A hydrogen-organic hybrid flow battery (FB) has been developed using methylene blue (MB) in an aqueous acid electrolyte with a theoretical positive electrolyte energy storage capacity of 65.4 A h L. MB paired with the versatile H/H redox couple at the negative electrode forms the H-MB rechargeable fuel cell, with no loss in capacity (5 sig.
View Article and Find Full Text PDFThis study introduces a simple method to produce ultralow loading catalyst-coated membrane electrodes, with an integrated carbon "nanoporous layer", for use in polymer electrolyte membrane fuel cells or other electrochemical devices. This approach allows fabrication of electrodes with loadings down to 5.2 μg cm on the anode and cathode (total 10.
View Article and Find Full Text PDFThe mechanistic understanding of electrochemical CO reduction reaction (CO RR) requires a rapid and accurate characterisation of product distribution to unravel the activity and selectivity, which is yet hampered by the lack of advanced correlative approaches. Here, we present the time-resolved identification of CO RR products by using the synchronised electrochemistry-mass spectrometry (sEC-MS). Transients in product formation can be readily captured in relation to electrochemical conditions.
View Article and Find Full Text PDFWe examine the performance of a number of single-atom M-N/C electrocatalysts with a common structure in order to deconvolute the activity of the framework N/C support from the metal M-N sites in M-N/Cs. The formation of the N/C framework with coordinating nitrogen sites is performed using zinc as a templating agent. After the formation of the electrically conducting carbon-nitrogen metal-coordinating network, we (trans)metalate with different metals producing a range of different catalysts (Fe-N/C, Co-N/C, Ni-N/C, Sn-N/C, Sb-N/C, and Bi-N/C) without the formation of any metal particles.
View Article and Find Full Text PDFThere are a number of critical requirements for electrolytes in aqueous redox flow batteries. This paper reviews organic molecules that have been used as the redox-active electrolyte for the positive cell reaction in aqueous redox flow batteries. These organic compounds are centred around different organic redox-active moieties such as the aminoxyl radical (TEMPO and N-hydroxyphthalimide), carbonyl (quinones and biphenols), amine (e.
View Article and Find Full Text PDFRedox flow batteries (RFBs) are promising for large-scale long-duration energy storage owing to their inherent safety, decoupled power and energy, high efficiency, and longevity. Membranes constitute an important component that affects mass transport processes in RFBs, including ion transport, redox-species crossover, and the net volumetric transfer of supporting electrolytes. Hydrophilic microporous polymers, such as polymers of intrinsic microporosity (PIM), are demonstrated as next-generation ion-selective membranes in RFBs.
View Article and Find Full Text PDFRedox flow batteries (RFBs) have great potential for long-duration grid-scale energy storage. Ion-conducting membranes are a crucial component in RFBs, allowing charge-carrying ions to transport while preventing the cross-mixing of redox couples. Commercial Nafion membranes are widely used in RFBs, but their unsatisfactory ionic and molecular selectivity, as well as high costs, limit the performance and the widespread deployment of this technology.
View Article and Find Full Text PDFRedox flow batteries (RFBs) based on aqueous organic electrolytes are a promising technology for safe and cost-effective large-scale electrical energy storage. Membrane separators are a key component in RFBs, allowing fast conduction of charge-carrier ions but minimizing the cross-over of redox-active species. Here, we report the molecular engineering of amidoxime-functionalized Polymers of Intrinsic Microporosity (AO-PIMs) by tuning their polymer chain topology and pore architecture to optimize membrane ion transport functions.
View Article and Find Full Text PDFRedox flow batteries using aqueous organic-based electrolytes are promising candidates for developing cost-effective grid-scale energy storage devices. However, a significant drawback of these batteries is the cross-mixing of active species through the membrane, which causes battery performance degradation. To overcome this issue, here we report size-selective ion-exchange membranes prepared by sulfonation of a spirobifluorene-based microporous polymer and demonstrate their efficient ion sieving functions in flow batteries.
View Article and Find Full Text PDFThe mechanism and dynamics of the CO reduction reaction (CORR) remain poorly understood, which is largely caused by mass transport limitations and lack of time-correlated product analysis tools. In this work, a custom-built gas accessible membrane electrode (GAME) system is used to comparatively assess the CORR behavior of Au and Au-Cu catalysts. The platform achieves high reduction currents (∼ - 50 mA cm at 1.
View Article and Find Full Text PDFWith the rapid development of renewable energy harvesting technologies, there is a significant demand for long-duration energy storage technologies that can be deployed at grid scale. In this regard, polysulfide-air redox flow batteries demonstrated great potential. However, the crossover of polysulfide is one significant challenge.
View Article and Find Full Text PDFNitrogen-doped porous carbons containing atomically dispersed iron are prime candidates for substituting platinum-based catalysts for oxygen reduction reaction (ORR) in fuel cells. These carbon catalysts are classically synthesizedviacomplicated routes involving multiple heat-treatment steps to form the desired Fe-N sites. We herein developed a highly active FeNC catalyst comprising of exclusive Fe-N sites by a simplified solid-state synthesis protocol involving only a single heat-treatment.
View Article and Find Full Text PDFThe nature of anionic alkali metals in solution is traditionally thought to be "gaslike" and unperturbed. In contrast to this noninteracting picture, we present experimental and computational data herein that support ion pairing in alkalide solutions. Concentration dependent ionic conductivity, dielectric spectroscopy, and neutron scattering results are consistent with the presence of superalkali-alkalide ion pairs in solution, whose stability and properties have been further investigated by DFT calculations.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2020
Hybrid redox flow cells (HRFC) are key enablers for the development of reliable large-scale energy storage systems; however, their high cost, limited cycle performance, and incompatibilities associated with the commonly used carbon-based electrodes undermine HRFC's commercial viability. While this is often linked to lack of suitable electrocatalytic materials capable of coping with HRFC electrode processes, the combinatory use of nanocarbon additives and carbon paper electrodes holds new promise. Here, by coupling electrophoretically deposited nitrogen-doped graphene (N-G) with carbon electrodes, their surprisingly beneficial effects on three types of HRFCs, namely, hydrogen/vanadium (RHVFC), hydrogen/manganese (RHMnFC), and polysulfide/air (S-Air), are revealed.
View Article and Find Full Text PDFThe thin-film rotating disk electrode (TF-RDE) is a well-developed, conventional electrochemical method that is limited by poor mass transport in the dissolved phase and hence can only measure the kinetic response for Pt-based catalysts in a narrow overpotential range. Thus, the applicability of TF-RDE results in assessing how catalysts perform in fuel cells has been questioned. To address this problem, we use the floating electrode (FE) technique, which can facilitate high-mass transport to a catalyst layer composed of an ultralow loading of catalyst (1-15 μg cm) at the gas/electrolyte interface.
View Article and Find Full Text PDFThe effect of doping Cr on the electrocatalytic activity of CoP supported on carbon black (CrCoP/CB) for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline solution was investigated. A beneficial improvement in the performance of CoP toward HER and OER was discovered. For the HER at -200 mV overpotential, the turnover frequency (TOF) increases almost 6-fold from 0.
View Article and Find Full Text PDFA simple, modified Metal-Organic Chemical Deposition (MOCD) method for Pt, PtRu and PtCo nanoparticle deposition onto a variety of support materials, including C, SiC, BC, LaB, TiB, TiN and a ceramic/carbon nanofiber, is described. Pt deposition using Pt(acac) as a precursor is shown to occur a mixed solid/liquid/vapour precursor phase which results in a high Pt yield of 90-92% on the support material. Pt and Pt alloy nanoparticles range 1.
View Article and Find Full Text PDFTuning the properties of optical metamaterials in real time is one of the grand challenges of photonics. Being able to do so will enable a class of adaptive photonic materials for use in applications such as surface enhanced Raman spectroscopy and reflectors/absorbers. One strategy to achieving this goal is based on the electrovariable self-assembly and disassembly of two-dimensional nanoparticle arrays at a metal | liquid interface.
View Article and Find Full Text PDFIn the version of this Article originally published, the last sentence of the acknowledgements incorrectly read 'L.V. acknowledges the support of a Marie Skodowska-Curie fellowship (N-SHEAD)'; it should have read 'L.
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