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3D printing and carbonisation is used to produce designed gas diffusion layer materials for polymer electrolyte membrane fuel cells (PEMFC). Using a desktop UV 3D printer, designed porous microstructures are printed with micro and macro-scale features. Successful improvement of the pyrolysis process maintains the structural accuracy during carbonisation, reducing the material to electrically conductive carbon. The size of the material allows for testing in a lab scale fuel cell with 1.5 × 1.5 cm electrode size, which shows lower but interesting electrochemical performance (power density of 205 mW cm−2). Challenges associated with integration of a 3D printed structure into a membrane electrode assembly are highlighted, including the low open circuit voltage caused by large amounts of membrane deformation and subsequent hydrogen crossover. This study shows that it is possible to design and manufacture a gas diffusion layer for fuel cells. Numerical simulation on the new GDL structure shows that advective-diffusive transport of oxygen in the 3D printed design is superior to conventional carbon paper. This study serves as the first attempt to implement 3D printed microstructures as GDL into PEMFC. [Display omitted] • A designed carbon gas diffusion layer is manufactured using 3D printing. • Controlled pyrolysis is used to preserve microstructure. • Challenges for 3D printed materials integrated into fuel cells are highlighted. • Simulations show an 8% higher oxygen concentration at the catalyst layer. [ABSTRACT FROM AUTHOR]

PIM-1-based freestanding mixed matrix membranes (MMMs) and thin film nanocomposites (TFNs) were prepared by incorporating porous silica nanosheets (SN) and exfoliated SN (E-SN) derived from natural vermiculite (Verm) in the PIM-1 polymer matrix. In addition, SN were functionalized by sulfonic acid and amine groups (S-SN and N-SN, respectively) and were also used as fillers for the preparation of MMMs. The gas separation performance was evaluated using CO 2 /CH 4 and CO 2 /N 2 (1:1, v:v) binary gas mixtures. Among freestanding membranes, fresh ones (i.e. tested right after preparation) containing 0.05 wt% functionalized SN and E-SN outperformed the neat PIM-1, surpassing the 2008 Robeson upper bound. At the same filler concentration, fresh MMMs with sulfonic acid-functionalized SN (S-SN) exhibited 40% higher CO 2 permeability, 20% higher CO 2 /N 2 selectivity and almost the same CO 2 /CH 4 selectivity as neat PIM-1 membranes. Moreover, after 150 days of aging, these membranes were capable of maintaining up to 68% of their initial CO 2 permeability (compared to 37% for neat PIM-1). When prepared as TFN membranes, the incorporation of 0.05 wt% of S-SN led to 35% higher initial CO 2 permeance and five times higher CO 2 permeance after 28 days. [Display omitted] • Freestanding and thin PIM-1-based films were fabricated using silica nanosheets (SNs). • The prepared MMMs and TFNs were tested for CO 2 /N 2 and CO 2 /CH 4 separation. • PIM-1/sulfonated SNs (0.05 wt%) showed the best initial performance. • The incorporation of SNs partially prevented aging in both TFNs and MMMs. [ABSTRACT FROM AUTHOR]

To improve the performance and durability of phosphoric acid (PA) doped polybenzimidazole (PBI) membranes in high–temperature proton exchange membrane fuel cells (HT–PEMFCs), in this work, as–received natural muscovite (Mus), a clay material, was successfully incorporated into PBI matrix as an inorganic filler through the doctor blade method. The amount of Mus was varied (0.5–2 wt%) to explore its impact on the proton conductivity, mechanical and dimensional stability, power density, durability, and acid retention ability of the composite membranes. As the incorporation of Mus into membranes can introduce interactions with polymer chains and PA molecules to afford additional proton transport pathways at the interfaces in Mus–PBI and Mus–PA crosslinks, the membrane with 1 wt% Mus showed highest power density of 586 mW cm−2 at 150 °C without humidification, 24% higher than the pure PBI membrane (474 mW cm−2). Meanwhile, the PA doped composite membrane with 1 wt% Mus also displayed the highest mechanical strength (7.5 MPa) and lowest dimensional swelling (70.99% in area swelling and 202% in volume swelling). Compared with the pristine PBI membrane, the composite membranes had significantly improved durability under accelerated stress test (AST). The decreased ohmic resistance and increased polarization resistance after AST are related to the membrane thinning and the loss of catalyst active area, respectively. Most importantly, it was found that the strong interactions between Mus and PA molecules lead to improved acid retention ability of the composite membranes, thus less leached acid from the composite membrane reduces the negative effects on the catalyst degradation to alleviate degradation on cell performance and durability. [Display omitted] • Natural muscovite was successfully incorporated into PBI membranes using the doctor blade method. • The prepared composite membranes show better power density and durability than the pure PBI membrane. • The interactions between Mus and PA explored by EDS, TGA and XPS benefit improved acid retention ability. [ABSTRACT FROM AUTHOR]

A direct methanol fuel cell (DMFC) is one prominent alternative energy technology. However, there are many problems that prevent the commercialization of DMFC, such as methanol crossover, low power density, and degradation of the membrane. To resolve these issues, functionalized graphene oxide (GO) and calcium hydroxy phosphate (CHP) were incorporated into the Nafion membrane to make a composite membrane. The content of the CHP was varied to determine and further investigation involved spraying the same amount of CHP onto the Nafion membrane to compare with the composite membrane. The fillers were characterized using Fourier-transform infrared spectroscopy and X-ray Powder Diffraction. The ex-situ tests investigated water uptake, solubility, and chemical degradation, while the in-situ tests investigated electrochemical impedance (EIS), methanol permeability, fuel cell performance, and durability. Adding both 1 wt% of CHP and 0.05 wt% functionalized GO into the Nafion membrane, resulting in a 1.86-fold higher durability than that of recast Nafion. In addition, the maximum power density of the composite membrane was 1.34-fold higher (75.41 mW/cm2) than that of the recast Nafion (56.11 mW/cm2) at 1 M methanol and 70 °C. At 2 M methanol and 70 °C, the maximum power density of the composite membrane increased to 80.19 mW/cm2 but then decreased to 46.00 mW/cm2 when the methanol feed increased to 4 M, due to the large amount of methanol crossover. • 1 wt% CHP functionalized 0.05 wt% GO/Nafion was used for DMFC. • The composite membrane was 1.86-fold higher durability than that of recast Nafion. • Power density was 1.34-fold higher than that of Nafion at 1 M methanol and 70 °C. • At 2 M methanol and 70 °C was the optimum condition for DMFC. [ABSTRACT FROM AUTHOR]

• Operando synchrotron X-ray study on Phosphorus and Platinum migration. • Graphene-related-material applied as interventional materials for comparison. • X-ray Absorption Near Edge Structure applied to study chemical structural change. • Conducting mechanistic studies via the three-phase interface. • Performance and durability of high-temperature proton exchange membrane fuel cells. The application of high-temperature proton exchange membrane fuel cells (HT-PEMFCs) addresses challenges in water management, fuel purity, and overheating under high current density. However, phosphoric acid (PA) migration hinders their development. This study uses synchrotron-based X-ray fluorescence spectroscopy to investigate PA and catalyst migration. Interventions with single-layer graphene and electrochemically exfoliated graphene oxide improve performance and durability. X-ray absorption spectroscopy provides insights into relevant mechanisms, advancing understanding of membrane electrode assembly preparation and the intricate influences of PA and catalyst migration on performance and durability in HT-PEMFCs. [ABSTRACT FROM AUTHOR]

• Defect-free ZIF-8/GO/PIM-1 thin-film nanocomposite (TFN) membranes were fabricated. • 2D ZIF/GO was produced by in situ growth of ZIF-8 on GO sheets as a continuous, uniform and thin layer. • ZIF-8/GO composite results in high dispersity and compatibility of ZG within PIM-1. • PIM-1 infiltration into PVDF substrate was avoided by water pre-impregnation. • ZIF-8/GO/PIM-1 TFN membranes display a high PSI (228 kg m−2h−1). In this work, thin film nanocomposite (TFN) membranes of super-glassy polymer PIM-1 containing zeolitic imidazolate framework-8 (ZIF-8)/graphene oxide (GO) composites (ZG) have been prepared by dip-coating onto water pre-impregnated polyvinylidene fluoride (PVDF) substrates. Higher flux and improved separation factors as compared to bare PIM-1 thin film composite (TFC) membranes have been achieved in organophilic pervaporation; for an aqueous feed solution with 5 wt% of butanol at 65 °C, a total permeate flux of 7.9 ± 0.69 kg m−2h−1 and a separation factor (β BtOH/H2O) of 29.9 ± 1.99 have been obtained with a TFC membrane containing 0.5 wt% of ZG filler. The pervaporation separation index (PSI) of this membrane (228 kg m−2h−1) is amongst the highest values reported in the literature. This excellent performance is attributed to the formation of a defect-free PIM-1 active layer (<1 μm) and the hydrophobic nature of the ZG fillers. [ABSTRACT FROM AUTHOR]

In this work, a 3D-printed reactor was designed to enable natural graphite flakes to be used for electrochemical exfoliation to quickly obtain graphene oxide. Graphite foil as a typical raw material of electrochemical exfoliation was also exfoliated for comparison. Under the same conditions (10 V, 1 mol L-1 ammonium sulphate solution as electrolyte), the graphene products obtained by one-step electrochemical exfoliation using natural graphite flakes based on the reactor, have a significantly higher degree of oxidation than products obtained using graphite foil (the oxygen content is increased by 50.2%). In addition, the degree of oxidation can be further increased by increasing the electrolyte concentration or reaction time. This design achieves one-step exfoliation using natural graphite flakes to obtain graphene oxide with tunable oxygen content in short time without using any strong oxidants or strong acids. The as-prepared electrochemically exfoliated graphene oxide (EGO) was used to prepare polybenzimidazole (PBI)/graphene oxide (GO) composite membranes for high-temperature polymer electrolyte membrane fuel cells (HTPEMFC). The 0.5%, 1% and 2% EGO loadings in the PBI membrane increased the peak power density by 13.8%, 24.4% and 29.2%, respectively. Image 1 • The use of natural graphite flakes as raw materials for electrochemical exfoliation. • No oxidant and acid used to obtain graphene oxide. • A novel reactor design achieves the above goals. • Electrochemically exfoliated graphene oxide enhances the performance of PBI membrane. [ABSTRACT FROM AUTHOR]