Abstract:We report the synthesis of a new fuel cell membrane, poly((vinyloxy)ethanesulfonic acid)-grafted poly(ethylene-co-tetrafluoroethylene) (ETFE) film by simultaneous radiation grafting of 2-chloroethyl vinyl ether onto ETFE film followed by sulfonation. The effects of various irradiation conditions such as the solvents, dose rate, and monomer concentration on the degree of grafting were investigated in detail. The sulfonation procedure of the grafted ETFE films used to replace the chlorine group with a sulfonic a… Show more
“…These line maps were recorded so that the Raman data could be validated with an EDX line map (Fig. 6 (bottom)): as the F distribution represents the ETFE backbone and the Cl distribution represents the grafts (-CH 2 Cl groups), 35 the grafting level is represented by the Cl/F ratio. A comparison of Fig.…”
Section: Raman Micro-spectroscopic and Edx Datamentioning
High performance benzyltrimethylammonium-type alkaline anion-exchange membranes (AEM), for application in electrochemical devices such as anion-exchange membrane fuel cells (AEMFC), were prepared by the radiation grafting (RG) of vinylbenzyl chloride (VBC) onto 25 μm thick poly(ethylene-co-tetrafluoroethylene) (ETFE) films followed by amination with trimethylamine. Reductions in electron-beam absorbed dose and amount of expensive, potentially hazardous VBC were achieved by using water as a diluent (reduced to 30 – 40 kGy absorbed dose and 5%vol VBC) instead of the prior-art method that used organic propan-2-ol diluent (required 70 kGy dose and 20%vol VBC monomer). Furthermore, the water from the aqueous grafting mixture was easily separated from residual monomer (after cooling) and was reused for a further grafting reaction: the resulting AEM exhibited an ion-exchange capacity of 2.1 mmol g-1 (cf. 2.1 mmol g-1 for the AEM made using fresh grafting mixture). The lower irradiation doses resulted in mechanically stronger RG-AEMs compared to the reference RG-AEM synthesised using the prior-art method. A further positive off-shoot of the optimisation process was the discovery that using water as a diluent resulted in an enhanced (i.e. more uniform) distribution of VBC grafts as proven by Raman microscopy and corroborated using EDX analysis: this led to enhancement in the Cl- anion-conductivities (up to 68 mS cm-1 at 80°C for the optimised fully hydrated RG-AEMs vs. 48 mS cm-1 for the prior-art RG-AEM reference). A down-selected RG-AEM of ion-exchange capacity = 2.0 mmol g-1, that was synthesised using the new greener protocol with 30 kGy electron-beam absorbed dose, led to an exceptional beginning-of-life H2/O2 AEMFC peak power density of 1.16 W cm−2 at 60°C in a benchmark test using industrial standard Pt-based electrocatalysts and unpressurised gas supplies: this was higher than the 0.91 W cm-1 obtained with the reference RG-AEM (IEC = 1.8 mmol g-1) synthesised using the prior-art protocol
“…These line maps were recorded so that the Raman data could be validated with an EDX line map (Fig. 6 (bottom)): as the F distribution represents the ETFE backbone and the Cl distribution represents the grafts (-CH 2 Cl groups), 35 the grafting level is represented by the Cl/F ratio. A comparison of Fig.…”
Section: Raman Micro-spectroscopic and Edx Datamentioning
High performance benzyltrimethylammonium-type alkaline anion-exchange membranes (AEM), for application in electrochemical devices such as anion-exchange membrane fuel cells (AEMFC), were prepared by the radiation grafting (RG) of vinylbenzyl chloride (VBC) onto 25 μm thick poly(ethylene-co-tetrafluoroethylene) (ETFE) films followed by amination with trimethylamine. Reductions in electron-beam absorbed dose and amount of expensive, potentially hazardous VBC were achieved by using water as a diluent (reduced to 30 – 40 kGy absorbed dose and 5%vol VBC) instead of the prior-art method that used organic propan-2-ol diluent (required 70 kGy dose and 20%vol VBC monomer). Furthermore, the water from the aqueous grafting mixture was easily separated from residual monomer (after cooling) and was reused for a further grafting reaction: the resulting AEM exhibited an ion-exchange capacity of 2.1 mmol g-1 (cf. 2.1 mmol g-1 for the AEM made using fresh grafting mixture). The lower irradiation doses resulted in mechanically stronger RG-AEMs compared to the reference RG-AEM synthesised using the prior-art method. A further positive off-shoot of the optimisation process was the discovery that using water as a diluent resulted in an enhanced (i.e. more uniform) distribution of VBC grafts as proven by Raman microscopy and corroborated using EDX analysis: this led to enhancement in the Cl- anion-conductivities (up to 68 mS cm-1 at 80°C for the optimised fully hydrated RG-AEMs vs. 48 mS cm-1 for the prior-art RG-AEM reference). A down-selected RG-AEM of ion-exchange capacity = 2.0 mmol g-1, that was synthesised using the new greener protocol with 30 kGy electron-beam absorbed dose, led to an exceptional beginning-of-life H2/O2 AEMFC peak power density of 1.16 W cm−2 at 60°C in a benchmark test using industrial standard Pt-based electrocatalysts and unpressurised gas supplies: this was higher than the 0.91 W cm-1 obtained with the reference RG-AEM (IEC = 1.8 mmol g-1) synthesised using the prior-art protocol
“…Radiation grafting can be carried out either by simultaneous or pre-irradiation methods [ 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 ]. In the former, both the monomer and base films are irradiated simultaneously, and the grafting was carried out under the irradiation environments [ 19 , 20 ], while in the latter, the base films are irradiated initially and the grafting is performed after irradiation [ 21 , 22 , 23 ]. Homopolymerization in the monomer solution is a solution-phase reaction that strongly affects graft polymerization and lowers monomer utilization.…”
Reversible addition-fragmentation chain transfer (RAFT) agent was added into a simultaneous radiation grafting system and its effects on graft polymerization and homopolymerization were investigated. Chloromethylstyrene (CMS) was graft polymerized onto ethylene-tetrafluoroethylene copolymer (ETFE) films under γ-ray sources via simultaneous irradiation. The non-grafted poly(CMS) in the grafted films were extracted by xylene at 120 • C. The poly(CMS) was characterized by NMR and GPC instruments. Addition of the RAFT agent suppressed both graft polymerization and homopolymerization. However, under a high concentration of RAFT agent, the homopolymerization in the monomer solution could occur through a typical RAFT polymerization while polymerization in the ETFE films proceeded via RAFT and conventional radical polymerization, resulting in poly(CMS) in the ETFE films with molecular weight dispersity higher than 1.0 but lower than that without RAFT agent. Furthermore, it was found that the molecular weight of the poly(CMS) in the ETFE films was several times higher than that of the poly(CMS) in the monomer solution.
“…Polymer electrolyte membrane fuel cell (PEMFC) displays the most promising alternative source of energy for a variety of portable electronic devices, stationary, and vehicle applications . The PEMFC operates at relatively low temperature (60–100°C) and has a high specific power and compactness.…”
Highly filled graphite polybenzoxazine composites as bipolar plate material for polymer electrolyte membrane fuel cell (PEMFC) are developed. At the maximum graphite content of 80 wt % (68 vol %), storage modulus was increased from 5.9 GPa of the neat polybenzoxazine matrix to 23 GPa in the composite. Glass transition temperatures (T g ) of the composites were ranging from 176 C to 195 C and the values substantially increased with increasing the graphite contents. Thermal conductivity as high as 10.2 W/ mK and electrical conductivity of 245 S cm 21 were obtained in the graphite filled polybenzoxazine at its maximum graphite loading. The obtained properties of the graphite filled polybenzoxazine composites exhibit most values exceed the United States department of energy requirements for PEMFC applications.
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