Materials Letters: X 17 (2023) 100183

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Materials Letters: X
journal homepage: www.sciencedirect.com/journal/materials-letters-x

Data-driven predictive modeling of FeCrAl oxidation

Indranil Roy , Subhrajit Roychowdhury , Bojun Feng , Sandipp Krishnan Ravi , Sayan Ghosh ,
Rajnikant Umretiya , Raul B. Rebak , Daniel M. Ruscitto , Vipul Gupta , Andrew Hoffman *
GE Research, Schenectady, NY 12309, United States

A R T I C L E I N F O A B S T R A C T

Keywords: FeCrAl alloys are among the most promising candidates for accident-tolerant fuel cladding material in light water
FeCrAl nuclear reactors. Despite their high-temperature oxidation resistance in corrosive environments coupled with
Machine Learning their hydrothermal corrosion resistance, a key challenge remains in optimizing the composition of the alloy that
Oxidation
can be achieved through statistical analysis. However, the current literature on FeCrAl alloy design lack studies
for designing alloys based on oxidation resistance. This study addresses that gap by developing a predictive
model for the oxidation of FeCrAl alloys based on an experimental dataset, which lays the groundwork for model-
based optimization for alloy composition.

Introduction In this work, we applied conventional machine learning tools [5,6]

After the events at the Fukishima Diaachi nuclear power station in
2011, there is an increasing demand for accident tolerant fuel cladding
material in nuclear power plants. This has led to growing interest in
oxidation resistant material discovery to modify/replace Zr-based al­
loys. Among different high temperature (<1000 ◦ C) oxidation resistant
concepts, FeCrAl [1] is one of the most promising candidates due to its
several advantageous properties, e.g., superior mechanical properties in
different radiation environment [2], high tensile and yield strength [3],
and excellent resistance to both hydrothermal corrosion and high tem­
perature steam oxidation [1]. However, an exceptionally vast compo­
sitional space of the FeCrAl family presents a significant challenge to
find the optimal composition to meet desired set of objectives. One way
to address this challenge is to resort to model-based optimization tech­
niques [4]. The current literature for FeCrAl lacks the predictive models
that forms the backbone of model-based optimization techniques.
Additionally, the physics is too complex to develop a physics-based
model of suitable fidelity that can be used for this purpose. The cur­
rent work takes the first step at bridging the gap by developing Machine
Learning (ML) based predictive models, which lays the groundwork for
future optimization frameworks. The models employ a high volume of
data generated from corrosion experiments over the years on FeCrAl
alloy under accident tolerant fuel (ATF) program at GE Research, Oak
Ridge National Laboratory, and many other institutions developing
FeCrAl alloys.
and a state-of-the-art Bayesian Hybrid Modeling tool developed by GE
Global Research [7] on a varied experimental dataset produced on
FeCrAl alloy both from literature and from current work being per­
formed by GE. To the best of the authors’ knowledge, there is only one
report on utilizing ML techniques for prediction of FeCrAl alloy prop­
erties, and this report has focused on mechanical property prediction
[8]. While leveraging of ML for nuclear material research is encouraged
by Morgan et al [9], this work is the first approach towards data-driven
modeling for prediction of FeCrAl alloy oxidation based on composition.
Data & modeling
The goal of this paper is to derive a data-driven model to predict
specific mass change of the FeCrAl for a given compositional range. In
particular, the weight % of Fe, Cr, Al, Mo and Ni are chosen as input
features to the model in addition to temperature, test duration and
environmental chemistries. Two different approaches, namely the
Random Forest (RF) and the Bayesian Hybrid Modeling (BHM) were
chosen to develop the predictive models. Random forest is primarily
chosen for its ease of implementation, robustness to data quality (e.g.,
outliers) and ability to handle categorical and continuous values
simultaneously. The BHM on the other hand provides additional insights
on uncertainty quantification and guide us to design experiments
pointing to the data-scarce regions. Python scikit learn library is used for
development of the random forest models whereas proprietary GE

* Corresponding author.
E-mail address: andrew.hoffman@ge.com (A. Hoffman).

https://doi.org/10.1016/j.mlblux.2023.100183
Received 3 June 2022; Received in revised form 3 January 2023; Accepted 15 January 2023
Available online 21 January 2023
2590-1508/© 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-
nc-nd/4.0/).
I. Roy et al. Materials Letters: X 17 (2023) 100183

Fig. 1. The performance of (a) RF and (b) BHM for predicting mass change in 20% random split of the dataset; (c)Splitting of data into train and test set for ensemble
and separate models.

Table 1 √̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
}̅
√{
Prediction errors of Random Forest (RF) and BHM. √ 1 ∑ N
RMSE = √ (yi − ŷi ) 2
(1)
Normalized RMSE N i=1
Conditions No. of test cases RF BHM
RMSE
NRMSE = (2)
Steam 18 1.80 3.20 ymax − ymin
Air 6 0.20 0.45
BWR-HWC 6 0.71 3.5 Here N is the size of test set, yi is the experimental mass change and ŷi
BWR-NWC 5 10.77 13.5 is the predicted mass change for ith data entry. Fig. 1 shows the per­
Ensemble 35 1.13 2.26 formance comparisons of the unified or ensemble models for (a)RF and
(b)BHM. The distribution of the training and test data is shown in Fig. 1
(c). Along with training RF and BHM with the whole dataset, we trained
and tested for four separate experimental conditions, e.g., steam, air,
libraries are used for development of BHM models.
BWR-HWC and BWR-NWC and the normalized RMSE of the four cases
Additionally, both modeling approaches are implemented in two
and listed in Table 1.
different ways. RF and BHM models are developed as a unified or
The importance of various features in predicting sp. mass change are
ensemble model first where they are trained for all oxidation conditions,
ranked and plotted (Fig. 2). Fig. 2(a) shows that for the former model Fe
e.g., steam, air, and prototypic boiling water reactor (BWR)-[hydrogen
concentration has the most impact in mass change prediction followed
water chemistry (HWC), and normal water chemistry (NWC)]. The
by the temperature. From the material science point of view, however,
different oxidation conditions are one hot encoded to the models. Then,
Fe is used as strengthening element for majority of Fe-containing alloys,
another two models of RF and BHM are developed for each individual
including steel, and thus should not be the most important factor from
conditions.
oxidation perspective. The specific mass change is sensitive to concen­
tration of Al and Cr individually. Imagine two FeCrAl alloys where Fe
Result and discussion concentration is the same because the sum of Al and Cr concentration
remains fixed. But those two alloys are expected to have different
To compare the predictive performance of the different models oxidation chemistry, therefore, we reconstructed a model without Fe
quantitatively, Normalized Root Mean Square Error (NRMSE) for the (filler element) concentration as an input feature. In that case, Fig. 2(b)
predictions are defined by the following equations:

2
I. Roy et al.
Fig. 2. Features importance in random forest for predicting mass change in FeCrAl alloy during steam test (a) with and (b) without wt. % of Fe as a feature.
shows Al and Cr concentration to have the most impact in mass change
prediction among the constituents. This emphasizes the need to bring in
the available domain knowledge in constructing the machine learning
models to generate meaningful outputs that should always be cross
validated by expert knowledge.
Using both RF and BHM models, we analyze the effect of varying Cr
(12 to 25 wt%) and Al (0 to 10 wt%) concentration on sp. mass change
prediction of FeCrAl. For high temperature oxidation for 2 h, we choose,
(1) 1000 ◦ C and (2) 1200 ◦ C, to demonstrate the ability of predictive
modeling. We have also plotted the confidence of each of these models in
a surface plot (Fig. 3). Although the results from BHM and RF are
similar, the trend of the heatmap of sp. mass change is more continuous
for BHM than RF because of the inherent smooth nature of the gaussian
process which is the underlying model in the in BHM framework.
The eight subplots in Fig. 3 presents the response surface of specific
mass change across different Al and Cr wt. % using the BHM (Fig. 3
(a–d)) and RF (Fig. 3(e–h)) models. Fig. 3(a, c, e, g) represent the 2D
plots where the colormap correspond to the specific mass change and
Fig. 3(b, d, f, h) represent the 3D plots where the Z axis correspond to the
specific mass change and color map correspond to the uncertainty
(standard deviation) of the predictions. From Fig. 3(a), it can be seen
that low Cr (12–14 wt%) and Al (0–2 wt%) results in high negative
specific mass gain and the model has high confidence in that region as
well (Fig. 3(b)). It comes as no surprise as without a protective Alumina
layer, Chromia tends to vaporize at high temperature (1200 ◦ C). The
high Al and high Cr in Fig. 3(a, c) regions for both 1000 ◦ C and 1200 ◦ C
show very small mass gain after two hours that may look ideal compo­
sition space for alloy development. Both these regions fall under low
confidence regime Fig. 3(b, d), indicating that more experimental data is
necessary. From a metallurgic point of view, we cannot blindly trust ML
alone and disregard regions in the Al-Cr composition space without a
deeper dive into the domain knowledge. Furthermore, specific mass gain
is only one of the many deciding parameters of high temperature
oxidation. However, in this study we show how predictive modeling and
intelligent visualization techniques allows us to focus on regions of in­
terest where the model has high confidence and design future experi­
ments is low confidence regime.
3
Materials Letters: X 17 (2023) 100183
Conclusions
The work described in this article is the first step towards developing
a systematic optimization framework for FeCrAl composition design,
which is of immediate importance in the nuclear power industry. A
predictive model forms the backbone of such optimization work. As
complicated physics precludes the possibility of developing a physics-
based model of suitable fidelity, data-driven modeling remains the
most obvious choice. Although the skewness in the dataset makes it
difficult for the predictive models to perform well in all ranges, the
benefits of ML in conjunction with domain expert knowledge are
demonstrated, nevertheless. To summarize, a cumulative approach of
predictive modeling, optimization, and explainable artificial intelli­
gence needs to be integrated with conventional metallurgic theoretical
and experimental, computational tools for faster convergence of optimal
composition for alloy design, and this work is an early step towards that
vision.
CRediT authorship contribution statement
Indranil Roy: Writing – original draft, Writing – review & editing,
Project administration, Supervision. Subhrajit Roychowdhury: Vali­
dation, Methodology, Visualization. Bojun Feng: Formal analysis,
Validation, Methodology, Visualization. Sandipp Krishnan Ravi:
Formal analysis, Validation, Methodology, Visualization. Sayan Ghosh:
Formal analysis, Validation, Methodology, Visualization. Rajnikant
Umretiya: Data curation, Validation. Raul B. Rebak: Funding acqui­
sition. Daniel M. Ruscitto: Supervision. Vipul Gupta: Supervision.
Andrew Hoffman: Supervision, Data curation, Validation.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
I. Roy et al. Materials Letters: X 17 (2023) 100183

Fig. 3. Specific mass gain is predicted during oxidation after 2 h in steam of FeCrAl alloy with varying Cr and Al concentration (left column) and the uncertainty of
the model (right column). BHM prediction for (a)1200 ◦ C, (c)1000 ◦ C with their respective uncertainty (b and d). RF prediction for (e)1200 ◦ C, (g)1000 ◦ C with their
respective uncertainty (f and h).

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I. Roy et al. Materials Letters: X 17 (2023) 100183

Acknowledgment
This work is supported by the US Department of Energy, National
Nuclear Security Administration, under award number DE-NE0009047
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