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Stephen R. Duncan

Publications and source records attributed to Stephen R. Duncan.

17 recordsLinked to original sources

Multisine electrochemical impedance spectroscopy for Li-ion battery characterisation

Electrochemical impedance spectroscopy (EIS) is a valuable tool for non-invasive battery characterisation, providing a compact representation of physical processes over a wide range of time scales. Commonly, sinusoids at different frequencies are injected sequentially (single-sines). Alternatively, a multisine excitation (a sum of sines) is advantageous for reducing experiment time and allowing impedance to be measured during operation. In this work, we demonstrate high-fidelity multisine EIS measurements on Li-ion cells over a wide frequency range (20 mHz to 1 kHz), taken with a commercial potentiostat modified to give access to the underlying current and voltage time-series data, and compare these to single-sine EIS. We show how this allows the conditions of linearity and stationarity to be verified directly, which is not possible with impedance data alone. We then measure broadband impedance during charging and discharging, temperature change, and relaxation. Because impedance is a linearisation of the response about an operating point, each of these conditions probes a state that classical EIS excludes by definition: kinetics linearised about a non-zero current, thermally activated reaction rates, and relaxing concentration gradients, respectively. Operando multisine EIS is therefore not simply a faster measurement approach, but one that resolves behaviour that steady-state EIS cannot.

eess.SY

Opportunities for real-time process control of electrode properties in lithium-ion battery manufacturing

Lithium-ion batteries (LIBs) have an important role in the shift required to achieve a global net-zero carbon target of 2050. Electrode manufacture is amongst the most expensive steps of the LIB manufacturing process and, despite its apparent maturity, optimised manufacturing conditions are arrived at by largely trial and error. Currently, LIB manufacturing plants are controlled to follow the fixed "recipe" obtained by trial and error, which may nonetheless be suboptimal. Moreover, regulating the process as a whole to conform to the set conditions is not widespread. Inspired by control approaches used in other film and sheet processes, we discuss opportunities for implementing real-time process control of electrode-related products, which has the potential to reduce the electrode manufacturing cost, CO2 emissions, usage of resources by increases in process yield, and throughput. We highlight the challenges and significant opportunities of implementing real-time process control in LIB electrode production lines.

eess.SY

Physics-based battery model parametrisation from impedance data

Non-invasive parametrisation of physics-based battery models can be performed by fitting the model to electrochemical impedance spectroscopy (EIS) data containing features related to the different physical processes. However, this requires an impedance model to be derived, which may be complex to obtain analytically. We have developed the open-source software PyBaMM-EIS that provides a fast method to compute the impedance of any PyBaMM model at any operating point using automatic differentiation. Using PyBaMM-EIS, we investigate the impedance of the single particle model, single particle model with electrolyte (SPMe), and Doyle-Fuller-Newman model, and identify the SPMe as a parsimonious option that shows the typical features of measured lithium-ion cell impedance data. We provide a grouped parameter SPMe and analyse the features in the impedance related to each parameter. Using the open-source software PyBOP, we estimate 18 grouped parameters both from simulated impedance data and from measured impedance data from a LG M50LT lithium-ion battery. The parameters that directly affect the response of the SPMe can be accurately determined and assigned to the correct electrode. Crucially, parameter fitting must be done simultaneously to data across a wide range of states-of-charge. Overall, this work presents a practical way to find the parameters of physics-based models.

eess.SY

Graded lithium-ion battery pouch cells to homogenise current distributions and mitigate lithium plating

Spatial distributions in current, temperature, state-of-charge and degradation across the plane of large format lithium-ion battery pouch cells can significantly impact their performance, especially at high C-rates. In this paper, a method to smooth out these spatial distributions by grading the electrode microstructure in-the-plane is proposed. A mathematical model of a large format pouch cell is developed and validated against both temperature and voltage experimental data. An analytical solution for the optimal graded electrode that achieves a uniform current distribution across the pouch cell is then derived. The model predicts that the graded electrodes could significantly reduce the likelihood of lithium plating in large format pouch cells, with grading increasing the C-rate at which plating occurs from 2.4C to 4.3C. These results indicate the potential of designing spatially varying electrode architectures to homogenise the response of large format pouch cells and improve their high rate performance.

cond-mat.mtrl-sci

A Higher-Order Generalized Singular Value Decomposition for Rank Deficient Matrices

The higher-order generalized singular value decomposition (HO-GSVD) is a matrix factorization technique that extends the GSVD to $N \ge 2$ data matrices, and can be used to identify shared subspaces in multiple large-scale datasets with different row dimensions. The standard HO-GSVD factors $N$ matrices $A_i\in\mathbb{R}^{m_i\times n}$ as $A_i=U_iΣ_i V^\text{T}$, but requires that each of the matrices $A_i$ has full column rank. We propose a modification of the HO-GSVD that extends its applicability to rank-deficient data matrices $A_i$. If the matrix of stacked $A_i$ has full rank, we show that the properties of the original HO-GSVD extend to our approach. We extend the notion of common subspaces to isolated subspaces, which identify features that are unique to one $A_i$. We also extend our results to the higher-order cosine-sine decomposition (HO-CSD), which is closely related to the HO-GSVD. Our extension of the standard HO-GSVD allows its application to datasets with with $m_i<n$ or $\text{rank}(A_i)<n$, such as are encountered in bioinformatics, neuroscience, control theory or classification problems.

math.NA

Bounding the difference between model predictive control and neural networks

There is a growing debate on whether the future of feedback control systems will be dominated by data-driven or model-driven approaches. Each of these two approaches has their own complimentary set of advantages and disadvantages, however, only limited attempts have, so far, been developed to bridge the gap between them. To address this issue, this paper introduces a method to bound the worst-case error between feedback control policies based upon model predictive control (MPC) and neural networks (NNs). This result is leveraged into an approach to automatically synthesize MPC policies minimising the worst-case error with respect to a NN. Numerical examples highlight the application of the bounds, with the goal of the paper being to encourage a more quantitative understanding of the relationship between data-driven and model-driven control.

eess.SY

Reduced-Order Neural Network Synthesis with Robustness Guarantees

In the wake of the explosive growth in smartphones and cyberphysical systems, there has been an accelerating shift in how data is generated away from centralised data towards on-device generated data. In response, machine learning algorithms are being adapted to run locally on board, potentially hardware limited, devices to improve user privacy, reduce latency and be more energy efficient. However, our understanding of how these device orientated algorithms behave and should be trained is still fairly limited. To address this issue, a method to automatically synthesize reduced-order neural networks (having fewer neurons) approximating the input/output mapping of a larger one is introduced. The reduced-order neural network's weights and biases are generated from a convex semi-definite programme that minimises the worst-case approximation error with respect to the larger network. Worst-case bounds for this approximation error are obtained and the approach can be applied to a wide variety of neural networks architectures. What differentiates the proposed approach to existing methods for generating small neural networks, e.g. pruning, is the inclusion of the worst-case approximation error directly within the training cost function, which should add robustness. Numerical examples highlight the potential of the proposed approach. The overriding goal of this paper is to generalise recent results in the robustness analysis of neural networks to a robust synthesis problem for their weights and biases.

cs.LG

Regional Stability Analysis of Transitional Fluid Flows

A method to bound the maximum energy perturbation for which regional stability of transitional fluid flow models can be guaranteed is introduced. The proposed method exploits the fact that the fluid model's nonlinearities are both lossless and locally bounded and uses the axes lengths of the ellipsoids for the trajectory set containment as variables in the stability conditions. Compared to existing approaches, the proposed method leads to an average increase in the maximum allowable energy perturbation of 29% for the Waleffe-KimHamilton (WKH) shear flow model and of 38% for the 9-state reduced model of Couette flow.

physics.flu-dyn

Model Predictive Control for Electron Beam Stabilization in a Synchrotron

Electron beam stabilization in a synchrotron is a disturbance rejection problem, with hundreds of inputs and outputs, that is sampled at frequencies higher than $10$ kHz. In this feasibility study, we focus on the practical issues of an efficient implementation of model predictive control (MPC) for the heavily ill-conditioned plant of the electron beam stabilization problem. To obtain a tractable control problem that can be solved using only a few iterations of the fast gradient method, we investigate different methods for preconditioning the resulting optimization problem and relate our findings to standard regularization techniques from cross-directional control. We summarize the single- and multi-core implementations of our control algorithm on a digital signal processor (DSP), and show that MPC can be executed at the rate required for synchrotron control. MPC overcomes various problems of standard electron beam stabilization techniques, and the successful implementation can increase the stability of photon beams in synchrotron light sources.

eess.SY

Robust error bounds for quantised and pruned neural networks

With the rise of smartphones and the internet-of-things, data is increasingly getting generated at the edge on local, personal devices. For privacy, latency and energy saving reasons, this shift is causing machine learning algorithms to move towards decentralisation with the data and algorithms stored, and even trained, locally on devices. The device hardware becomes the main bottleneck for model capability in this set-up, creating a need for slimmed down, more efficient neural networks. Neural network pruning and quantisation are two methods that have been developed for this, with both approaches demonstrating impressive results in reducing the computational cost without sacrificing significantly on model performance. However, the understanding behind these reduction methods remains underdeveloped. To address this issue, a semi-definite program is introduced to bound the worst-case error caused by pruning or quantising a neural network. The method can be applied to many neural network structures and nonlinear activation functions with the bounds holding robustly for all inputs in specified sets. It is hoped that the computed bounds will provide certainty to the performance of these algorithms when deployed on safety-critical systems.

cs.LG

Structural Identifiability of a Pseudo-2D Li-ion Battery Electrochemical Model

Growing demand for fast charging and optimised battery designs is fuelling significant interest in electrochemical models of Li-ion batteries. However, estimating parameter values for these models remains a major challenge. In this paper, a structural identifiability analysis was applied to a pseudo-2D Li-ion electrochemical battery model that can be considered as a linearised and decoupled form of the benchmark Doyle-Fuller-Newman model. From an inspection of the impedance function, it was shown that this model is uniquely parametrised by 21 parameters, being combinations of the electrochemical parameters like the conductivities and diffusion coefficients. The well-posedness of the parameter estimation problem with these parameters was then established. This result could lead to more realistic predictions about the internal state of the battery by identifying the parameter set that can be uniquely identified from the data.

eess.SY

Multi-Array Electron Beam Stabilization using Block-Circulant Transformation and Generalized Singular Value Decomposition

We introduce a novel structured controller design for the electron beam stabilization problem of the UK's national synchrotron light source. Because changes to the synchrotron will not allow the application of existing control approaches, we develop a novel method to diagonalize the multi-input multi-output (MIMO) system. A generalized singular value decomposition (GSVD) is used to simultaneously diagonalize the actuator response matrices, which is applicable to an arbitrary number of actuator dynamics in a cross-directional setting. The resulting decoupled systems are regulated using mid-ranged control and the controller gains derived as a function of the generalized singular values. In addition, we exploit the inherent block-circulant symmetry of the system. The performance of our controller is demonstrated using simulations that involve machine data.

eess.SY

Symmetry Exploitation in Orbit Feedback Systems of Synchrotron Storage Rings

Structural symmetries in the storage ring of synchrotrons are intentionally created during the design phase of the magnetic lattices, but they are not considered in the design of control algorithms that stabilize the beam of accelerated particles. The choice of control algorithm, however, is limited by the speed requirements of the synchrotron. Standard control algorithms for synchrotrons are based on a singular value decomposition (SVD) of the orbit response matrix. SVD controllers neither exploit the structural symmetries nor exhibit any speed advantages. Based on the periodicity and the reflection properties of the betatron function, we show that these structural symmetries are inherited by the orbit response matrix. We show that the resulting block-circulant and centrosymmetric properties of the matrix can be used for different computationally efficient decompositions of the controller. We also address the case of broken symmetry due to odd placements of magnets and monitors. Our efficient decomposition could enable the use of more advanced control techniques for synchrotrons, such as control algorithms that require real-time optimization. These advanced control techniques could in turn increase the quality of research in synchrotron light sources.

physics.acc-ph

Identifiability and parameter estimation of the single particle lithium-ion battery model

This paper investigates the identifiability and estimation of the parameters of the single particle model (SPM) for lithium-ion battery simulation. Identifiability is addressed both in principle and in practice. The approach begins by grouping parameters and partially non-dimensionalising the SPM to determine the maximum expected degrees of freedom in the problem. We discover that, excluding open circuit voltage, there are only six independent parameters. We then examine the structural identifiability by considering whether the transfer function of the linearised SPM is unique. It is found that the model is unique provided that the electrode open circuit voltage functions have a known non-zero gradient, the parameters are ordered, and the electrode kinetics are lumped into a single charge transfer resistance parameter. We then demonstrate the practical estimation of model parameters from measured frequency-domain experimental electrochemical impedance spectroscopy (EIS) data, and show additionally that the parametrised model provides good predictive capabilities in the time domain, exhibiting a maximum voltage error of 20 mV between model and experiment over a 10 minute dynamic discharge.

eess.SY

Circuit Synthesis of Electrochemical Supercapacitor Models

This paper is concerned with the synthesis of RC electrical circuits from physics-based supercapacitor models describing conservation and diffusion relationships. The proposed synthesis procedure uses model discretisation, linearisation, balanced model order reduction and passive network synthesis to form the circuits. Circuits with different topologies are synthesized from several physical models. This work will give greater understanding to the physical interpretation of electrical circuits and will enable the development of more generalised circuits, since the synthesized impedance functions are generated by considering the physics, not from experimental fitting which may ignore certain dynamics.

eess.SY

Observability analysis and state estimation of lithium-ion batteries in the presence of sensor biases

This paper investigates the observability of one of the most commonly used equivalent circuit models (ECMs) for lithium-ion batteries and presents a method to estimate the state of charge (SOC) in the presence of sensor biases, highlighting the importance of observability analysis for choosing appropriate state estimation algorithms. Using a differential geometric approach, necessary and sufficient conditions for the nonlinear ECM to be observable are derived and are shown to be different from the conditions for the observability of the linearised model. It is then demonstrated that biases in the measurements, due to sensor ageing or calibration errors, can be estimated by applying a nonlinear Kalman filter to an augmented model where the biases are incorporated into the state vector. Experiments are carried out on a lithium-ion pouch cell and three types of nonlinear filters, the first-order extended Kalman filter (EKF), the second-order EKF and the unscented Kalman filter (UKF) are applied using experimental data. The different performances of the filters are explained from the point of view of observability.

eess.SY

Low-Order Mathematical Modelling of Electric Double Layer Supercapacitors Using Spectral Methods

This work investigates two physics-based models that simulate the non-linear partial differential algebraic equations describing an electric double layer supercapacitor. In one model the linear dependence between electrolyte concentration and conductivity is accounted for, while in the other model it is not. A spectral element method is used to discretise the model equations and it is found that the error convergence rate with respect to the number of elements is faster compared to a finite difference method. The increased accuracy of the spectral element approach means that, for a similar level of solution accuracy, the model simulation computing time is approximately 50% of that of the finite difference method. This suggests that the spectral element model could be used for control and state estimation purposes. For a typical supercapacitor charging profile, the numerical solutions from both models closely match experimental voltage and current data. However, when the electrolyte is dilute or where there is a long charging time, a noticeable difference between the numerical solutions of the two models is observed. Electrical impedance spectroscopy simulations show that the capacitance of the two models rapidly decreases when the frequency of the perturbation current exceeds an upper threshold.

eess.SY