 2025, 68: 155-176.

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Figures/Tables 19

Scheme 1. The table of contents of this review.

Fig. 1. (A) PO4 adsorbed through Pt-O in the different mode. Reprinted with permission from Ref. [54]. Copyright 2013, American Chemical Society. (B) Trends in ORR activity concerned about oxygen binding strength (ΔEO: O binding energy from DFT calculation) of various metal. Reprinted with permission from Ref. [53]. Copyright 2004, American Chemical Society. (C) Schematic illustration of d band theory of a transition metal surface. Reprinted with permission from Ref. [60]. Copyright 2005, Springer Nature.

Fig. 2. The adsorption competition of H, OH, and PO4? on the Pt surface (A) and (B) at different cell voltages, (C) temperature, (D) phosphoric acid concentration Reprinted with permission from Ref. [33]. Copyright 2013, American Chemical Society.

Fig. 3. (A) H3PO3 oxidation behavior observed in CV of the Pt electrode in single H3PO4. (B) Anodic/cathodic charge ratio. Reprinted with permission from Ref. [25] Copyright 2023, American Chemical Society. (C) Poisoning effect of both H3PO3 and H3PO4 at different potential observed from coordination numbers of Pt-Pt, Pt-O, Pt-P gained through EXAFS fitting. Reprinted with permission from Ref. [64]. Copyright 2022, American Chemical Society.

Fig. 4. (A) Phosphoric acid adsorption characteristics in the CV of Pt3Co/C. Reprinted with permission from Ref. [29]. Copyright 2011, Elsevier. (B) N2O reduction curves of Pt3Co/C [29] affected by PA. (C) Schematic of the in-situ XAS setup. Reprinted with permission from Ref. [68], Copyright 2015, IOP Publishing, Ltd. (D) Schematic presentation of the Δμ and δΔμ method. Reprinted with permission from Ref. [33]. Copyright 2013, American Chemical Society.

Fig. 5. (A) Schematic of EC-SERS setup. (B) SER spectra get in (C) CV scans at Au surface in different pH solutions. Reprinted with permission from Ref. [72]. Copyright 2015, Elsevier. (D) FTIR spectra taken from a platinum electrode at different potentials in 0.015 mol L-1 phosphate (79% H2PO4-, 21% H3PO4). (E) The H2PO4- in C2V and Cs symmetries at low and high potentials respectively. Reprinted with permission from Ref. [10] Copyright 1992, Elsevier.

Fig. 6. (A) Supercell structure and top view supercell of Ptskin-Pt3M. (B) Adsorption strength of Ptskin-Pt3M determined by DFT calculation. (C) DOS near the Fermi level. Reprinted with permission from Ref. [51], Copyright 2017, Springer Nature. (D) Schematic diagram of “Self-Healing” effect. [81] (E) The scaling relationship of the O2 and PO4 adsorption energy on Pt3M(111) alloy surface. Reprinted with permission from Ref. [19]. Copyright 2023, Elsevier. (F) The LSV of PtRhCu@Pt/C with and without phosphate anion. (G) Performance of HT-PEMFC at 160 °C. (H) Stability test at 200 mA cm?2. Reprinted with permission from Ref. [81]. Copyright 2024, American Chemical Society.

Fig. 7. (A) CV of PtSn(111) single crystals electrodes. LSV of Pt(111) (B) and PtSn(111) (C) single crystals electrodes with/without PA. Reprinted with permission from Ref. [30] Copyright 2010, Royal Society of Chemistry. (D) The charge density difference of the CuPtFe alloy catalysts. (E) H2PO4? adsorption energy of Cu-PtFe and PtFe catalysts. (F) The activity of catalysts with/without the presence of H3PO4. (G) HT-PEMFC performance. (H) H2-air fuel cell performance. (I) Durability test results at 200 mA cm?2. Reprinted with permission from Ref. [80].Copyright 2021, Wiley.

Fig. 8. (A) Schematic illustration of Cu alloying strategy. The d-band center (B), H3PO4 anion adsorption energy (C), image (D) of the HT-RDE. (E) Relationship of PA coverage, O-reduction area, and E1/2 of O-PtCu/S-C and reference catalysts by HT-RDE test in 0.5 mol L?1 H3PO4. (F). Fuel cell performance in H2-O2 at 160 °C. Reprinted with permission from Ref. [67]. Copyright 2024, Elsevier. (G) Current densities of pure Pt and PtAu alloy catalysts with/without PA. (H) CV of PtAu alloy catalysts with/without PA. Reprinted with permission from Ref. [72]. Copyright 2015, Elsevier. (I) Current densities of pure Pt, PtCo physical mixture catalysts and PtCo alloy catalysts with/without PA. Reprinted with permission from Ref. [76]. Copyright 2022, Elsevier.

Fig. 9. (A) The schematic presentation of the anti-poisoning effect of cyanide. (B) The LSV of Pt(111)/Pt(111)-CNad in the phosphoric acid and perchloric acid. Reprinted with permission from Ref. [82]. Copyright2010, Springer Nature. (C) Visual explanation of manipulating the d-band structure by adsorbed oleylamine. (D) Increased factors compared to Pt/C related to the difference of the εd. Reprinted with permission from Ref. [84]. Copyright 2013, American Chemical Society. (E) Schematic illustration of the coulombic barrier on Pt surface. Reprinted with permission from Ref. [86]. Copyright 2015, Elsevier. (F) The relationship of activity and the varying coverages of butylamine. Reprinted with permission from Ref. [83]. Copyright 2016, Elsevier.

Fig. 10. (A) Schematic diagram showing the molecular sieve layer effect of carbon shell structure. (B) The difference value in mass activity of different catalysts with/without carbon shells before and after ADTs in 0.1 mol L?1 HClO4 with and without 0.1 mol L?1 H3PO4. Reprinted with permission from Ref. [87]. Copyright 2023, Wiley. (C) LSV of O-Pt-Fe@NC/C and Pt/C with and without H3PO4. (D) Full fuel performance at 160 °C under H2/O2. Reprinted with permission from Ref. [78]. Copyright 2020, Elsevier. (E) LSV of PtCo@MoOx-NC with and without PA. (F) The mass activity, durability, and H3PO4 tolerance of PtCo@MoOx-NC comparing to PtC. Reprinted with permission from Ref. [88]. Copyright 2023, Royal Society of Chemistry.

Fig. 11. (A) Graphical representation of SiO2 promoting PA distribution. LSV (B) and CV (C) of CNT@SiO2-Pt with/without the H3PO4. HT-PEMFC performance (D) and stability (E) in a single cell. Reprinted with permission from Ref. [90]. Copyright 2021, Springer Nature. (F) mass and specific activity the prepared PtP2/C and Pt/C-TKK catalysts with/without H3PO4. (G) Activity and durability of HT-PEMFC under H2/O2 at 180 °C. Reprinted with permission from Ref. [52]. Copyright 2023, Royal Society of Chemistry.

Table 1 Summary of recent performance of HT-PEMFC using Pt-based catalysts. T, an./ca., v, P and PPD refer to temperature, anode/cathode, flow rate pressure and peak power density, respectively.

T (°C)	v at an./ca. (mL min⁻¹)	P (bar)	Membrane/thickness (mm)	Cat./Pt loading of ca. (mg cm⁻²)	PPD (mW cm⁻²)	Ref.
160	H₂-60/air-50	—	PA/PBI	Cu-PtFe/NC/0.5	432.6	[80]
160	H₂-60/O₂-50	—	PA/PBI	Cu-PtFe/NC/ 0.5	793.5	[80]
160	H₂/air	—	PA/PES-PVP^a	CNT@SiO₂-Pt/1.0	486	[90]
160	H₂/O₂	—	PA/PES-PVP^a	CNT@SiO₂-Pt/1.0	765	[90]
220	H₂/O₂	—	PA/PES-PVP^a	CNT@SiO₂-Pt/.0	1061	[90]
160	H₂-200/Air-600	—	PA/PBI	Pt₂Cu/C/1.5	383.4	[19]
180	H₂/O₂	1.5	PA/PBI	PtP₂/C/0.5	1180	[52]
160	H₂-100/O₂-100	—	PA/PBI/SiO₂	O-Pt-Fe@NC/C/1	384	[78]
160	H₂-100/O₂-100	—	PA/PBI	O-PtCu/S-C/0.5	800.5	[67]
160	H₂-100/O₂-200	—	PA/PBI	PtRhCu@Pt/C/1.5	529	[81]
160	H₂-100/Air-200	—	PA/PBI	PtRhCu@Pt/C/1.5	977	[81]

Fig. 12. (A) Schematic diagram of catalyst synthesis steps. TEM (B), aberration-corrected scanning TEM (C), and STEM-EDS mapping (D). (E) LSV for phosphate ions poisoning effect on Pt/C and Fe-NC, Fe-NCP. (F) HT-PEMFC performance under H2/O2. (G) Free energy diagram of ORR reaction. (H) Adsorption energy of phosphate ions on Pt(111), Fe-NC, Fe-NCP, and Fe-NPC. Reprinted with permission from Ref. [96].Copyright 2022, Springer Nature.

Fig. 13. TEM (A), STEM-EDS mapping (B), aberration-corrected scanning TEM (C,D) of FeCu/N-CNTs. (E) Scheme of the phosphate promoting effect. (F) LSV of ORR on FeCu catalysts with the presence of PA. (G) Potential energy on Fe, Cu, Fe-Cu diatomic sites with different distance with/without PA. (H) XPS of Cu 2p affected by PA. Fuel cell activity at 230 °C under H2/O2 (I) and stability test (J). Reprinted with permission from Ref. [98]. Copyright 2021, Elsevier.

Fig. 14. (A) LSV of FeSA-G and Pt/C in with/without the H3PO4. Fuel cell performance at 160 °C (B) and 230 °C (C) under H2/O2. (D) Stability of the cells at 0.5 V. Reprinted with permission from Ref. [101]. Copyright 2019, Wiley.

Fig. 15. (A) TEM images of pore structure. (B) LSV of Pt/C and Fe-N-C with/without PA. (C) Accelerated durability tests. (D) Single-cell performance at 150 °C under H2/O2. Reprinted with permission from Ref. [104]. Copyright 2020 American Chemical Society.

Table 2 Summary of recent performance of HT-PEMFC using Fe-based catalysts. T, an./ca., v, P and PPD refer to temperature, anode/ cathode, flow rate pressure and peak power density, respectively.

T (°C)	gas-v at an./ca. (mL min⁻¹)	P (bar)	Membrane	Cat./catalysts loading (mg cm⁻²)	PPD (mW cm⁻²)	Ref.
160	H₂/O₂	—	PA/PBI	BP-FeNC/7.8	184.6	[94]
150	H₂/O₂	1.5	PA/PBI	LEDFe5-NH₃/3.8	260	[104]
240	H₂-150/O₂-100	—	PA/SiO₂/PBI	FeSA/HP/4	266	[102]
160	H₂-100/O₂-100	—	SiO₂/PA/PBI	FeSA-G/0.3Fe	276	[101]
230	H₂-100/O₂-100	—	SiO₂/PA/PBI	FeSA-G/0.3Fe	325	[101]
160	H₂/O₂	—	PBI	Fe-NCP/2.5	357	[96]
230	H₂-100/O₂-100	—	SiO₂/PA/PBI	FeCu/N-CNTs/4	302	[98]
160	H₂-100/O₂-200	—	SiO₂/PA/PBI	Fe-N-C-1100/3	229	[97]

Fig. 16. The aspects are currently being developed and the Aspects that should be emphasized in the future.

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Focus on the catalysts to resist the phosphate poisoning in high-temperature proton exchange membrane fuel cells

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