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Published on: March 7, 2018
Boosting stable lithium deposition via Li3N-Enriched inorganic SEI induced by a polycationic polymer layer
Wenzhu Cao1, Weimin Chen2, Zhenghan Lai2
1Key Laboratory for Green Chemical Process of Ministry of Education, Hubei Key Laboratory for Novel Reactor and Green Chemistry Technology, Hubei Engineering Research Center for Advanced Fine Chemicals, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, China; Institute of Nanoscience and Nanotechnology, School of Physical Science and Technology, Central China Normal University, Wuhan 430079, China.
This study introduces a novel Si@PDDA interfacial layer for lithium metal anodes, enabling uniform lithium deposition and enhancing battery safety and energy density. The new design significantly improves cycle life and performance in rechargeable batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Lithium (Li) metal anodes are key for high-energy batteries but suffer from uneven lithium deposition and safety risks due to excess Li.
- Electrochemical pre-lithiation is used to control Li content, but traditional substrates lead to inhomogeneous surfaces and fragile solid electrolyte interphase (SEI) layers.
- Developing stable and efficient lithium metal anodes (LMAs) is critical for next-generation batteries.
Purpose of the Study:
- To design an interfacial layer that promotes homogeneous lithium plating/stripping and forms a stable, Li3N-rich SEI.
- To improve the interfacial stability and electrochemical cycling performance of lithium metal anodes.
- To address the challenges of inhomogeneous surfaces and high nucleation barriers in traditional pre-lithiation methods.
Main Methods:
- Fabrication of an interfacial layer using nano-Si particles and cationic polymer (poly(diallyldimethylammonium chloride)), denoted as Si@PDDA.
- Utilizing the Si@PDDA layer to induce the formation of a Li3N-rich inorganic SEI on lithium metal anodes.
- Investigating the effects of the Si@PDDA layer on Li+ nucleation overpotential, Li metal growth, and electrolyte decomposition kinetics.
- Testing symmetrical cells and practical full cells to evaluate electrochemical cycling performance and stability.
Main Results:
- The Si@PDDA interfacial layer successfully induced a Li3N-rich SEI, enhancing interfacial stability.
- Uniform lithium plating and stripping were achieved, suppressing dendrite formation.
- Nano-Si particles reduced Li+ nucleation overpotential via alloying, while PDDA provided electrostatic shielding and accelerated electrolyte decomposition.
- Symmetrical cells demonstrated a cycle life of 900 hours at 1 mA cm-2, and full cells operated for over 160 cycles at a low N/P capacity ratio of ~3.
Conclusions:
- The Si@PDDA interfacial layer is an effective strategy for developing stable and high-performance lithium metal anodes.
- The engineered SEI layer significantly improves the cycling stability and safety of lithium metal batteries.
- This approach offers a promising pathway for advancing high-energy rechargeable battery technology.
