高温聚合物电解质膜燃料电池膜电极中磷酸分布及调控策略研究进展

doi:10.3866/PKU.WHXB202010071

Abstract

Abstract:

High-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) have the unique advantages of fast electrode reaction kinetics, high CO tolerance, and simple water and thermal management at their operating temperature (140–200 ℃), which are considered as one of the important research directions of PEMFCs. Membrane electrode assemblies (MEAs), as the core component of HT-PEMFCs, are usually fabricated by sandwiching phosphoric acid (PA)-doped polymer membrane (HT-PEM) between two electrodes. Technically, high PA content is required in HT-PEMs to ensure fast proton conduction, since PA acts as a proton transport carrier, while a high content of PA decreases the interaction among polymer molecules, thus enhancing the movement of the polymer molecules and leading to a decrease in the mechanical strength of the polymer membranes. In addition, PA is driven into catalyst layers owing to capillary force caused by micropore structures, crack connectivity, and accessibility. The PA content in the electrodes is also affected by the hydrophilic/hydrophobic characteristics of the catalyst layers and the surface tension of the acid when it is in close contact with the catalyst layers. Furthermore, PA plays an important role in the construction of electrochemical triple-phase boundaries to promote electrochemical reactions in the catalyst layers. Simultaneously, as a liquid or "free molecule", the migration of PA may be accelerated by the current and the water produced, owing to the formation of charged phosphates or hydronium ions. This process encourages the redistribution of PA within the catalyst layers, and results in acid flooding of the catalytic layers and adsorption on the surface of the platinum catalyst, leading to increased mass transfer resistance for the gas reaction and reduced catalyst activity. Moreover, the increase in supplied absolute flow rate and the temperature elevation in the HT-PEMFC process could accelerate the evaporation of PA from the electrolyte membrane, resulting in a decrease in the stability of HT-PEMFC and corrosion of the metal end plate. Therefore, it is crucial to regulate the distribution and migration of PA in MEAs for the construction of HT-PEMFCs with high performance and stability. Hence, this paper reviews the research status of PA distribution in HT-PEM electrodes in recent years, and summarizes the corresponding regulations and optimization strategies as well as its future development trend.

Key words: Fuel cell, Membrane-electrode assembly, High temperature polymer electrolyte membrane, Catalyst layer, Phosphoric acid

Jujia Zhang, Jin Zhang, Haining Wang, Yan Xiang, Shanfu Lu. Advancement in Distribution and Control Strategy of Phosphoric Acid in Membrane Electrode Assembly of High-Temperature Polymer Electrolyte Membrane Fuel Cells[J]. Acta Phys. -Chim. Sin. 2021, 37(9), 2010071. doi: 10.3866/PKU.WHXB202010071

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References 109

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Membranes	Phosphoric acid doping level (PA molecules per repeat unit)	Tensile stress (MPa)	Acid retention capability (%)	Proton conductivity (mS?cm^?1)	References
SiO₂/Cross-linked PBI	23.1	15.0 ± 4.0	57	199@160 ℃	59
α-ZrP/ABPBI	6.5	36.0 ± 3.0	–	49@180 ℃	60
C₃N₄/PES-PVP	6.1	6.0	–	120@180 ℃	62
HPW/PES-PVP	6.6	2.1	–	144@160 ℃	63
carbon dots/PES-PVP	146 a	11.9 ± 1.5	–	86@180 ℃	64
TDAP-PSU	186.4 ^a	2.1	–	46@160 ℃	65
P-g-V-3.82	220.3 ^a	7.94	–	127@160 ℃	66
1,2,3-triazole-functionalized PSU	5.0	13.0	–	27.3@140 ℃	67
g-PBI-20	22.1	6.5	–	154@160 ℃	69
PPT	159.9 ^a	12.0±0.3	82	96@180 ℃	74
ABPBI/IL@SNR	3.4	-	67%	48@180 ℃	77
PBI-SC-5	6.8	8±0.4	82	78@160 ℃	78

Catalyst	Fabrication method	Binder	Addition	Phosphoric acid content (mg?cm^?2)	Gas flow of anode and cathode (L?min^?1)	Current density at 0.6 V@160 ℃ (mA?cm^?2)	References
40% (w) Pt/C	Coating	Phosphonated polysulfones	–	–	0.2/0.2 H₂/O₂	~140	5
40% (w) Pt/C	Spraying	PBI	–	1.125	0.134/0.4 H₂/Air	~100	38
40% (w) Pt/C	Spraying	PBI	–	0.225	0.134/0.4 H₂/Air	~130	38
48.3% (w) PtCo/C	Spraying	PTFE	–	3	0.3/1 H₂/Air	~410	81
40% (w) Pt/C	Ultrasonic Spraying	PTFE	CNT	–	0.10/0.40 H₂/O₂	492	83
40% (w) Pt/C	Spraying	PTFE	Zirconium hydrogen phosphate	–	0.5/1 H₂/Air	400	84
20% Pt/C	Ultrasonic Spraying	PTFE	–	–	λ(H₂) : λ(O₂) = 1.4:2	~200	87
20% (w) Pt/C	Coating	PTFE	–	–	λ(H₂) : λ(O₂) = 1.4:2	~200	87
40% (w) Pt/C	Spraying	PVDF/PBI	–	0.81	0.2/0.2 H₂/O₂	~340	88
40% (w) Pt/C	Spraying	PVDF/PBI	–	0.13	0.2/0.2 H₂/O₂	~120	88

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Advancement in Distribution and Control Strategy of Phosphoric Acid in Membrane Electrode Assembly of High-Temperature Polymer Electrolyte Membrane Fuel Cells

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