Rational Design of an Artificial SEI: Alloy/Solid Electrolyte Hybrid Layer for a Highly Reversible Na and K Metal Anode

Dongjun Li; Yingjie Sun; Menghao Li; Xiaolong Cheng; Yu Yao; Fanyang Huang; Shuhong Jiao; Meng Gu; Xianhong Rui; Zeeshan Ali; Cheng Ma; Zhong-Shuai Wu; Yan Yu

doi:10.1021/acsnano.2c07049

Rational Design of an Artificial SEI: Alloy/Solid Electrolyte Hybrid Layer for a Highly Reversible Na and K Metal Anode

ACS Nano. 2022 Oct 25;16(10):16966-16975. doi: 10.1021/acsnano.2c07049. Epub 2022 Oct 12.

Authors

Dongjun Li¹, Yingjie Sun², Menghao Li³, Xiaolong Cheng¹, Yu Yao¹, Fanyang Huang¹, Shuhong Jiao¹, Meng Gu³, Xianhong Rui⁴, Zeeshan Ali⁵, Cheng Ma^{1

6}, Zhong-Shuai Wu⁷, Yan Yu^{1

6}

Affiliations

¹ Hefei National Research Center for Physical Sciences at the Microscale, Department of Materials Science and Engineering, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei230026, Anhui, People's Republic of China.
² Hebei Key Laboratory of Photoelectric Control on Surface and Interface, College of Science, Hebei University of Science and Technology, Shijiazhuang050018, Hebei, People's Republic of China.
³ Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen518055, Guangdong, People's Republic of China.
⁴ School of Materials and Energy, Guangdong University of Technology, Guangzhou, 510006, Guangdong, People's Republic of China.
⁵ School of Chemical and Materials Engineering, National University of Sciences and Technology, H-12, Islamabad, 44000Pakistan.
⁶ National Synchrotron Radiation Laboratory, Hefei230026, Anhui, People's Republic of China.
⁷ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian116023, Liaoning, People's Republic of China.

PMID: 36222559
DOI: 10.1021/acsnano.2c07049

Abstract

The practical application of a Na/K-metallic anode is intrinsically hindered by the poor cycle life and safety issues due to the unstable electrode/electrolyte interface and uncontrolled dendrite growth during cycling. Herein, we solve these issues through an in situ reaction of an oxyhalogenide (BiOCl) and Na to construct an artificial solid electrolyte interphase (SEI) layer consisting of an alloy (Na₃Bi) and a solid electrolyte (Na₃OCl) on the surface of the Na anode. As demonstrated by theoretical and experimental results, such an artificial SEI layer combines the synergistic properties of high ionic conductivity, electronic insulation, and interfacial stability, leading to uniform dendrite-free Na deposition beneath the hybrid SEI layer. The protected Na anode presents a low voltage polarization of 30 mV, achieving an extended cycling life of 700 h at 1 mA cm^-2 in the carbonate-based electrolyte. The full cell based on the Na₃V₂(PO₄)₃ cathode and hybrid SEI-protected Na anode shows long-term stability. When this strategy is applied to a K metal anode, the protected K anode also reaches a cycling life of over 4000 h at 0.5 mA cm^-2 with a low voltage polarization of 100 mV. Our work provides an important insight into the design principles of a stable artificial SEI layer for high-energy-density metal batteries.

Keywords: alloys/solid electrolytes; artificial hybrid interphase; high ionic conductivity; long lifespan; low voltage polarization; metal batteries.