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Chen et al. Energy Mater. 2025, 5, 500064 https://dx.doi.org/10.20517/energymater.2024.163 Page 11 of 14

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Furthermore, TOF-SIMS was used to understand the degradation products such as oxidized COO
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functional group as a result of PEO being oxidized. Figure 5D and E displays the normalized COO signal
on the surface of NCM811 cathodes without or with alucone coating layers after cycling. Clearly, the
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intensity of COO signals for the alucone-coated NCM811 is much less than that of the NCM811 without
coating layers, indicating that the oxidative decomposition of PEO is suppressed . On the anode side, LMA
[58]
was peeled and subjected to microscopy measurements. Figure 5F(i) and (ii) shows the SEM images of LMA
surfaces from the cycled batteries with or without alucone coating layers, respectively. The LMA surface
from the battery with alucone coating layer shows a much more compact morphology in comparison to that
from the battery without alucone coating layer. By comparison, the LMA surface from the battery without
an alucone coating layer shows protrusions and aggregates because of the localized lithium plating. The
better lithium plating in the battery of LMA-Alucone|LLZO/PEO/LiTFSI|Alucone-NCM811 can be
attributed to both physical constraint and lithiophilic behavior of the alucone coating layer, which may be
similar to the Al O as discussed in previous publications [59-61] .
2
3
CONCLUSIONS
In this work, a “sandwich” configuration of a dual interface design is proposed to simultaneously protect the
cathode and anode sides in ASSBs. The thickness of the alucone coating layers through ALD methods can
be tuned at the nano-meter scale; such sufficiently thin coating layers can protect the batteries without
suffering the drawbacks of lowered ionic conductivity. A combination characterization of several advanced
techniques shows that the oxidative decomposition of the CSSE film of LLZO/PEO/LiTFSI is effectively
suppressed, which enables a significant enhancement in the battery performance, and the short-circuit is
prevented due to more uniform lithium plating on the anode side. As a result, the obtained LMA-Alucone|
LLZO/PEO/LiTFSI| Alucone-NCM811 battery demonstrates a capacity retention of 84% after cycling for
200 cycles at 0.1C, whereas the contrast cell without protection from the alucone coating layers shows both
fast capacity fading and micro-shorting behavior after 80 cycles. This work demonstrates the importance of
dual interface protection of using a much less explored ALD coating technique for alucone coating layers
for inorganic/organic CSSE-based ASSBs.

DECLARATIONS
Acknowledgments
The authors would like to acknowledge the financial support from the Natural Science Foundation of Fujian
Province, the Educational Research Projects for Young and Middle-aged Teachers in Fujian Province,
Fuzhou University Testing Fund of Precious Apparatus, the National Natural Science Foundation of China,
Pilot Group Program of the Research Fund for International Senior Scientists, the Fujian Province Super
100 Talents Program, Fujian Province 100 Talents Program, Fujian Province Minjiang Scholar Program,
and the Institute of New Energy Materials and Engineering, College of Materials Science and Engineering,
Fuzhou University, First-Class Discipline Training Project. The authors also acknowledge Yi Cui, Yaping
Kong, Rong Huang, and Nan Hu for the TOF-SIMS characterizations at the Vacuum Interconnected
Nanotech Workstation (Nano-X, C24012), Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese
Academy of Sciences. Lastly, the authors wish to acknowledge the anonymous reviewers who provided a lot
of helpful suggestions to enhance this article.

Authors’ contributions
Methodology, investigation, and manuscript writing: Chen, G.; Liu, X.; Liu, Z.; Qian, L.; Zheng, Y.; Dong, J.;
Ma, C.; Wei, S.
Performed data acquisition: Chen, G.; Liu, X.; Liu, Z.; Zhang, T.; Rahmati, F.; Yan, S.