Active and highly durable supported catalysts for proton exchange membrane electrolysers† † Electronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d4ey00026a
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ABSTRACT:
SUBMITTER: Belami D
PROVIDER: S-EPMC11375952 | biostudies-literature | 2024 Jun
REPOSITORIES: biostudies-literature
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Project description:A stable and cost effective oxygen evolution reaction (OER) catalyst is crucial for the large-scale market penetration of proton exchange membrane (PEM) water electrolyzers. We show that the synthesis of iridium nanoparticles in either low purity ethanol or water, or in the absence of a surfactant, is detrimental to the electrocatalytic properties of the materials. Adding NaBH4 in excess improves the purity of the catalyst enhancing the OER activity up to 100 A gIr-1 at 1.51 V vs. RHE, the highest value reported so far for high purity Ir nanoparticles. The measured OER activity correlates with the capacitive current rather than with the charge corresponding to the IrIII/IrIV oxidation peak. Operando near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) on membrane electrode assemblies (MEAs) with the synthesized catalysts reveals a metallic core surrounded by a thin layer of IrIII/IV oxides/hydroxides. Oxidation of IrIII leaves behind a porous ultrathin layer of IrIV oxides/hydroxides, which dominate the surface during the OER, while IrV was not detected.
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Project description:Rapid degradation of cell performance still remains a significant challenge for proton exchange membrane fuel cell (PEMFC). In this work, we develop novel CeO2 nanocubes-graphene oxide nanocomposites as durable and highly active catalyst support for proton exchange membrane fuel cell. We show that the use of CeO2 as the radical scavenger in the catalysts remarkably improves the durability of the catalyst. The catalytic activity retention of Pt-graphene oxide-8 wt.% CeO2 nanocomposites reaches as high as 69% after 5000 CV-cycles at a high voltage range of 0.8-1.23 V, in contrast to 19% for that of the Pt-graphene oxide composites. The excellent durability of the Pt-CeO2 nanocubes-graphene oxide catalyst is attributed to the free radical scavenging activity of CeO2, which significantly slows down the chemical degradation of Nafion binder in catalytic layers, and then alleviates the decay of Pt catalysts, resulting in the excellent cycle life of Pt-CeO2-graphene oxide nanocomposite catalysts. Additionally, the performance of single cell assembled with Nafion 211 membrane and Pt-CeO2-graphene oxide catalysts with different CeO2 contents in the cathode as well as the Pt-C catalysts in the anode are also recorded and discussed in this study.
| S-EPMC4261163 | biostudies-other
Project description:Although the acidic oxygen evolution reaction (OER) plays a crucial role in proton-exchange membrane water electrolysis (PEMWE) devices, challenges remain owing to the lack of efficient and acid-stable electrocatalysts. Herein, we present a low-iridium electrocatalyst in which tensile-strained iridium atoms are localized at manganese-oxide surface cation sites (TS-Ir/MnO2) for high and sustainable OER activity. In situ synchrotron characterizations reveal that the TS-Ir/MnO2 can trigger a continuous localized lattice oxygen-mediated (L-LOM) mechanism. In particular, the L-LOM process could substantially boost the adsorption and transformation of H2O molecules over the oxygen vacancies around the tensile-strained Ir sites and prevent further loss of lattice oxygen atoms in the inner MnO2 bulk to optimize the structural integrity of the catalyst. Importantly, the resultant PEMWE device fabricated using TS-Ir/MnO2 delivers a current density of 500 mA cm-2 and operates stably for 200 h.
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Project description:The performance of four polymorphs of manganese (Mn) dioxides as the catalyst for the oxygen evolution reaction (OER) in proton exchange membrane (PEM) electrolysers was examined. The comparison of the activity between Mn oxides/carbon (Mn/C), iridium oxide/carbon (Ir/C) and platinum/carbon (Pt/C) under the same condition in PEM electrolysers showed that the γ-MnO2/C exhibited a voltage efficiency for water electrolysis comparable to the case with Pt/C, while lower than the case with the benchmark Ir/C OER catalyst. The rapid decrease in the voltage efficiency was observed for a PEM electrolyser with the Mn/C, as indicated by the voltage shift from 1.7 to 1.9 V under the galvanostatic condition. The rapid deactivation was also observed when Pt/C was used, indicating that the instability of PEM electrolysis with Mn/C is probably due to the oxidative decomposition of carbon supports. The OER activity of the four types of Mn oxides was also evaluated at acidic pH in a three-electrode system. It was found that the OER activity trends of the Mn oxides evaluated in an acidic aqueous electrolyte were distinct from those in PEM electrolysers, demonstrating the importance of the evaluation of OER catalysts in a real device condition for future development of noble-metal-free PEM electrolysers.
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Project description:Cost reduction and high efficiency are the mayor challenges for sustainable H2 production via proton exchange membrane (PEM) electrolysis. Titanium-based components such as bipolar plates (BPP) have the largest contribution to the capital cost. This work proposes the use of stainless steel BPPs coated with Nb and Ti by magnetron sputtering physical vapor deposition (PVD) and vacuum plasma spraying (VPS), respectively. The physical properties of the coatings are thoroughly characterized by scanning electron, atomic force microscopies (SEM, AFM); and X-ray diffraction, photoelectron spectroscopies (XRD, XPS). The Ti coating (50 μm) protects the stainless steel substrate against corrosion, while a 50-fold thinner layer of Nb decreases the contact resistance by almost one order of magnitude. The Nb/Ti-coated stainless steel bipolar BPPs endure the harsh environment of the anode for more than 1000 h of operation under nominal conditions, showing a potential use in PEM electrolyzers for large-scale H2 production from renewables.
| S-EPMC5353588 | biostudies-literature
Project description:Chemically durable proton exchange membranes containing free radical scavengers have technically matured in recent years, and commercial products have come into the market. The most general type of free radical scavenger is ceria, which has been proven in many studies. However, the migration of cerium is inevitable in raw ceria particles, and the migrated cerium species can aggregate in catalyst layers, causing performance loss of fuel cells. In this work, the morphology of ceria was changed from conventional nanoparticles to nanorods, and the migration of cerium was mitigated significantly. Both ex situ Fenton's degradation tests and in situ fuel cell accelerated degradation tests (ADTs) indicated that ceria nanorods have free radical scavenging properties comparable to those of ceria nanoparticles. Moreover, the immobilization of ceria particles and antidissolving properties have been verified by Fenton's degradation tests, electric field tests and fuel cell ADTs.
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Project description:A new hydrocarbon-based (HC) composite membrane was developed using liquid crystal polymer (LCP)-nonwoven fabrics for application in proton exchange membrane water electrolysis (PEMWE). A copolymer of sulfonated poly(arylene ether sulfone) with a sulfonation degree of 50 mol% (SPAES50) was utilized as an ionomer for the HC membranes and impregnated into the LCP-nonwoven fabrics without any surface treatment of the LCP. The physical interlocking structure between the SPAES50 and LCP-nonwoven fabrics was investigated, validating the outstanding mechanical properties and dimensional stability of the composite membrane in comparison to the pristine membrane. In addition, the through-plane proton conductivity of the composite membrane at 80 °C was only 15% lower than that of the pristine membrane because of the defect-free impregnation state, minimizing the decrease in the proton conductivity caused by the non-proton conductive LCP. During the electrochemical evaluation, the superior cell performance of the composite membrane was evident, with a current density of 5.41 A/cm2 at 1.9 V, compared to 4.65 A/cm2 for the pristine membrane, which can be attributed to the smaller membrane resistance of the composite membrane. From the results of the degradation rates, the prepared composite membrane also showed enhanced cell efficiency and durability during the PEMWE operations.
| S-EPMC10181224 | biostudies-literature
Project description:For further commercializing proton-exchange membrane fuel cells, it is crucial to attain long-term durability while achieving high performance. In this study, a strategy for modifying commercial Nafion membranes by introducing ultrathin multiwalled carbon nanotubes (MWCNTs)/CeO2 layers on both sides of the membrane was developed to construct a mechanically and chemically reinforced membrane electrode assembly. The dispersion properties of the MWCNTs were greatly improved through chemical modification with acid treatment, and the mixed solution of MWCNTs/CeO2 was uniformly prepared through a high-energy ball-milling process. By employing a spray-coating technique, the ultrathin MWCNTs/CeO2 layers were introduced onto the membrane surfaces without any agglomeration problem because the solvent rapidly evaporated during the layer-by-layer stacking process. These ultrathin and highly dispersed MWCNTs/CeO2 layers effectively reinforced the mechanical properties and chemical durability of the membrane while minimizing the performance drop despite their non-ion-conducting properties. The characteristics of the MWCNTs/CeO2 layers and the reinforced Nafion membrane were investigated using various in situ and ex situ measurement techniques; in addition, electrochemical measurements for fuel cells were conducted.
| S-EPMC9698217 | biostudies-literature
Project description:We demonstrated highly active and durable hybrid catalysts (HCs) composed of small reduced graphene oxide (srGO) and carbon nanotubes (CNTs) for use as oxygen reduction reaction (ORR) catalysts in proton exchange membrane fuel cells. Pt/srGO and Pt/CNTs were prepared by loading Pt nanoparticles onto srGO and CNTs using a polyol process, and HCs with different Pt/CNT and Pt/srGO ratios were prepared by mechanically mixing the two components. The prepared HCs consisted of Pt/CNTs well dispersed on Pt/srGO, with catalyst HC55, which was prepared using Pt/srGO and Pt/CNTs in a 5:5 ratio, exhibiting excellent oxygen reduction performance and high stability over 1000 cycles of the accelerated durability test (ADT). In particular, after 1000 cycles of the ADT, the normalized electrochemically active surface area of Pt/HC55 decreased by 11.9%, while those of Pt/srGO and Pt/C decreased by 21.2% and 57.6%, respectively. CNTs have strong corrosion resistance because there are fewer defect sites on the surface, and the addition of CNTs in rGO further improved the durability and the electrical conductivity of the catalyst. A detailed analysis of the structural and electrochemical properties of the synthesized catalysts suggested that the synergetic effects of the high specific surface area of srGO and the excellent electrical conductivity of CNTs were responsible for the enhanced efficiency and durability of the catalysts.
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Project description:The controlled formation of a functional adlayer at the catalyst-water interface is a highly challenging yet potentially powerful strategy to accelerate proton transfer and deprotonation for ultimately improving the performance of proton-exchange membrane water electrolysis (PEMWE). In this study, the synthesis of robust vinylene-linked covalent organic frameworks (COFs) possessing high proton conductivities is reported, which are subsequently hybridized with ruthenium dioxide yielding high-performance anodic catalysts for the acidic oxygen evolution reaction (OER). In situ spectroscopic measurements corroborated by theoretical calculations reveal that the assembled hydrogen bonds formed between COFs and adsorbed oxo-intermediates effectively orient interfacial water molecules, stabilizing the transition states for intermediate formation of OER. This determines a decrease in the energy barriers of proton transfer and deprotonation, resulting in exceptional acidic OER performance. When integrated into a PEMWE device, the system achieves a record current density of 1.0 A cm-2 at only 1.54 V cell voltage, with a long-term stability exceeding 180 h at industrial-level 200 mA cm-2. The approach relying on the self-assembly of an oriented hydrogen-bonded adlayer highlights the disruptive potential of COFs with customizable structures and multifunctional sites for advancing PEMWE technologies.
| S-EPMC11923516 | biostudies-literature