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  <front>
    <journal-meta />
    <article-meta>
      <title-group>
        <article-title>Quasi-Unsupervised Learning of Open Circuit Voltage Profiles for Efficiency Degradation Diagnosis in Operation</article-title>
      </title-group>
      <contrib-group>
        <contrib contrib-type="author">
          <string-name>Masahito Arima</string-name>
          <email>m-arima@mail.daiwa-can.co.jp</email>
          <xref ref-type="aff" rid="aff0">0</xref>
        </contrib>
        <contrib contrib-type="author">
          <string-name>Lei Lin</string-name>
          <xref ref-type="aff" rid="aff0">0</xref>
        </contrib>
        <contrib contrib-type="author">
          <string-name>Masahiro Fukui</string-name>
          <email>mfukui@fc.ritsumei.ac.jp</email>
          <xref ref-type="aff" rid="aff1">1</xref>
        </contrib>
        <aff id="aff0">
          <label>0</label>
          <institution>Daiwa Can Company</institution>
          ,
          <addr-line>Kanagawa</addr-line>
          ,
          <country country="JP">Japan</country>
        </aff>
        <aff id="aff1">
          <label>1</label>
          <institution>Ritsumeikan University</institution>
          ,
          <addr-line>Shiga</addr-line>
          ,
          <country country="JP">Japan</country>
        </aff>
      </contrib-group>
      <abstract>
        <p>The main focus of LIB degradation has been capacity fade so far. On the other hands, efficiency degradation was pointed out in recent years. Battery aggregation, that is expected to absorb the surplus of variable renewable energies like photovoltaic energy, would be affected in terms of economic gain decrease by efficiency degradation. Reuse LIB would be used as a component of aggregation in the future, naturally, the variety of charge-discharge efficiency might be more complex. To improve an operation efficiency of aggregation including reuse LIB, we proposed the quasiunsupervised learning of open circuit voltage profiles. This method showed good accuracy of the estimation of charge-discharge energy. From this, it is expected that this diagnosis could be contribute to an economic improvement of battery aggregation.</p>
      </abstract>
    </article-meta>
  </front>
  <body>
    <sec id="sec-1">
      <title>1 Introduction</title>
      <p>* Created this document
Transmission and Distribution Co., 2021). Naturally, it would be resulted in the loss of economic and
environmental benefits despite of renewable energy capital investment.</p>
      <p>
        One of its expected solutions is aggregated rechargeable batteries supported by IoT(Isono et al.,
2013). That is, the surplus renewable energy could be charged, and discharged later in the time of
demand dominance. Lithium-ion battery (LIB) is an important candidate and has been adopted as the
components of electric vehicles and stable energy storage systems. For lower resource demands,
lower prices and more commercially widespread of LIB, many considerations of reuse
        <xref ref-type="bibr" rid="ref1">(Ahmadi et al.,
2017)</xref>
        have been carried out. In consequence, new international standard of requirements for reuse of
LIB are under discussion as IEC 63330 aiming for issuance at the end of 2023. From this, we can
understand that a lot of aggregated rechargeable batteries consisted of reuse LIB would be popular in
the future.
1.2
      </p>
      <sec id="sec-1-1">
        <title>Research Question</title>
        <p>
          LIB has an important characteristic of performance decline depending on cycle times and storing
period (Ramadass et al., 2002)
          <xref ref-type="bibr" rid="ref1">(Schmitt et al., 2017)</xref>
          (Farmann and Sauer, 2017). It is called
degradation. A decrease of full-charge capacity is discussed as a main aspect of the degradation.
Therefore, a lot of capacity degradation diagnosis of LIB have been studied (Hou et al., 2020). On the
other hands, a decrease of charge–discharge energy efficiency called ‘efficiency degradation’ was
reported as another aspect of degradation in recent years
          <xref ref-type="bibr" rid="ref3 ref4">(Redondo-Iglesias, Venet and Pelissier,
2019)</xref>
          . It causes the increase of energy loss during LIB operation
          <xref ref-type="bibr" rid="ref2 ref4">(Arima et al., 2018)</xref>
          . Especially, it
would induce the order effect of charging in the case of aggregated multiple LIBs
          <xref ref-type="bibr" rid="ref3 ref4">(Arima, Lin and
Fukui, 2019a)</xref>
          . This can be understood in the following way. A degradation degree of each LIB differs
since it depends on the conditions of operation. In addition, aggregated batteries could include various
LIB of models, manufacturers, and reuse histories. This naturally indicates that each LIB has various
characteristic of charge–discharge efficiency. Operation of high efficiency LIB could be resulted in
low losses of energy and economic gain. How to find a highly efficient LIB would be necessary for
economic and energy saving operation of battery aggregation. Namely, an efficiency degradation
diagnosis is necessary instead of capacity.
        </p>
        <p>
          An efficiency degradation diagnosis has three essential parameters. That is, a value of full charge
capacity, and profiles of open circuit voltage and internal impedance
          <xref ref-type="bibr" rid="ref3 ref4">(Arima, Lin and Fukui, 2019b)</xref>
          .
A lot of cases of degradation diagnosis of full charge capacity were already reported as mentioned
above. Internal impedance could be estimated by regressive algorithms like Kalman filter (Plett,
2004). However, a profile of open circuit voltage is usually given as a premise in the case of Kalman
filter. It is difficult to estimate profiles of open circuit voltage while keeping estimation accuracies of
state of charge that is main purpose (Haus and Mercorelli, 2020). Especially, the estimation of
transitive profiles of open circuit voltage depending on degradation by this have not been reported.
Therefore, the estimation of profiles of open circuit voltage is important for an efficiency degradation
diagnosis.
        </p>
        <p>Moreover, it is desirable that the training data of efficiency degradation diagnosis is few. In this
case, the measurement data of charge–discharge cycle test for establishing LIB’s degradation models
is applicable. A large amount of training data would improve the accuracy of these models however it
would be necessary to spend many times and works of measurements. Furthermore, there would be
many models and manufacturers of aggregated LIB, therefore there would be a lot of test samples to
be measured.</p>
        <p>In consequence, the estimation of open circuit voltage profiles with few teacher data, that is,
quasi-unsupervised learning, is required. In addition, it should be carried out using data measured by a
battery management system mounted on LIB for reducing its cost.
1.3</p>
      </sec>
      <sec id="sec-1-2">
        <title>Proposal</title>
        <p>There are many reports of open circuit voltage profile measurements, and these could be roughly
divided into two groups. One group is ‘pseudo open circuit voltage (pOCV)’ (Pastor-Fernández et al.,
2019). pOCV is the method of charge–discharge in the range of full-discharge to full-charge with
lower than 10 hours rate constant current (C/10). Other is called ‘Galvanostatic intermittent titration
technique (GITT)’ (Birkl et al., 2015). GITT is the method of square waved current charge or
discharge with long time relaxation between waves. The conditions of pOCV and GITT are quite
different from battery aggregation. We propose the unsupervised learning of open circuit voltage
profiles using data of a battery management system. The contribution of this study is the adaption to
real LIB operation of profile information acquisition.
2</p>
      </sec>
    </sec>
    <sec id="sec-2">
      <title>Proposed</title>
    </sec>
    <sec id="sec-3">
      <title>Method</title>
      <p>The unsupervised learning of open circuit voltage profiles that we proposed is described as below.
2.1</p>
      <sec id="sec-3-1">
        <title>Deformative Learning of Open Circuit Voltage Profiles</title>
        <p>This method adopts the additive processing of gaussian function profiles estimated by the value of
open circuit voltage at that time. The equation of it is defined as follows.</p>
        <p>− =   + 
  =   
= ⎜
−

  ,
⎛   , ⎞</p>
        <p>⋮
⎝  , ⎠</p>
        <p>⎟ +
−  −    ,</p>
        <p>⋮</p>
        <p>≤  ≤</p>
        <p>,  ∈  +
  , can be defined as follows.</p>
        <p>charge,</p>
        <p>is the deformation amount and   are the sample values of 
estimated open circuit voltage profile and   , are the sample values of  
Where   − denotes the estimated open circuit voltage profile after transformation,</p>
        <p>is the calculated estimation error of open circuit voltage,  is the learning rate,  is a standard
deviation of gaussian function namely the index of deformation width,   ,0 is the deformation center
on the axis of state of charge   . The image of one deformation process is described in Fig.1.
was calculated from chronological data of charge–discharge cycles. Charge–discharge voltage
for each 0.01 state of
for each 0.01 state of charge,
  , =   +  
+  +    ,
(2)
Where  denotes the estimated internal resistance and  is the estimation error of it,   , is the
charge–discharge current and it defined charge as positive value and discharge as negative. In this
study, it was assumed that  is given as the correct values from calculation of chronological data, and
the contributions of errors of open circuit voltage and internal resistance are equal, that can be given
as follows.</p>
        <p>(1)
is the
pre   , −   ,
=  
=    ,
(3)
noted that the first  
learning.
  was calculated by comparing measured charge–discharge voltage with   and contributions of
errors according to equation (2) and (3). Thereafter,   − was calculated based on the additive
gaussian sample values  adjusted by learning rate  .   would be corrected without training data by
repeating a series of learning calculation periodically during charge–discharge cycles. It should be
values must be given artificially. Namely, it can be said as quasi-unsupervised
In this equation, the profile was denoted as a function of   .   (  ) was fitted by the estimated
sample values   − based on the deformative learning of equation (1)-(3). That is,   can be denoted
as the sample values based on equation (4) as follows.</p>
        <p>⋮</p>
        <p>⊺
 
=
  ×   × ⋯   ×
⎡   , ⎤
⎢   , ⎥
= ⎢⎢ ⋮ ⎥⎥</p>
        <p>⎣  , ⎦
 
 × = ⎢
⎡
⎢</p>
        <p>−</p>
        <p>− 

⎢  (
⎣ ( − 
−  ) ⎥
−  )⎦
⎤
⎥
⎥
 
 
⋮
 
 
 
⋮
  
  =
 
 ×  
 × ⋯  
 ×</p>
        <p>− 
 
 × =
(
(
(
−  )
−  )
⋮
−  )
(5)
(6)
as
(7)
(8)
(9)
function  1 including calculation of error with   − as follows.
  5×1 are coefficient vector of equation (4). Updated   (  ) were fitted based on the evaluation
  =
 
 ×  
 × ⋯  
 ×
−   −
follows.</p>
        <p>The estimated sampling data of internal resistance  was fitted as 6th order polynomial of  
based on correct values calculated from chronological charge–discharge data as follows.

 (  ) = ∑=   +  

  7×1 are coefficient vector of equation (7) and  (  ) were fitted based on the evaluation function  2.</p>
        <p>The values of full charge capacity    were set as a measured and calculated values of charge–
discharge of each cycle. Calculation of charge–discharge energy   , was carried out as follows.</p>
        <p>, =    ∫   (  ) +   , (  ) (  )  
  , (  ) is the function of operation current and it was defined by the charge–discharge operator.
Calculation of equation (9) was practically carried out as sectional quadrature. The estimation of
charge and discharge energy each would result in that of energy efficiency, namely, it could be said as
efficiency degradation.
3</p>
      </sec>
    </sec>
    <sec id="sec-4">
      <title>Verification</title>
      <p>For the verification of this profile learning, offset and noise were added to some parameters. First,
+10 % offset error was added to the overall profile of open circuit voltage which was set prior to all
learning processes. This was the assumption of reuse LIB having unknown profiles that was
introduced in a battery aggregation. Second, maximum ±25 % gaussian noise was added to an internal
detailed learning conditions are shown in Table 1.
resistance value of each learning opportunity. This was the assumption of estimation error by Kalman
filter or another similar method. In this verification, the learning rate 
was set as 3 types of fast,
medium, and slow. In addition, the index of deformation width  was adjusted depending on  .the</p>
      <p>This verification was carried out based on the chronological data of 700 times charge–discharge
cycle of LIB module. The detailed cycle conditions are shown in Table 2. The results were shown in
Fig 2. Black lines are actual values of each cycle charge–discharge energy. And red, blue, and green
lines are the estimated one based on the deformative learning of open circuit voltage. Solid lines are
denoted as charge, and dot lines are denoted as discharge. In the case of condition A, the estimated
values were fitted to the actual values within only dozens of cycles. On the other hands, about 150
cycles were necessary in condition B, and about 500 cycles in condition C. The errors of condition A
in the range between 601 to 700 cycles were less than 0.3 % in charge, and 0.7 % in discharge. From
this, we can conclude in the following way. This proposed method of quasi-unsupervised learning of
open circuit voltage profiles could realize the efficiency degradation diagnosis of LIB in combination
with capacity degradation diagnosis and internal resistance estimation. Together with this, it is
important that the appropriate values of  and  are selected. We should note that it could be valid for
reuse LIB having unknown profiles.</p>
      <sec id="sec-4-1">
        <title>Condition</title>
      </sec>
      <sec id="sec-4-2">
        <title>A (fast)</title>
      </sec>
      <sec id="sec-4-3">
        <title>B (medium) C (slow)</title>
        <p />
      </sec>
    </sec>
    <sec id="sec-5">
      <title>4 Conclusion</title>
      <p>In this study, we pointed out the problem of upcoming reuse LIBs from the point of efficiency
degradation. From this, we proposed the quasi-unsupervised learning of open circuit voltage profiles.
Compared to pOCV or GITT, this method has a demerit that an open circuit voltage profile might not
be obtained from only one charge–discharge process. On the other hands, the merit is a high
practicality based on the adaptability of real LIB operation. Therefore, it could realize the efficiency
degradation diagnosis in combination of capacity and internal resistance estimation. Moreover, wide
variety of open circuit voltage profiles would be expressed by not only reuse but also the difference of
active materials like iron phosphate cathode and titanium oxide anode, and the proposed method
might be applicable these overall conditions. It is expected that this diagnosis could be contribute to
an economic improvement of battery aggregation.</p>
      <sec id="sec-5-1">
        <title>Birkl, C. R. et al. (2015) ‘A Parametric Open Circuit Voltage Model for Lithium Ion Batteries’, Journal of The Electrochemical Society, 162(12), pp. A2271–A2280. doi: 10.1149/2.0331512jes.</title>
        <p>CAISO (2016) What the duck curve tells us about managing a green grid. Available at:
https://www.caiso.com/documents/flexibleresourceshelprenewables_fastfacts.pdf (Accessed: 1 June
2021).</p>
      </sec>
      <sec id="sec-5-2">
        <title>Farmann, A. and Sauer, D. U. (2017) ‘A study on the dependency of the open-circuit voltage on temperature and actual aging state of lithium-ion batteries’, Journal of Power Sources, 347, pp. 1–13. doi: 10.1016/j.jpowsour.2017.01.098.</title>
      </sec>
      <sec id="sec-5-3">
        <title>Haus, B. and Mercorelli, P. (2020) ‘Polynomial Augmented Extended Kalman Filter to Estimate the State of Charge of Lithium-Ion Batteries’, IEEE Transactions on Vehicular Technology, 69(2), pp. 1452–1463. doi: 10.1109/TVT.2019.2959720.</title>
      </sec>
      <sec id="sec-5-4">
        <title>Hou, Q. et al. (2020) ‘Embedding scrapping criterion and degradation model in optimal operation of peak-shaving lithium-ion battery energy storage’, Applied Energy, 278, p. 115601. doi: 10.1016/j.apenergy.2020.115601.</title>
        <p>IRENA (2021) Renewable Capacity Statistics 2021. Available at:
https://www.irena.org/publications/2021/March/Renewable-Capacity-Statistics-2021 (Accessed: 1
January 2021).</p>
      </sec>
      <sec id="sec-5-5">
        <title>Isono, E. et al. (2013) ‘Development of battery aggregation technology for smart grid’, in 2013</title>
        <p>IEEE Grenoble Conference. IEEE, pp. 1–6. doi: 10.1109/PTC.2013.6652141.</p>
      </sec>
      <sec id="sec-5-6">
        <title>Kyushu Electric Power Transmission and Distribution Co., I. (2021) Area supply and demand results. Available at: https://www.kyuden.co.jp/td_service_wheeling_rule-document_disclosure (Accessed: 1 June 2021).</title>
      </sec>
      <sec id="sec-5-7">
        <title>Pastor-Fernández, C. et al. (2019) ‘Critical review of non-invasive diagnosis techniques for quantification of degradation modes in lithium-ion batteries’, Renewable and Sustainable Energy Reviews, 109, pp. 138–159. doi: 10.1016/j.rser.2019.03.060.</title>
      </sec>
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        <title>Plett, G. L. (2004) ‘Extended Kalman filtering for battery management systems of LiPB-based HEV battery packs: part 2. Modeling and identification’, Journal of Power Sources, 134(2), pp. 262– 276. doi: 10.1016/j.jpowsour.2004.02.032.</title>
      </sec>
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        <title>Ramadass, P. et al. (2002) ‘Capacity fade of Sony 18650 cells cycled at elevated temperatures’,</title>
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      </sec>
    </sec>
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