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With the increasing focus on decarbonisation of the transport sector, it is imperative to consider routes to electrify vehicles beyond those achievable using lithium-ion battery technology. These include heavy goods vehicles and aerospace applications that require propulsion systems that can provide gravimetric energy densities, which are more likely to be delivered by fuel cell systems. While the discussion of light-duty vehicles is abundant in the literature, heavy goods vehicles are under-represented. This paper presents an overview of the electrochemical degradation of a proton exchange membrane fuel cell integrated into a simulated Class 8 heavy goods range-extender fuel cell hybrid electric vehicle operating in urban driving conditions. Electrochemical degradation data such as polarisation curves, cyclic voltammetry values, linear sweep voltammetry values, and electrochemical impedance spectroscopy values were collected and analysed to understand the expected degradation modes in this application. In this application, the proton exchange membrane fuel cell stack power was designed to remain constant to fulfil the mission requirements, with dynamic and peak power demands managed by lithium-ion batteries, which were incorporated into the hybridised powertrain. A single fuel cell or battery cell can either be operated at maximum or nominal power demand, allowing four operational scenarios: maximum fuel cell maximum battery, maximum fuel cell nominal battery, nominal fuel cell maximum battery, and nominal fuel cell nominal battery. Operating scenarios with maximum fuel cell operating power experienced more severe degradation after endurance testing than nominal operating power. A comparison of electrochemical degradation between these operating scenarios was analysed and discussed. By exploring the degradation effects in proton exchange membrane fuel cells, this paper offers insights that will be useful in improving the long-term performance and durability of proton exchange membrane fuel cells in heavy-duty vehicle applications and the design of hybridised powertrains. [ABSTRACT FROM AUTHOR]

Although proton exchange membranes (PEMs) are widely deployed in an array of commercial applications, limitations linked to their proton conductivity, water retention, and gas permeability still limit ultimate device performance. While ex situ studies have shown additives can enhance membrane stability and mass transport, to date few have demonstrated that these performance enhancements are maintained when tested in commercially relevant electrochemical technologies, such as fuel cells or electrolyzers. Herein, a new multifunctional additive, 2D poly(triazine imide) (PTI), is demonstrated for composite PEMs, which is shown to boost proton conductivity by 37% under optimal high relative humidity (RH) conditions and 67% at low RHs. PTI also enables major improvements (over 55%) in both current and power densities in industrially relevant PEM fuel cells (PEMFCs). Most importantly, in situ and ex situ characterization suggests that the enhanced performance is due to polymer aggregate‐PTI clusters that form with increasing 2D character and improved long‐range connectivity, while acid‐base interactions with pyridinic nitrogen facilitate the critical proton hopping mechanism at all RHs. Hence, this work offers both a new membrane concept with proven benefits for important electrochemical technologies, as well as design principles for future optimization of proton transport and water management within PEMs. [ABSTRACT FROM AUTHOR]

Automotive drive cycles have existed since the 1960s. They started as requirements as being solely used for emissions testing. During the past decade, they became popular with scientists and researchers in the testing of electrochemical vehicles and power devices. They help simulate realistic driving scenarios anywhere from system to component-level design. This paper aims to discuss the complete history of these drive cycles and their validity when used in an electrochemical propulsion scenario, namely with the use of proton exchange membrane fuel cells (PEMFC) and lithium-ion batteries. The differences between two categories of drive cycles, modal and transient, were compared; and further discussion was provided on why electrochemical vehicles need to be designed and engineered with transient drive cycles instead of modal. Road-going passenger vehicles are the main focus of this piece. Similarities and differences between aviation and marine drive cycles are briefly mentioned and compared and contrasted with road cycles. The construction of drive cycles and how they can be transformed into a 'power cycle' for electrochemical device sizing purposes for electrochemical vehicles are outlined; in addition, how one can use power cycles to size electrochemical vehicles of various vehicle architectures are suggested, with detailed explanations and comparisons of these architectures. A concern with using conventional drive cycles for electrochemical vehicles is that these types of vehicles behave differently compared to combustion-powered vehicles, due to the use of electrical motors rather than internal combustion engines, causing different vehicle behaviours and dynamics. The challenges, concerns, and validity of utilising 'general use' drive cycles for electrochemical purposes are discussed and critiqued. [ABSTRACT FROM AUTHOR]

Fuel cell based micro-combined heat and power (CHP) units used for domestic applications can provide significant cost and environmental benefits for end users and contribute to the UK’s 2050 emissions target by reducing primary energy consumption in dwellings. Lately there has been increased interest in the development of systematic methods for the design of such systems and their smoother integration with domestic building services. Several models in the literature, whether they use a simulation or an optimisation approach, ignore the dwelling side of the system and optimise the efficiency or delivered power of the unit. However the design of the building services is linked to the choice of heating plant and its characteristics. Adding the dwelling’s energy demand and temperature constraints in a model can produce more general results that can optimise the whole system, not only the micro-CHP unit. The fuel cell has various heat streams that can be harvested to satisfy heat demand in a dwelling and the design can vary depending on the proportion of heat needed from each heat stream to serve the energy demand. A mixed integer non-linear programming model (MINLP) that can handle multiple heat sources and demands is presented in this paper. The methodology utilises a process systems engineering approach. The model can provide a design that integrates the temperature and water flow constraints of a dwelling’s heating system with the heat streams within the fuel cell processes while optimising total CO 2 emissions. The model is demonstrated through different case studies that attempt to capture the variability of the housing stock. The predicted CO 2 emissions reduction compared to a conventionally designed building vary from 27% to 30% and the optimum capacity of the fuel cell ranges between 1.9 kW and 3.6 kW. This research represents a significant step towards an integrated fuel cell micro-CHP and dwelling design. [ABSTRACT FROM AUTHOR]

Hybrid fuel cell battery electric vehicles require complex energy management systems (EMS) in order to operate effectively. Poor EMS can result in a hybrid system that has low efficiency and a high rate of degradation of the fuel cell and battery pack. Many different types of EMS have been reported in the literature, such as equivalent consumption minimisation strategy and fuzzy logic controllers, which typically focus on a single objective optimisations, such as minimisation of H 2 usage. Different vehicle and system specifications make the comparison of EMSs difficult and can often lead to misleading claims about system performance. This paper aims to compare different EMSs, against a range of performance metrics such as charge sustaining ability and fuel cell degradation, using a common modelling framework developed in MATLAB/Simulink - the Electric Vehicle Simulation tool-Kit (EV-SimKit). A novel fuzzy logic controller is also presented which mutates the output membership function depending on fuel cell degradation to prolong fuel cell lifetime – the Mutative Fuzzy Logic Controller (MFLC). It was found that while certain EMSs may perform well at reducing H 2 consumption, this may have a significant impact on fuel cell degradation, dramatically reducing the fuel cell lifetime. How the behaviour of common EMS results in fuel cell degradation is also explored. Finally, by mutating the fuzzy logic membership functions, the MFLC was predicted to extend fuel cell lifetime by up to 32.8%. [Display omitted] • Comparison of energy management systems for hybrid fuel cell/battery vehicles. • Mutative Fuzzy Logic Controller prolongs fuel cell lifetime. • Reducing H2 consumption can degrade performance. [ABSTRACT FROM AUTHOR]

Fuel cells offer many benefits for residential micro-cogeneration because of their high electrical efficiency, low emissions, and low heat-to-power ratio. However, the current design of fuel cell micro combined heat and power (CHP) systems for dwellings can be improved by better matching of the heat generated by the plant with the dwelling’s load profile and heat emitters. This paper explores the design options in building services using fuel cell micro-CHP and aims to bring the two research fields together in order to design superior integrated systems. Therefore a review of current literature on the field is performed and current available options for heat recovery from fuel cells, including the grades of heat available from different fuel cell process units are discussed. This is discussed in relation to the heat demand in a dwelling and the required temperature of the most suitable heat emitters for building services design. The paper motivates a methodology that considers all possible interconnections of plant in the design of fuel cell micro-CHP in dwellings and provides an example of how multi-objective optimisation can be used to identify promising system designs. [ABSTRACT FROM AUTHOR]

Electrochemical clean energy conversion and the production of sustainable chemicals are critical in the journey to realizing a truly sustainable society. To progress electrochemical storage and conversion devices to commercialization, improving the electrocatalyst performance and cost are of utmost importance. Research into dual‐metal atom catalysts (DACs) is rising in prominence due to the advantages of these sites over single‐metal atom catalysts (SACs), such as breaking scaling relationships for the adsorption energy of reaction intermediates and synergistic effects. This review provides an examination of the fundamental theoretical principles and experimental electrochemical performance of DACs in idealized half cells, as well as fuel cells, before proceeding to analyze the methods used for producing and identifying DACs. Current challenges and potential future research directions of DACs are also discussed. [ABSTRACT FROM AUTHOR]

Atomically dispersed transition metal‐nitrogen‐carbon catalysts are emerging as low‐cost electrocatalysts for the oxygen reduction reaction in fuel cells. However, a cost‐effective and scalable synthesis strategy for these catalysts is still required, as well as a greater understanding of their mechanisms. Herein, iron, nitrogen co‐doped carbon spheres (Fe@NCS) have been prepared via hydrothermal carbonization and high‐temperature post carbonization. It is determined that FeN4 is the main form of iron existing in the obtained Fe@NCS. Two different precursors containing Fe2+ and Fe3+ are compared. Both chemical and structural differences have been observed in catalysts starting from Fe2+ and Fe3+ precursors. Fe2+@NCS‐A (starting with Fe2+ precursor) shows better catalytic activity for the oxygen reduction reaction. This catalyst is studied in an anion exchange membrane fuel cell. The high open‐circuit voltage demonstrates the potential approach for developing high‐performance, low‐cost fuel cell catalysts. [ABSTRACT FROM AUTHOR]

Polymer electrolyte fuel cells (PEFCs) are a promising replacement for the fossil fuel–dependent automotive and energy sectors. They have become increasingly commercialized in the last decade; however, significant limitations on durability and performance limit their commercial uptake. Catalyst layer (CL) design is commonly reported to impact device power density and durability; although, a consensus is rarely reached due to differences in testing conditions, experimental design, and types of data reported. This is further exacerbated by aspects of CL design such as catalyst support, proton conduction, catalyst, fabrication, and morphology, being significantly interdependent; hence, a wider appreciation is required in order to optimize performance, improve durability, and reduce costs. Here, the cutting‐edge research within the field of PEFCs is reviewed, investigating the effect of different manufacturing techniques, electrolyte distribution, support materials, surface chemistries, and total porosity on power density and durability. These are critically appraised from an applied perspective to inform the most relevant and promising pathways to make and test commercially viable cells. This holistic view of the competing aspects of CL design and preparation will facilitate the development of optimized CLs, especially the incorporation of novel catalyst support materials. [ABSTRACT FROM AUTHOR]

The development of non‐Pt hydrogen oxidation reaction catalysts for hydrogen‐fuelled polymer electrolyte fuel cells allows for an overall reduction in electrode Pt content and therefore helps reduce the cost of devices, one of the biggest commercial challenges. Herein, a novel ternary alloy catalyst supported on carbon, PdIrAu/C, has been synthesised, characterised and compared to the binary PdIr/C to show how the addition of Au improves the stability of the catalyst. Transmission electron microscopy was utilised to analyse electrode structure as a function of the synthesis method, showing the optimum annealing temperature, of those tested, to be 400 °C, while inductively‐coupled plasma mass spectrometry provided analysis of the degradation of the two catalysts, confirming the PdIrAu/C catalyst is more stable at potentials similar to those at a fuel cell anode than PdIr/C. [ABSTRACT FROM AUTHOR]

The development of alternative electrocatalysts exhibiting high activity in the oxygen reduction reaction (ORR) is vital for the deployment of large‐scale clean energy devices, such as fuel cells and zinc–air batteries. N‐doped carbon materials offer a promising platform for the design and synthesis of electrocatalysts due to their high ORR activity, high surface area, and tunable porosity. In this study, materials in which MnO nanoparticles are entrapped in N‐doped mesoporous carbon (MnO/NC) were developed as electrocatalysts for the ORR, and their performances were evaluated in zinc–air batteries. The obtained carbon materials had large surface area and high electrocatalytic activity toward the ORR. The carbon compounds were fabricated by using NaCl as template in a one‐pot process, which significantly simplifies the procedure for preparing mesoporous carbon materials and in turn reduces the total cost. A primary zinc–air battery based on this material exhibits an open‐circuit voltage of 1.49 V, which is higher than that of conventional zinc–air batteries with Pt/C (Pt/C cell) as ORR catalyst (1.41 V). The assembled zinc–air battery delivered a peak power density of 168 mW cm−2 at a current density of about 200 mA cm−2, which is higher than that of an equivalent Pt/C cell (151 mW cm−2 at a current density of ca. 200 mA cm−2). The electrocatalytic data revealed that MnO/NC is a promising nonprecious‐metal ORR catalyst for practical applications in metal–air batteries. Composite electrocatalysts: Materials in which MnO nanoparticles are entrapped in N‐doped mesoporous carbon (MnO/NC) were developed as electrocatalysts for the oxygen evolution reaction, and their performance was evaluated in a zinc–air battery (see figure), which delivered a peak power density of 168 mW cm−2 at a current density of about 200 mA cm−2, which is higher than that of an equivalent Pt/C cell (151 mW cm−2 at a current density of ca. 200 mA cm−2). [ABSTRACT FROM AUTHOR]

Network-like metallic alloys of solid nanoparticles have been frequently reported as promising electrocatalysts for fuel cells. The three-dimensional structure of such networks is rich in pores in the form of voids between nanoparticles, which collectively expose a large surface area for catalytic activity. Herein, we present a novel solution to this problem using a precursor comprising a flocculent core-shell PtNi@Ni to produce PtNi network catalysts with nanoparticle intraporosity after carefully controlled electrochemical dealloying. Physical characterization shows a hierarchical level of nanoporosity (intrapores within nanoparticles and pores between them) evolves during the controlled electrochemical dealloying, and that a Pt-rich surface also forms after 22 cycles of Ni leaching. In ORR cycling, the PtNi networks gain 4-fold activity in both j ECSA and j mass over a state of the art Pt/C electrocatalyst, and also significantly exceed previously reported PtNi networks. In ORR degradation tests, the PtNi networks also proved stable, dropping by 30.4% and 62.6% in j ECSA and j mass respectively. The enhanced performance of the catalyst is evident, and we also propose that the presented synthesis procedure can be generally applied to developing other metallic networks. [ABSTRACT FROM AUTHOR]

The redox properties of gadolinium doped ceria (CGO) and nickel oxide (NiO) composite cermets underpin the operation of solid oxide electrochemical cells. Although these systems have been widely studied, a full comprehension of the reaction dynamics at the interface of these materials is lacking. Here, in situ Raman spectroscopic monitoring of the redox cycle is used to investigate the interplay between the dynamic and competing processes of hydrogen spillover and water dissociation on the doped ceria surface. In order to elucidate these mechanisms, the redox process in pure CGO and NiO is studied when exposed to wet and dry hydrogen and is compared to the cermet behavior. In dry hydrogen, CGO reduces relatively rapidly via a series of intermediate phases, while NiO reduces via a single‐step process. In wet reducing atmospheres, however, the oxidation state of pure CGO is initially stabilized due to the dissociation of water by reduced Ce(III) and subsequent incorporation of oxygen into the structure. In the reduction process involving the composite cermet, the close proximity of the NiO improves the efficiency and speed of the composite reduction process. Although NiO is already incorporated into working cells, these observations suggest direct routes to further improve cell performance. [ABSTRACT FROM AUTHOR]

The mechanical compression used in the construction of PEFCs improves effective current collection and gas sealing, however it results in structural deformation of the MEA, affecting reactant transport with adverse consequences for the electrochemical performance of the cell. The present study uses X-ray CT to characterise MEA under compression and determine effective properties of the porous domain. The comprehensive modelling approach couples a structural model of the MEA under compression to a multi-phase, non-isothermal electrochemical performance model. Liquid water saturation in the cathode domain that promotes mass transport losses is validated with neutron radiography. Here, the structural model considers the fuel cell stacking process at three compressions and highlights the non-uniform distribution of porosity and effective properties under non-uniform cell compression, affecting localised current distribution and water transport. An increase in compression showed a negligible effect on the performance in the activation region, the performance was marginally improved in the ohmic region and significantly affected in mass transport region, promoting cell flooding. The non-uniform compression effects are found to be important considerations for robust modelling studies as it increases the nonuniformity in localised current, temperature and flooding that would further alter the durability of the fuel cell. [Display omitted] • Coupled structural and electrochemical modelling study of PEFC compression. • X-ray CT study of the MEA to generate modelling parameters and validate structural model. • Neutron radiography to validate the electrochemical model models at variable compressions. • Effect of compression and channel/land arrangement on the cell performance. • Effect of compression on water management and thermal performance. [ABSTRACT FROM AUTHOR]

A machine-learning approach is used to segment 14 X-ray computed-tomography datasets acquired by lab-based scanning of laser-milled, high-temperature polymer electrolyte fuel cell samples mounted in a 3D-printed sample holder. Two modes of operation, one with constant current load and the other with current cycling, are explored and their impact on microstructural change is correlated with electrochemical performance degradation. Constant-current testing shows the overall quantity of phosphoric acid in the gas diffusion layers is effectively unchanged between 50 and 100 h of operation but that inter-electrode distribution becomes less uniform. Current-cycling tests reveal similar quantities of phosphoric acid but a different intra-electrode distribution. Membrane swelling appears more pronounced after current-cycling tests and in both cases, significant catalyst layer migration is observed. The present analysis provides a lab-based approach to monitoring microstructural degradation in high-temperature polymer electrolyte fuel cells and provides a more accessible and more statistically robust platform for assessing the impact of phosphoric acid mitigation strategies. • Lab-based X-ray micro-computed tomography to investigate phosphoric acid leaching. • Machine learning segmentation yields quantification of microstructural changes. • Electrochemical performance loss linked to microstructure evolution. • Redistribution of phosphoric acid depends on fuel cell operation mode. • Accelerated stress tests give more membrane swelling and less uniform Pt migration. [ABSTRACT FROM AUTHOR]

Polymer electrolyte fuel cells hold great promise for a range of applications but require advances in durability for widespread commercial uptake. Corrosion of the carbon support is one of the main degradation pathways; hence, corrosion-resilient graphene has been widely suggested as an alternative to traditional carbon black. However, the performance of bulk graphene-based electrodes is typically lower than that of commercial carbon black due to their stacking effects. This article reports a simple, scalable and non-destructive method through which the pore structure and platinum utilisation of graphene-based membrane electrode assemblies can be significantly improved. Urea is incorporated into the catalyst ink before deposition, and is then simply removed from the catalyst layer after spraying by submerging the electrode in water. This additive hinders graphene restacking and increases porosity, resulting in a significant increase in Pt utilisation and current density. This technique does not require harsh template etching and it represents a pathway to significantly improve graphene-based electrodes by introducing hierarchical porosity using scalable liquid processes. [ABSTRACT FROM AUTHOR]

Photo-electrochemical (PEC) hydrogen generation is a promising technology and alternative to photovoltaic (PV)-electrolyser combined systems. Since there are no commercially available PEC cells and very limited field trials, a computer simulation was used to assess the efficacy of the approach for different domestic applications. Three mathematical models were used to obtain a view on how PEC generated hydrogen is able to cover demands for a representative dwelling. The analysed home was grid-connected and used a fuel cell based micro-CHP (micro-combined heat and power) system. Case studies were carried out that considered four different photo-electrode technologies to capture a range of current and possible future device efficiencies. The aim for this paper was to evaluate the system performance such as efficiency, fuel consumption and CO2 reduction capability. At the device unit level, the focus was on photo-electrode technological aspects, such as the effect of band-gap energy represented by different photo-materials on productivity of hydrogen and its uncertainty caused by the incident photon-to-current conversion efficiency (IPCE), which is highly electrode preparation specific. The presented dynamic model allows analysis of the performance of a renewable energy source integrated household with variable loads, which will aid system design and decision-making. [ABSTRACT FROM AUTHOR]