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Journal of Energy Storage 19 (2018) 272–290

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Journal of Energy Storage 19 (2018) 272–290 Journal of Energy Storage 19 (2018) 272–290 Contents lists available at ScienceDirect Journal of Energy Storage journal homepage: www.elsevier.com/locate/est Understanding the functions of carbon in the negative active-mass of the lead–acid battery: A review of progress T ⁎ Patrick T. Moseleya, , David A.J. Randb, Alistair Davidsonc, Boris Monahovd a Ivy Cottage, Chilton, OX110RT, United Kingdom b CSIRO Energy, Melbourne, Victoria, 3169, Australia c International Lead Association, London, United Kingdom d Advanced Lead-Acid Battery Consortium, Durham, NC, USA ARTICLE INFO ABSTRACT Keywords: The addition of supplementary carbon to lead–acid batteries that are intended for use in emerging automotive Capacitance duties can provide improvement in two aspects of performance. Extra-carbon effect (i) In both hybrid electric and battery electric vehicles that are designed to preserve energy through the Functional group operation of regenerative-braking, conventional lead–acid batteries exhibit a rapid decline in the efficiency of Hydrogen evolution the recuperative charging (which can involve rates up to 30C ) and fail quickly as a result of an accumulation of Metal additives 1 lead sulfate on the negative plate. It has been widely reported that supplementary carbon — either intimately Physical effects mixed with the negative active-material or included as a separate component attached to the plate — can enhance charge-acceptance. (ii) Full-hybrid electric and battery electric vehicles employ high-voltage batteries composed of large numbers of cells connected in series. Consequently, when conventional lead–acid batteries are used in such configura- tions, the continuous cycling encountered in normal driving will almost certainly lead to divergence in the states- of-charge of the unit cells and thereby demand periodic equalization charges. In this application, it has been demonstrated that lead–acid batteries with supplementary carbon incorporated into the negative plate are rendered immune to the divergence problem and therefore operate without the need for an equalization charge. The inclusion of supplementary carbon does, however, promote hydrogen evolution and failure due to the loss of water from the electrolyte solution. Current research efforts are directed towards methods by which this disadvantage can be mitigated without losing the benefits that the addition of carbon provides. This review covers the extensive research that has been conducted to understand the mechanism by which the additional carbon operates, the additional studies that have sought to identify the best types and optimum amounts of carbon that should be used, together with the most effective manner for their deployment. 1. Recognition of extra carbon as a boost to dynamic charge- batteries varies between 1.0 and 2.5 wt.% with respect to the weight of efficiency the oxide in the paste mix. The individual additions of carbon, barium sulfate and organic material vary according to the manufacturer’s For decades, negative plates in lead–acid batteries have been pro- specifications [1]. vided with a combination of carbon, barium sulfate and an organic The benefits of including additional carbon in the negative active- additive, which is usually a wood extract, e.g., a lignosulfonate. These mass beyond the level that is normal for the ‘expander’ function were additives are collectively called an ‘expander’, although this term is first demonstrated by the work of Nakamura and Shiomi [2,3], who often used purely for the organic component of the mix. During char- made negative plates that contained up to ten times the customary level ge–discharge cycling, the expander serves to prevent individual crystals of carbon. The actual amounts were not disclosed but, based on typical of lead from growing and combining into a dense structure with a low practice, were believed to be about 2.0 wt.% of the negative active- surface-area and, therefore, a low electrical capacity. The total amount material loading. The trials, which were directed towards both electric of expander used in industrial valve-regulated lead–acid (VRLA) vehicle and photovoltaic (PV) power applications, were conducted with ⁎ Corresponding author. E-mail addresses: [email protected] (P.T. Moseley), [email protected] (D.A.J. Rand), [email protected] (A. Davidson), [email protected] (B. Monahov). https://doi.org/10.1016/j.est.2018.08.003 Received 3 July 2018; Received in revised form 2 August 2018; Accepted 2 August 2018 Available online 22 August 2018 2352-152X/ © 2018 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/BY-NC-ND/4.0/). P.T. Moseley et al. Journal of Energy Storage 19 (2018) 272–290 Nomenclature time, usually in hours) d Thickness of double-layer (m) Acronyms and initialisms used in the text e Mathematical constant = 2.71828 − e– Electron (negative charge: 1.602 × 10 19 C; mass: 9.109 −31 1BS Monobasic lead sulfate (PbO∙PbSO4) ×10 kg) 3BS Tribasic lead sulfate (3PbO∙PbSO4∙H2O) EF Fermi level energy 4B3 Tetrabasic lead sulfate (4PbO∙PbSO4) EV Energy of the valence band a.c. Alternating current EC Energy of the conduction band − AC Activated carbon F Farad (= C V 1) − AGM Absorptive glass mat F Faraday constant (= 96 485 C mol 1) ALABC Advanced Lead–Acid Battery Consortium g Gram −2 BET Brunauer–Emmett–Teller (technique for measuring spe- io Exchange-current density (A cm ) cific surface-area) I Current (A) BM Ball mill Ibat Current (A) through the parallel connection of a capacitor BP Barton pot and a charge-transfer component (a Faradaic element) BMS Battery management system IC Current (A) through a capacitor BSS Battery support system ICT Current (A) through a charge-transfer component (a CB Carbon black Faradaic element) CSIRO Commonwealth Scientific and Industrial Research J Joule (1 J = 1 W s) Organisation k Kilo (103) d.c. Direct current km Kilometer DCA Dynamic charge-acceptance kW Kilowatt DCE Dynamic charge-efficiency kWh Kilowatt–hour EAC Electrochemically active carbon K Kelvin (a measure of absolute temperature) – EES Electrical energy storage m Metre; also milli (10 3) EF Fermi level mg Milligram EG Expanded graphite min Minute FG Flake graphite ms Millisecond GO Graphene oxide m Mass (kg) – HER Hydrogen evolution reaction pm Picometre (10 12 m) HEV Hybrid electric vehicle Q Electric charge (in C= 1As) HRPSoC High-rate partial-state-of-charge R Ohmic resistance (in⟵Ω), real part of impedance LD Donor level RCT Resistance (in Ω) of a charge-transfer component (a OAN Oil Absorption Number Faradaic element) − − PSoC Partial state-of-charge R Universal gas constant (8.3145 J mole 1 K 1) − − S Siemens (= A V 1 or Ω 1) s Second SoC State-of-charge S Surface-area (m2) SoCOT Operational state-of-charge T Absolute temperature (K) VRLA Valve-regulated lead–acid (battery) U Volt (V); symbol commonly used in German forums; SI XPS X-ray photoelectron spectroscopy symbol is V V Voltage; also volume (m3) − Roman letters W Watt (1 W = 1 J s 1) Wh Watt–hour A Ampere; also real electrode surface-area (in m2) wt.% Percentage by weight – Å Angstrom (10 10 m) AC Activated carbon Greek letters Ah Ampere-hour −1 −12 −1 c Molar concentration (mol L ) ε0 Permittivity of vacuum (98.854 × 10 Fm ) cm Centimetre εr Relative permittivity of the dielectric – °C Degree Celsius μ Micro (10 6) − C Coulomb (= 1 A s) ρ Density (kg m 3) − C Capacitance (in F = AsV 1) τ Time constant (s), τ = RC fi −2 Cs Speci c-area capacitance (F cm ) ϕm Work function fi −1 Cm Speci c capacitance (F g ) ϕB0 Schottky barrier height Cdiff Ionic diffuse-layer capacitance (F) χ Electron affinity CH Helmholtz double-layer capacitance (F) Ω Ohms Csc Space charge capacitance (F) CX/t Discharge rate (X = hour rate; t = specified discharge AGM-VRLA batteries that operated under PSoC conditions to lessen has been reported [4] that the additional carbon results not only in an overcharge effects. Batteries with standard levels of carbon failed increased cycle-life but also in greater specific energy at high rates. quickly due to the build-up of lead sulfate in the negative plate. By To date, the prime aim of the work on carbon addition has been to contrast, the companion positive plate was fully-charged. Batteries with support 12-V automotive batteries in micro-HEVS with regenerative- extra carbon enjoyed appreciably longer operating lives. Recently, it braking where the shortcomings of ‘dynamic charge-acceptance’ (DCA) 273 P.T. Moseley et al. Journal of Energy Storage 19 (2018) 272–290 have emerged. The DCA is quantified as the average charging current (or charge integral) over either one or all recuperation pulses of a re- presentative PSoC micro-cycling sequence, and can be normalized to − the battery’s nominal capacity, i.e., A Ah 1. In practice, however, DCA represents the charge that is accepted by both the reduction of lead sulfate to lead and the evolution of hydrogen. Nevertheless, since it is primarily the former reaction that should be encouraged, it is the ‘dy- namic charge-efficiency’ (DCE), which represents only the PbSO4 |Pb reaction, that should be the focus of attention and quoted in terms of only those amperes (A) accepted into the lead sulfate reduction per ampere-hour (Ah) of battery capacity. Developments [5] have revealed that extra carbon enhances charge efficiency under the high-rate charging conditions that occur during the ‘stop–start’ duty of micro-HEVs. Studies conducted on higher voltage fl lead–acid batteries for medium- and full-HEVs found that the states-of- Fig. 1. Schematic of current uxes during and after a short charge event on a charge of series-connected cells with additional carbon in their negative negative plate that contains carbon [6].
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