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  • Journal article
    Gayon-Lombardo A, Lukas M, Brandon N, Cooper Set al., 2020,

    Pores for thought: Generative adversarial networks for stochastic reconstruction of 3D multi-phase electrode microstructures with periodic boundaries

    , npj Computational Materials, Vol: 6, Pages: 1-11, ISSN: 2057-3960

    The generation of multiphase porous electrode microstructures is a critical step in the optimisation of electrochemical energy storage devices. This work implements a deep convolutional generative adversarial network (DC-GAN) for generating realistic n-phase microstructural data. The same network architecture is successfully applied to two very different three-phase microstructures: A lithium-ion battery cathode and a solid oxide fuel cell anode. A comparison between the real and synthetic data is performed in terms of the morphological properties (volume fraction, specific surface area, triple-phase boundary) and transport properties (relative diffusivity), as well as the two-point correlation function. The results show excellent agreement between datasets and they are also visually indistinguishable. By modifying the input to the generator, we show that it is possible to generate microstructure with periodic boundaries in all three directions. This has the potential to significantly reduce the simulated volume required to be considered “representative” and therefore massively reduce the computational cost of the electrochemical simulations necessary to predict the performance of a particular microstructure during optimisation.

  • Journal article
    Tan R, Wang A, Malpass-Evans R, Williams R, Zhao EW, Liu T, Ye C, Zhou X, Darwich BP, Fan Z, Turcani L, Jackson E, Chen L, Chong SY, Li T, Jelfs KE, Cooper AI, Brandon NP, Grey CP, McKeown NB, Song Qet al., 2020,

    Hydrophilic microporous membranes for selective ion separation and flow-battery energy storage

    , Nature Materials, Vol: 19, Pages: 195-202, ISSN: 1476-1122

    Membranes with fast and selective ion transport are widely used for water purification and devices for energy conversion and storage including fuel cells, redox flow batteries and electrochemical reactors. However, it remains challenging to design cost-effective, easily processed ion-conductive membranes with well-defined pore architectures. Here, we report a new approach to designing membranes with narrow molecular-sized channels and hydrophilic functionality that enable fast transport of salt ions and high size-exclusion selectivity towards small organic molecules. These membranes, based on polymers of intrinsic microporosity containing Tröger’s base or amidoxime groups, demonstrate that exquisite control over subnanometre pore structure, the introduction of hydrophilic functional groups and thickness control all play important roles in achieving fast ion transport combined with high molecular selectivity. These membranes enable aqueous organic flow batteries with high energy efficiency and high capacity retention, suggesting their utility for a variety of energy-related devices and water purification processes.

  • Journal article
    Zhang D, Forner-Cuenca A, Taiwo OO, Yufit V, Brushett FR, Brandon NP, Gu S, Cai Qet al., 2020,

    Understanding the role of the porous electrode microstructure in redox flow battery performance using an experimentally validated 3D pore-scale lattice Boltzmann model

    , JOURNAL OF POWER SOURCES, Vol: 447, ISSN: 0378-7753
  • Journal article
    Wang Y, Banerjee A, Wehrle L, Shi Y, Brandon N, Deutschmann Oet al., 2019,

    Performance analysis of a reversible solid oxide cell system based on multi-scale hierarchical solid oxide cell modelling

    , ENERGY CONVERSION AND MANAGEMENT, Vol: 196, Pages: 484-496, ISSN: 0196-8904
  • Journal article
    Boldrin P, Brandon NP, 2019,

    Progress and outlook for solid oxide fuel cells for transportation applications

    , Nature Catalysis, Vol: 2, Pages: 571-577, ISSN: 2520-1158

    With their high temperatures and brittle ceramic components, solid oxide fuel cells (SOFCs) might not seem the obvious fit for a power source for transportation applications. However, over recent years, advances in materials and cell design have begun to mitigate these issues, leading to the advantages of SOFCs such as fuel flexibility and high efficiency being exploited in vehicles. Here, we review these advances, look at the vehicles that SOFCs have already been used in, discuss the areas that need improvement for full commercial breakthrough and the ways in which catalysis can assist with these. In particular, we identify lifetime and degradation, fuel flexibility, efficiency and power density as key aspects for SOFCs’ improvement. Expertise from the catalysis landscape, ranging from surface science and computational materials design, to improvements in reforming catalysts and reformer design, are instrumental to this goal.

  • Journal article
    Chen J, Ouyang M, Boldrin P, Liu X, Darr J, Atkinson A, Brandon NPet al., 2019,

    Fabrication and Characterisation of Nanoscale Ni-CGO Electrode from Nano-Composite Powders

    , ECS Transactions, Vol: 91, Pages: 1799-1805, ISSN: 1938-6737
  • Journal article
    Crow DJG, Balcombe P, Brandon N, Hawkes ADet al., 2019,

    Assessing the impact of future greenhouse gas emissions from natural gas production

    , Science of the Total Environment, Vol: 668, Pages: 1242-1258, ISSN: 0048-9697

    Greenhouse gases (GHGs) produced by the extraction of natural gas are an important contributor to lifecycle emissions and account for a significant fraction of anthropogenic methane emissions in the USA. The timing as well as the magnitude of these emissions matters, as the short term climate warming impact of methane is up to 120 times that of CO 2 . This study uses estimates of CO 2 and methane emissions associated with different upstream operations to build a deterministic model of GHG emissions from conventional and unconventional gas fields as a function of time. By combining these emissions with a dynamic, techno-economic model of gas supply we assess their potential impact on the value of different types of project and identify stranded resources in various carbon price scenarios. We focus in particular on the effects of different emission metrics for methane, using the global warming potential (GWP) and the global temperature potential (GTP), with both fixed 20-year and 100-year CO 2 -equivalent values and in a time-dependent way based on a target year for climate stabilisation. We report a strong time dependence of emissions over the lifecycle of a typical field, and find that bringing forward the stabilisation year dramatically increases the importance of the methane contribution to these emissions. Using a commercial database of the remaining reserves of individual projects, we use our model to quantify future emissions resulting from the extraction of current US non-associated reserves. A carbon price of at least 400 USD/tonne CO 2 is effective in reducing cumulative GHGs by 30–60%, indicating that decarbonising the upstream component of the natural gas supply chain is achievable using carbon prices similar to those needed to decarbonise the energy system as a whole. Surprisingly, for large carbon prices, the choice of emission metric does not have a significant impact on cumulative emissions.

  • Journal article
    Song B, Bertei A, Wang X, Cooper S, Ruiz-Trejo E, Chowdhury R, Podor R, Brandon Net al., 2019,

    Unveiling the mechanisms of solid-state dewetting in Solid Oxide Cells with novel 2D electrodes

    , Journal of Power Sources, Vol: 420, Pages: 124-133, ISSN: 0378-7753

    During the operation of Solid Oxide Cell (SOC) fuel electrodes, the mobility of nickel can lead to significant changes in electrode morphology, with accompanying degradation in electrochemical performance. In this work, the dewetting of nickel films supported on yttriastabilized zirconia (YSZ), hereafter called 2D cells, is studied by coupling in-situ environmentalscanning electron microscopy (E-SEM), image analysis, cellular automata simulation and electrochemical impedance spectroscopy (EIS). Analysis of experimental E-SEM images shows that Ni dewetting causes an increase in active triple phase boundary (aTPB) length up to a maximum, after which a sharp decrease in aTPB occurs due to Ni de-percolation. Thismicrostructural evolution is consistent with the EIS response, which shows a minimum in polarization resistance followed by a rapid electrochemical degradation. These results reveal that neither evaporation-condensation nor surface diffusion of Ni are the main mechanisms of dewetting at 560-800 °C. Rather, the energy barrier for pore nucleation within the dense Ni film appears to be the most important factor. This sheds light on the relevant mechanisms and interfaces that must be controlled to reduce the electrochemical degradation of SOC electrodes induced by Ni dewetting.

  • Journal article
    Trudgeon DP, Qiu K, Li X, Mallick T, Taiwo OO, Chakrabarti B, Yufit V, Brandon NP, Crevillen-Garcia D, Shah Aet al., 2019,

    Screening of effective electrolyte additives for zinc-based redox flow battery systems

    , JOURNAL OF POWER SOURCES, Vol: 412, Pages: 44-54, ISSN: 0378-7753
  • Report
    Speirs J, Balcombe P, Blomerus P, Stettler M, Brandon N, Hawkes Aet al., 2019,

    Can natural gas reduce emissions from transport?: Heavy goods vehicles and shipping

  • Conference paper
    Stevenson GR, Boldrin P, Brandon NP, 2019,

    Liquid-based synthesis of nickel- And lanthanum- co-doped strontium titanates for use as anodes in all-ceramic solid oxide fuel cell anodes

    , Pages: 1761-1770, ISSN: 1938-6737

    © The Electrochemical Society. Nickel- lanthanum- co-doped compositions of strontium titanate have been synthesized and characterized by a scaleable liquid-based synthesis that may offer an alternative to conventional solid-state synthesis. La0.52Sr0.28Ti0.94Ni0.06O3 is synthesized from soluble precursors followed by calcination in air. The materials can be made phase pure at temperatures as low as 1250°C, as highlighted by X-ray diffraction, and nickel exsolves in hydrogen in the same way as solid-state-synthesized materials. The particle size can be varied by calcination temperature and ball milling between 2 µm and 20 µm. The material is then measured electrochemically by electrochemical impedance spectroscopy and 4-point DC conductivity. A reduction in particle size from 20 µm to 9 µm results in a large improvement in impedance response measured.

  • Journal article
    Ouyang M, Bertei A, Cooper SJ, Wu Y, Liu X, Boldrin P, Kishimoto M, Wu B, Brandon NPet al., 2019,

    Design of fibre Ni/CGO anode and model interpretation

    , ECS Transactions, Vol: 91, Pages: 1721-1739, ISSN: 1938-6737

    © The Electrochemical Society. A new structure of Ni/gadolinium-doped ceria (CGO) is prepared by a highly tuneable and facile combination of electrospinning and tape-casting method. The structure consists of a network made by continuous Ni fibres and filled in with CGO matrices. When used as the anode of solid oxide fuel cell (SOFC), though it has a lower triple phase boundary (TPB) density, it exhibits better performance compared with impregnated and cermet Ni/CGO with higher nickel loading. An algorithm is developed to determine the ceria-pore double phase boundary (DPB) density with different distance from nickel phase. Using the results, the relative electrochemical reaction rate on DPB and TPB of three different electrodes are calculated and proves that fibre-matrices structure has the morphology advantage of efficiently making use of all ceria-pore DPB. The relative contribution of DPB and TPB in anode reaction of SOFC is quantified in the first time and the importance of DPB is further stressed. This work provides new inspirations in material design of SOFC/SOEC and develops a novel strategy to evaluate the performance of electrodes quantitatively.

  • Journal article
    Rubio-Garcia J, Kucernak A, Zhao D, Lei D, Fahy K, Yufit V, Brandon N, Gomez-Gonzalez Met al., 2019,

    Hydrogen/manganese hybrid redox flow battery

    , JPhys Energy, Vol: 1, ISSN: 2515-7655

    Electrochemical energy storage is a key enabling technology for further integration of renewables sources. Redox flow batteries (RFBs) are promising candidates for such applications as a result of their durability, efficiency and fast response. However, deployment of existing RFBs is hindered by the relatively high cost of the (typically vanadium-based) electrolyte. Manganese is an earth-abundant and inexpensive element that is widely used in disposable alkaline batteries. However it has hitherto been little explored for RFBs due to the instability of Mn(III) leading to precipitation of MnO2 via a disproportionation reaction. Here we show that by combining the facile hydrogen negative electrode reaction with electrolytes that suppress Mn(III) disproportionation, it is possible to construct a hydrogen/manganese hybrid RFB with high round trip energy efficiency (82%), and high power and energy density (1410 mW cm−2, 33 Wh l−1), at an estimated 70% cost reduction compared to vanadium redox flow batteries.

  • Journal article
    Pino-Muñoz CA, Chakrabarti BK, Yufit V, Brandon NPet al., 2019,

    Characterization of a regenerative hydrogen-vanadium fuel cell using an experimentally validated unit cell model

    , Journal of the Electrochemical Society, Vol: 166, Pages: A3511-A3524, ISSN: 0013-4651

    © The Author(s) 2019. A hydrogen-vanadium electrochemical system was characterized using extensive experimental tests at different current densities and flow rates of vanadium electrolyte. The maximum peak power density achieved was 2840 W m−2 along with a limiting current density of over 4200 A m−2. The cycling performance presented a stable coulombic efficiency over 51 cycles with a mean value of 99.8%, while the voltage efficiency decreased slowly over time from a value of 90.3% to 87.0%. The capacity loss was of 5.6 A s per cycle, which could be related to crossover of ionic species and liquid water. A unit cell model, previously proposed by the authors, was modified to include the effect of species crossover and used to predict the cell potential. Reasonable agreement between the model simulations and the experimental charge-discharge data was observed, with Normalized Root-Mean-Square Errors (NRMSEs) within the range of 0.8–5.3% and 2.9–19.0% for charge and discharge, respectively. Also, a good degree of accuracy was observed in the simulated trend of the polarization and power density, with NRMSEs of 3.1% and 1.0%, and 1.1% and 1.9%, for the operation at a flow rate of vanadium electrolyte of 100 and 50 mL min−1, respectively, while the voltage efficiency during the cycling test were estimated within a Root-Mean-Square Error (RMSE) of 1.9%. A study of the effect of the component properties on the cell potential was carried out by means of a model sensitivity analysis. The cell potential was sensitive to the cathodic transfer coefficient and the cathode porosity, which are directly related to the cathodic overpotential through the Butler-Volmer equation and the cathodic ohmic overpotential. It was recognized that a kinetic study for the cathodic reaction is needed to obtain more reliable kinetic parameters at practical vanadium concentrations, as well as reliable microstructural parameters of carbon electrodes.

  • Journal article
    Budinis S, Krevor S, Mac Dowell N, Brandon N, Hawkes Aet al., 2018,

    An assessment of CCS costs, barriers and potential

    , Energy Strategy Reviews, Vol: 22, Pages: 61-81, ISSN: 2211-467X

    © 2018 Elsevier Ltd Global decarbonisation scenarios include Carbon Capture and Storage (CCS) as a key technology to reduce carbon dioxide (CO2) emissions from the power and industrial sectors. However, few large scale CCS plants are operating worldwide. This mismatch between expectations and reality is caused by a series of barriers which are preventing this technology from being adopted more widely. The goal of this paper is to identify and review the barriers to CCS development, with a focus on recent cost estimates, and to assess the potential of CCS to enable access to fossil fuels without causing dangerous levels of climate change. The result of the review shows that no CCS barriers are exclusively technical, with CCS cost being the most significant hurdle in the short to medium term. In the long term, CCS is found to be very cost effective when compared with other mitigation options. Cost estimates exhibit a high range, which depends on process type, separation technology, CO2transport technique and storage site. CCS potential has been quantified by comparing the amount of fossil fuels that could be used globally with and without CCS. In modelled energy system transition pathways that limit global warming to less than 2 °C, scenarios without CCS result in 26% of fossil fuel reserves being consumed by 2050, against 37% being consumed when CCS is available. However, by 2100, the scenarios without CCS have only consumed slightly more fossil fuel reserves (33%), whereas scenarios with CCS available end up consuming 65% of reserves. It was also shown that the residual emissions from CCS facilities is the key factor limiting long term uptake, rather than cost. Overall, the results show that worldwide CCS adoption will be critical if fossil fuel reserves are to continue to be substantively accessed whilst still meeting climate targets.

  • Journal article
    Balcombe P, Speirs JF, Brandon NP, Hawkes ADet al., 2018,

    Methane emissions: choosing the right climate metric and time horizon

    , Environmental Science: Processes and Impacts, Vol: 20, Pages: 1323-1339, ISSN: 2050-7895

    Methane is a more potent greenhouse gas (GHG) than CO2, but it has a shorter atmospheric lifespan, thus its relative climate impact reduces significantly over time. Different GHGs are often conflated into a single metric to compare technologies and supply chains, such as the global warming potential (GWP). However, the use of GWP is criticised, regarding: (1) the need to select a timeframe; (2) its physical basis on radiative forcing; and (3) the fact that it measures the average forcing of a pulse over time rather than a sustained emission at a specific end-point in time. Many alternative metrics have been proposed which tackle different aspects of these limitations and this paper assesses them by their key attributes and limitations, with respect to methane emissions. A case study application of various metrics is produced and recommendations are made for the use of climate metrics for different categories of applications. Across metrics, CO2 equivalences for methane range from 4–199 gCO2eq./gCH4, although most estimates fall between 20 and 80 gCO2eq./gCH4. Therefore the selection of metric and time horizon for technology evaluations is likely to change the rank order of preference, as demonstrated herein with the use of natural gas as a shipping fuel versus alternatives. It is not advisable or conservative to use only a short time horizon, e.g. 20 years, which disregards the long-term impacts of CO2 emissions and is thus detrimental to achieving eventual climate stabilisation. Recommendations are made for the use of metrics in 3 categories of applications. Short-term emissions estimates of facilities or regions should be transparent and use a single metric and include the separated contribution from each GHG. Multi-year technology assessments should use both short and long term static metrics (e.g. GWP) to test robustness of results. Longer term energy assessments or decarbonisation pathways must use both short and long-term metrics and where this has a lar

  • Journal article
    Zhang D, Cai Q, Taiwo OO, Yufit V, Brandon NP, Gu Set al., 2018,

    The effect of wetting area in carbon paper electrode on the performance of vanadium redox flow batteries: A three-dimensional lattice Boltzmann study

    , Electrochimica Acta, Vol: 283, Pages: 1806-1819, ISSN: 0013-4686

    The vanadium redox flow battery (VRFB) has emerged as a promising technology for large-scale storage of intermittent power generated from renewable energy sources due to its advantages such as scalability, high energy efficiency and low cost. In the current study, a three-dimensional(3D) Lattice Boltzmann model is developed to simulate the transport mechanisms of electrolyte flow, species and charge in the vanadium redox flow battery at the micro pore scale. An electrochemical model using the Butler-Volmer equation is used to provide species and charge coupling at the surface of active electrode. The detailed structure of the carbon paper electrode is obtained using X-ray Computed Tomography(CT). The new model developed in the paper is able to predict the local concentration of different species, over-potential and current density profiles under charge/discharge conditions. The simulated capillary pressure as a function of electrolyte volume fraction for electrolyte wetting process in carbon paper electrode is presented. Different wet surface area of carbon paper electrode correspond to different electrolyte volume fraction in pore space of electrode. The model is then used to investigate the effect of wetting area in carbon paper electrode on the performance of vanadium redox flow battery. It is found that the electrochemical performance of positive half cell is reduced with air bubbles trapped inside the electrode.

  • Journal article
    Niania M, Podor R, Britton TB, Li C, Cooper SJ, Svetkov N, Skinner S, Kilner Jet al., 2018,

    In situ study of strontium segregation in La<inf>0.6</inf>Sr<inf>0.4</inf>Co<inf>0.2</inf>Fe<inf>0.8</inf>O<inf>3- δ</inf>in ambient atmospheres using high-temperature environmental scanning electron microscopy

    , Journal of Materials Chemistry A, Vol: 6, Pages: 14120-14135, ISSN: 2050-7496

    Samples of the solid oxide fuel cell cathode material La0.6Sr0.4Co0.2Fe0.8O3-δ(LSCF) were annealed using High-Temperature Environmental Scanning Electron Microscopy (HT-ESEM) from room temperature to 1000 °C in atmospheres of pure oxygen, pure water and ambient lab air. Image series of each heat treatment were taken where microstructural changes were observed and compared between samples. Strontium segregation rate was found to be significantly increased in the presence of pure water as compared to pure O2and ambient air. Electron backscattered diffraction (EBSD) was performed in order to assess the effect of crystal orientation on particle formation and surface sensitive chemical analysis techniques were used to determine the chemical changes at the grain surface as a result of the different heat treatments. It was shown that crystal orientation affected the nature and growth rate of strontium-based particles, however, due to the pseudo-symmetry of La0.6Sr0.4Co0.2Fe0.8O3-δ, precise crystal orientation relationships could not be determined. The chemical composition of the grain surface was found to be approximately equal under each atmosphere.

  • Journal article
    Balcombe P, Speirs J, Johnson E, Martin J, Brandon N, Hawkes Aet al., 2018,

    The carbon credentials of hydrogen gas networks and supply chains

    , Renewable and Sustainable Energy Reviews, Vol: 91, Pages: 1077-1088, ISSN: 1364-0321

    Projections of decarbonisation pathways have typically involved reducing dependence on natural gas grids via greater electrification of heat using heat pumps or even electric heaters. However, many technical, economic and consumer barriers to electrification of heat persist. The gas network holds value in relation to flexibility of operation, requiring simpler control and enabling less expensive storage. There may be value in retaining and repurposing gas infrastructure where there are feasible routes to decarbonisation. This study quantifies and analyses the decarbonisation potential associated with the conversion of gas grids to deliver hydrogen, focusing on supply chains. Routes to produce hydrogen for gas grids are categorised as: reforming natural gas with (or without) carbon capture and storage (CCS); gasification of coal with (or without) CCS; gasification of biomass with (or without) CCS; electrolysis using low carbon electricity. The overall range of greenhouse gas emissions across routes is extremely large, from − 371 to 642 gCO 2 eq/kW h H2 . Therefore, when including supply chain emissions, hydrogen can have a range of carbon intensities and cannot be assumed to be low carbon. Emissions estimates for natural gas reforming with CCS lie in the range of 23–150 g/kW h H2 , with CCS typically reducing CO 2 emissions by 75%. Hydrogen from electrolysis ranges from 24 to 178 gCO 2 eq/kW h H2 for renewable electricity sources, where wind electricity results in the lowest CO 2 emissions. Solar PV electricity typically exhibits higher emissions and varies significantly by geographical region. The emissions from upstream supply chains is a major contributor to total emissions and varies considerably across different routes to hydrogen. Biomass gasification is characterised by very large negative emissions in the supply chain and very large positive emissions in the gasification process. Therefore, improvements in total emissions are large if even small i

  • Journal article
    Speirs JF, balcombe P, johnson E, martin J, brandon N, hawkes Aet al., 2018,

    A Greener Gas Grid: What Are the Options?

    , Energy Policy, Vol: 118, Pages: 291-297, ISSN: 0301-4215

    There is an ongoing debate over future decarbonisation of gas networks using biomethane, and increasingly hydrogen, in gas network infrastructure. Some emerging research presents gas network decarbonisation options as a tractable alternative to ‘all-electric’ scenarios that use electric appliances to deliver the traditional gas services such as heating and cooking. However, there is some uncertainty as to the technical feasibility, cost and carbon emissions of gas network decarbonisation options. In response to this debate the Sustainable Gas Institute at Imperial College London has conducted a rigorous systematic review of the evidence surrounding gas network decarbonisation options. The study focuses on the technologies used to generate biomethane and hydrogen, and examines the technical potentials, economic costs and emissions associated with the full supply chains involved. The following summarises the main findings of this research. The report concludes that there are a number of options that could significantly decarbonise the gas network, and doing so would provide energy system flexibility utilising existing assets. However, these options will be more expensive than the existing gas system, and the GHG intensity of these options may vary significantly. In addition, more research is required, particularly in relation to the capabilities of existing pipework to transport hydrogen safely.

  • Journal article
    Munoz CAP, Dewage HH, Yufit V, Brandon NPet al., 2017,

    A unit cell model of a regenerative hydrogen-vanadium fuel cell

    , Journal of The Electrochemical Society, Vol: 164, Pages: F1717-F1732, ISSN: 1945-7111

    In this study, a time dependent model for a regenerative hydrogen-vanadium fuel cell is introduced. This lumped isothermal model is based on mass conservation and electrochemical kinetics, and it simulates the cell working potential considering the major ohmic resistances, a complete Butler–Volmer kinetics for the cathode overpotential and a Tafel–Volmer kinetics near mass-transport free conditions for the anode overpotential. Comparison of model simulations against experimental data was performed by using a 25 cm2 lab scale prototype operated in galvanostatic mode at different current density values (50−600Am−2). A complete Nernst equation derived from thermodynamic principles was fitted to open circuit potential data, enabling a global activity coefficient to be estimated. The model prediction of the cell potential of one single charge-discharge cycle at a current density of 400Am−2 was used to calibrate the model and a model validation was carried out against six additional data sets, which showed a reasonably good agreement between the model simulation of the cell potential and the experimental data with a Root Mean Square Error (RMSE) in the range of 0.3–6.1% and 1.3–8.8% for charge and discharge, respectively. The results for the evolution of species concentrations in the cathode and anode are presented for one data set. The proposed model permits study of the key factors that limit the performance of the system and is capable of converging to a meaningful solution relatively fast (s–min).

  • Journal article
    Téllez Lozano H, Druce J, Cooper SJ, Kilner JAet al., 2017,

    Double perovskite cathodes for proton-conducting ceramic fuel cells: are they triple mixed ionic electronic conductors?

    , Science and Technology of Advanced Materials, Vol: 18, Pages: 977-986, ISSN: 1468-6996

    Published by National Institute for Materials Science in partnership with Taylor & Francis. 18 O and 2 H diffusion has been investigated at a temperature of 300 °C in the double perovskite material PrBaCo 2 O 5+δ (PBCO) in flowing air containing 200 mbar of 2 H 2 16 O. Secondary ion mass spectrometry (SIMS) depth profiling of exchanged ceramics has shown PBCO still retains significant oxygen diffusivity (~1.3 × 10 −11 cm 2 s −1 ) at this temperature and that the presence of water ( 2 H 2 16 O), gives rise to an enhancement of the surface exchange rate over that in pure oxygen by a factor of ~3. The 2 H distribution, as inferred from the 2 H 2 16 O − SIMS signal, shows an apparent depth profile which could be interpreted as 2 H diffusion. However, examination of the 3-D distribution of the signal shows it to be nonhomogeneous and probably related to the presence of hydrated layers in the interior walls of pores and is not due to proton diffusion. This suggests that PBCO acts mainly as an oxygen ion mixed conductor when used in PCFC devices, although the presence of a small amount of protonic conductivity cannot be discounted in these materials.

  • Journal article
    Balcombe P, Brandon NP, Hawkes AD, 2017,

    Characterising the distribution of methane and carbon dioxide emissions from the natural gas supply chain

    , Journal of Cleaner Production, Vol: 172, Pages: 2019-2032, ISSN: 0959-6526

    Methane and CO2 emissions from the natural gas supply chain have been shown to vary widely butthere is little understanding about the distribution of emissions across supply chain routes,processes, regions and operational practises. This study defines the distribution of total methaneand CO2 emissions from the natural gas supply chain, identifying the contribution from each stageand quantifying the effect of key parameters on emissions. The study uses recent high-resolutionemissions measurements with estimates of parameter distributions to build a probabilistic emissionsmodel for a variety of technological supply chain scenarios. The distribution of emissions resemblesa log-log-logistic distribution for most supply chain scenarios, indicating an extremely heavy tailedskew: median estimates which represent typical facilities are modest at 18 – 24 g CO2 eq./ MJ HHV,but mean estimates which account for the heavy tail are 22 – 107 g CO2 eq./ MJ HHV. To place thesevalues into context, emissions associated with natural gas combustion (e.g. for heat) areapproximately 55 g CO2/ MJ HHV. Thus, some supply chain scenarios are major contributors to totalgreenhouse gas emissions from natural gas. For methane-only emissions, median estimates are 0.8 –2.2% of total methane production, with mean emissions of 1.6 - 5.5%. The heavy tail distribution isthe signature of the disproportionately large emitting equipment known as super-emitters, whichappear at all stages of the supply chain. The study analyses the impact of different technologicaloptions and identifies a set of best technological option (BTO) scenarios. This suggests thatemissions-minimising technology can reduce supply chain emissions significantly, with this studyestimating median emissions of 0.9% of production. However, even with the emissions-minimisingtechnologies, evidence suggests that the influence of the super-emitters remains. Therefore,emissions-minimising technology is only part of the soluti

  • Journal article
    Jing R, Wang M, Wang W, Brandon N, Li N, Chen J, Zhao Yet al., 2017,

    Economic and environmental multi-optimal design and dispatch of solid oxide fuel cell based CCHP system

    , Energy Conversion and Management, Vol: 154, Pages: 365-379, ISSN: 0196-8904

    Combined cooling, heating and power system (CCHP) is an efficient alternative for building energy supply. Meanwhile, the advantages of high energy efficiency and low emission for solid oxide fuel cells (SOFCs) make the technology a promising prime mover for CCHP systems. In this study, a SOFC based CCHP system design and operation optimization model has been developed using the Mixed Integer Non-linear Programming (MINLP) approach. The model provides two capacity sizing options of the fixed size (user specified), and the optimal sizing. In the fixed size option, four dispatch strategies are considered, namely baseload, day/night, full-load, and electrical load following. In the optimal sizing option, the installed capacity of devices and the dispatch strategy are both optimized. Moreover, multi-objective optimizations are also conducted to optimize two conflicting objectives simultaneously by the Ɛ-constraint method. The optimal results are displayed by Pareto frontiers and the most desired solutions have been identified and verified by two decision-making approaches of LINMAP and TOPSIS. To make the model applicable to real world operation, novel constraints including part-load efficiency, equipment on/off, and numbers of start constraints are applied. Finally, the proposed model is applied to a case study of a hospital in Shanghai, China considering state-of-the-art technical specifications, time-of-use energy pricing, and emission factors. The results indicate environmental advantages of SOFC based CCHP system. Moreover, the levelized cost of energy (LCOE) identified by the proposed optimal design and dispatch model would be 0.17 $/kWh, which is lower than the conventional energy system.

  • Journal article
    Trogadas P, Cho JIS, Neville TP, Marquis J, Wu B, Brett DJL, Coppens MOet al., 2017,

    A lung-inspired approach to scalable and robust fuel cell design

    , Energy and Environmental Science, Vol: 11, Pages: 136-143, ISSN: 1754-5692

    A lung-inspired approach is employed to overcome reactant homogeneity issues in polymer electrolyte fuel cells. The fractal geometry of the lung is used as the model to design flow-fields of different branching generations, resulting in uniform reactant distribution across the electrodes and minimum entropy production of the whole system. 3D printed, lung-inspired flow field based PEFCs with N = 4 generations outperform the conventional serpentine flow field designs at 50% and 75% RH, exhibiting a 20% and 30% increase in performance (at current densities higher than 0.8 A cm2) and maximum power density, respectively. In terms of pressure drop, fractal flow-fields with N = 3 and 4 generations demonstrate 75% and 50% lower values than conventional serpentine flow-field design for all RH tested, reducing the power requirements for pressurization and recirculation of the reactants. The positive effect of uniform reactant distribution is pronounced under extended current-hold measurements, where lung-inspired flow field based PEFCs with N = 4 generations exhibit the lowest voltage decay (B5 mV h1). The enhanced fuel cell performance and low pressure drop values of fractal flow field design are preserved at large scale(25 cm2), in which the excessive pressure drop of a large-scale serpentine flow field renders its use prohibitive.

  • Journal article
    Cooper SJ, Bertei A, Finegan DP, Brandon NPet al., 2017,

    Simulated impedance of diffusion in porous media

    , Electrochimica Acta, Vol: 251, Pages: 681-689, ISSN: 0013-4686

    This paper describes the use of a frequency domain, finite-difference scheme to simulate the impedance spectra of diffusion in porous microstructures. Both open and closed systems are investigated for a range of ideal geometries, as well as some randomly generated synthetic volumes and tomographically derived microstructural data. In many cases, the spectra deviate significantly from the conventional Warburg-type elements typically used to represent diffusion in equivalent circuit analysis. A key finding is that certain microstructures show multiple peaks in the complex plane, which may be misinterpreted as separate electrochemical processes in real impedance data. This is relevant to battery electrode design as the techniques for nano-scale fabrication become more widespread. This simulation tool is provided as an open-source MatLab application and is freely available online as part of the TauFactor platform.

  • Report
    Speirs J, Balcombe P, Johnson E, Martin J, Brandon N, Hawkes Aet al., 2017,

    A Greener Gas Grid: What Are the Options?

    , A greener gas grid: what are the options?
  • Conference paper
    Ouyang M, Boldrin P, Brandon NP, 2017,

    Methane Pulse Study on Nickel Impregnated Gadolinium Doped Ceria

    , 15th International Symposium on Solid Oxide Fuel Cells (SOFC), Publisher: ELECTROCHEMICAL SOC INC, Pages: 1353-1366, ISSN: 1938-5862
  • Book chapter
    Cooper SJ, brandon NP, 2017,

    Solid Oxide Fuel Cell Lifetime and Reliability

    , Solid Oxide Fuel Cell Lifetime and Reliability Critical Challenges in Fuel Cells, Editors: Ruiz-Trejo, BOLDRIN, Publisher: Academic Press, Pages: 1-15, ISBN: 9780128097243

    For its holistic approach, this book can be used both as an introduction to these issues and a reference resource for all involved in research and application of solid oxide fuel cells, especially those developing understanding in ...

  • Book chapter
    Cassidy M, Neagu D, Savaniu C, Boldrin Pet al., 2017,

    New Materials for Improved Durability and Robustness in Solid Oxide Fuel Cell

    , Solid Oxide Fuel Cell Lifetime and Reliability: Critical Challenges in Fuel Cells, Pages: 193-216, ISBN: 9780081011027

    © 2017 Elsevier Ltd. All rights reserved. This chapter provides an overview of the considerations that must be made regarding new materials development for improved durability and robustness in solid oxide fuel cells (SOFCs). A number of recent development concepts are outlined for the core cell materials of anode, electrolyte, and cathode, in particular new catalytic approaches such as catalyst impregnation and exsolution on the anode to improve redox and fuel flexibility and reduced temperature cathodes. Some of the challenges of scaling up into larger stacks are also discussed. Here the interactions of cell materials with stack materials, in particular the interconnect, are summarized, such as chromium poisoning and cell to interconnect electrical contact, both of which feature prominently in SOFC stack lifetime issues. Barriers to new materials development are outlined along with the potential for accelerated testing.

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