Nafion-sulfonated silica composite membrane for proton exchange membrane fuel cells under operating low humidity condition

Oh, Kwangjin; Kwon, Osung; Son, Byungrak; Lee, Dong Ha; Shanmugam, Sangaraju

doi:10.1016/j.memsci.2019.04.031

Cited by 113 publications

(85 citation statements)

References 45 publications

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“…The existence of a ─OH bond, which was associated with the sulfate group on the surface of the nanoparticle, was confirmed by the peak at 1632 cm −1 . The broad peak between 3600 and 3200 cm −1 suggests the presence of hydroxyl groups in diblock at one terminal, which is in the form of absorbed water because of interaction with sulfonic groups . The intensity of the absorption bands for the nanocomposite membrane in this region is significantly stronger than plain SPEEK, because of the hygroscopic nature of nanoparticles.…”

Section: Resultsmentioning

confidence: 84%

“…63,64 The broad peak between 3600 and 3200 cm −1 suggests the presence of hydroxyl groups 46 in diblock at one terminal, which is in the form of absorbed water because of interaction with sulfonic groups. 65 The intensity of the absorption bands for the nanocomposite membrane in this region is significantly stronger than plain SPEEK, because of the hygroscopic nature of nanoparticles. The presence of Ti-O and Zr-O bond were corroborated by the peaks amongst 900 to 400 cm −1 .…”

Section: Characterization Of the Optimum Nanocomposite Membranementioning

confidence: 95%

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Simultaneous improvement of ionic conductivity and oxidative stability of sulfonated poly(ether ether ketone) nanocomposite proton exchange membrane for fuel cell application

2020

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Summary Simultaneous high proton conductivity with high oxidative stability is one of the major concerns in the proton exchange membrane (PEM) preparation. With this perspective, different loadings of the sulfated zirconia‐titania, a binary metal oxide that possesses enhanced physicochemical properties, nanoparticle in sulfonated poly(ether ether ketone) (SPEEK) polymer were evaluated by the response surface method to obtain the novel PEM with boosted proton conductivity and oxidative stability. Two models for correlation of proton conductivity and oxidative stability (in Fenton solution) with two independent factors, including sulfonation time and the weight percent of the nanoparticle loading, were obtained by central composite design. The optimum parameters to attain the highest proton conductivity with oxidative stability are found to be the sulfonation time of 6.48 hours and the nanoparticle weight percent of 10.12%. The nanoparticle loading was found to be the more significant factor in the proton conductivity model, while the sulfonation time in the oxidative stability model was the main affecting factor. The optimal membranes were characterized by 1H NMR, electrochemical impedance spectroscopy, Fenton test, Fourier transform infrared (FTIR), thermal gravimetric analysis (TGA), water uptake, swelling ratio, and atomic force microscopy (AFM) analysis. The results indicate that the introduction of the optimal contents of SZrTi nanoparticle into the polymer matrix would improve the water uptake and consequently the proton conductivity at a higher temperature while keeping the swelling ratio at an acceptable range. The highest achieved proton conductivity by the resulted nanocomposite was 29.21 mS cm−1 at 120°C with 186‐minute durability in the Fenton's reagent. Moreover, the maximum peak power density of 199 mW cm−2 was achieved at 90°C and 100% RH for the single‐cell performance test of nanocomposite‐based membrane electrode assembly (MEA), while it was recorded at 112 mW cm−2 for commercial MEA. Acceptable dispersion of SZrTi nanoparticle in the SPEEK matrix causes negligible fuel crossover flux (eg, 0.35 × 10−6 mmol s−1 cm−2 and 12.49 × 10−6 mmol s−1 cm−2 for nanocomposite‐based MEA and commercial MEA, respectively), which is indispensable to improve the mechanical and chemical stability. So, the novel prepared nanocomposite SPEEK‐based membrane would be a promising alternative for the Nafion membrane at moderate to high temperatures. Highlights Sulfated ZrO2‐TiO2 binary oxide was introduced into the SPEEK polymer matrix. Chemical stability and proton conductivity were promoted by design of experiments. The nanoparticle loading was the main factor in the proton conductivity model. Sulfonation time in the oxidative stability model was the most affecting factor. Fuel crossover was omitted because of the presence of SZrTi nanoparticle in the SPEEK matrix.

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Section: Resultsmentioning

confidence: 84%

Section: Characterization Of the Optimum Nanocomposite Membranementioning

confidence: 95%

Simultaneous improvement of ionic conductivity and oxidative stability of sulfonated poly(ether ether ketone) nanocomposite proton exchange membrane for fuel cell application

2020

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“…The fabricated composite membranes displayed greater water uptake of 61% at 100 • C compared to 29% for recast Nafion. This improvement in water uptake led to better proton conductivity at 100 The performance of sulphonated silica Nafion composites where assessed where the filler was synthesised with a simple sol-gel calcination process [148]. Optimisation studies revealed that a 1% filler was the optimum loading, outperforming 0.5, 1.5% and recast Nafion.…”

Section: Inorganic Fillersmentioning

confidence: 99%

Composite Polymers Development and Application for Polymer Electrolyte Membrane Technologies—A Review

et al. 2020

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Nafion membranes are still the dominating material used in the polymer electrolyte membrane (PEM) technologies. They are widely used in several applications thanks to their excellent properties: high proton conductivity and high chemical stability in both oxidation and reduction environment. However, they have several technical challenges: reactants permeability, which results in reduced performance, dependence on water content to perform preventing the operation at higher temperatures or low humidity levels, and chemical degradation. This paper reviews novel composite membranes that have been developed for PEM applications, including direct methanol fuel cells (DMFCs), hydrogen PEM fuel cells (PEMFCs), and water electrolysers (PEMWEs), aiming at overcoming the drawbacks of the commercial Nafion membranes. It provides a broad overview of the Nafion-based membranes, with organic and inorganic fillers, and non-fluorinated membranes available in the literature for which various main properties (proton conductivity, crossover, maximum power density, and thermal stability) are reported. The studies on composite membranes demonstrate that they are suitable for PEM applications and can potentially compete with Nafion membranes in terms of performance and lifetime.

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“…In the MD simulations, the simulation box size 4×4×4 nm 3 was built. The simulation processes were almost the same as used in previous paper with periodic conditions in xyz directions [37,38].…”

Section: Molecular Dynamics Simulation Of Hygroscopicitymentioning

confidence: 99%

“…Proton exchange membrane fuel cells (PEMFCs) are one of the most promising energy conversion devices owing to their advantageous features such as high efficiency, eco-friendliness, and rapid startup. [1][2][3][4] As the core component of PEMFCs, proton exchange membranes (PEMs) act as both a proton conductor and a fuel/oxidizer separator. [5][6][7] Water plays a vital role in the proton conduction process in PEMs.…”

Section: Introductionmentioning

confidence: 99%

Trifluoromethanesulfonimide-based hygroscopic semi-interpenetrating polymer network for enhanced proton conductivity of nafion-based proton exchange membranes at low humidity

Sun

Xiong

et al. 2020

Journal of Membrane Science

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In this study, a super acid with impressive hygroscopicity, 1-[3-(methacryloyloxy)propylsulfonyl]-1-(trifluoromethanesulfonyl)imide (MPTI), is exploited to improve the proton conductivity of PEMs at low humidity. Importantly, MPTI can deliquesce into an aqueous solution by capturing moisture from air at a considerable rate. Investigation of the hygroscopicity of MPTI and the corresponding mechanism by molecular dynamics simulation show a total interaction energy between MPTI and water of-368.13 kJ mol-1 , which greatly exceeds those of model derivatives with other typical hygroscopic groups. To apply MPTI in PEMs and prevent leakage, MPTI is incorporated into a semi-interpenetrating polymer network via in situ polymerization, and Nafionbased composite membranes are fabricated. The water uptake of the obtained hybrid membranes is substantially increased by up to 66.61% at 40% RH and 90.04% at 95% RH. This optimization of the water environment facilitates the dissociation of protons and the formation of hydrogen bond networks for high-speed proton conduction. As a result, the proton conductivity of the membranes increases by up to two orders of magnitude at low humidity. Notably, this composite membrane enhanced the performance of a single fuel cell at 60% RH by 41.9%.

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Nafion-sulfonated silica composite membrane for proton exchange membrane fuel cells under operating low humidity condition

Cited by 113 publications

References 45 publications

Simultaneous improvement of ionic conductivity and oxidative stability of sulfonated poly(ether ether ketone) nanocomposite proton exchange membrane for fuel cell application

Simultaneous improvement of ionic conductivity and oxidative stability of sulfonated poly(ether ether ketone) nanocomposite proton exchange membrane for fuel cell application

Composite Polymers Development and Application for Polymer Electrolyte Membrane Technologies—A Review

Trifluoromethanesulfonimide-based hygroscopic semi-interpenetrating polymer network for enhanced proton conductivity of nafion-based proton exchange membranes at low humidity

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